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doi: 10.1016/j.gee.2025.11.003
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2025, 10(10): 1957-1967.
doi: 10.1016/j.gee.2024.10.003
Abstract:
Sustainable H2 production based on hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) has attracted wide attention due to minimal energy consumption compared to overall water electrolysis. The present study focuses on the design and construction of heterostructured CoPB@NiFe-OH applied as efficient bifunctional catalysts to sustainably produce hydrogen and remove hydrazine in alkaline media. Impressively, CoPB@NiFe-OH heterointerface exhibits an HzOR potential of -135 mV at the current density of 10 mA cm-2 when the P to B atom ratio was 0.2, simultaneously an HER potential of -32 mV toward HER when the atom ratio of P and B was 0.5. Thus, hydrogen production without an outer voltage accompanied by a small current density output of 25 mA cm-2 is achieved, surpassing most reported catalysts. In addition, DFT calculations demonstrate the Co sites in CoPB upgrades H* adsorption, while the Ni sites in NiFe-OH optimizes the adsorption energy of N2H4* due to electron transfer from CoPB to NiFe-OH at the heterointerface, ultimately leading to exceptional performance in hydrazine-assistant water electrolysis via HER coupled with HzOR.
Sustainable H2 production based on hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) has attracted wide attention due to minimal energy consumption compared to overall water electrolysis. The present study focuses on the design and construction of heterostructured CoPB@NiFe-OH applied as efficient bifunctional catalysts to sustainably produce hydrogen and remove hydrazine in alkaline media. Impressively, CoPB@NiFe-OH heterointerface exhibits an HzOR potential of -135 mV at the current density of 10 mA cm-2 when the P to B atom ratio was 0.2, simultaneously an HER potential of -32 mV toward HER when the atom ratio of P and B was 0.5. Thus, hydrogen production without an outer voltage accompanied by a small current density output of 25 mA cm-2 is achieved, surpassing most reported catalysts. In addition, DFT calculations demonstrate the Co sites in CoPB upgrades H* adsorption, while the Ni sites in NiFe-OH optimizes the adsorption energy of N2H4* due to electron transfer from CoPB to NiFe-OH at the heterointerface, ultimately leading to exceptional performance in hydrazine-assistant water electrolysis via HER coupled with HzOR.
2025, 10(10): 1968-1980.
doi: 10.1016/j.gee.2024.06.008
Abstract:
Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides. Leveraging intrinsic heptazine/triazine phase and face-to-face contact, crystalline C3N5 (CC3N5) was combined with protonated g-C3N4 (pgCN) through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces. The highest photocatalytic performance was obtained through crystallinity and homojunction engineering, by controlling the pgCN:CC3N5 ratio. The 25:100 pgCN:CC3N5 homojunction (25CgCN) had the highest hydrogen production (1409.51 μmol h-1) and apparent quantum efficiency (25.04%, 420 nm), 8-fold and 180-fold higher than CC3N5 and pgCN, respectively. This photocatalytic homojunction improves benzaldehyde and hydrogen production activity, retaining 89% performance after 3 cycles (12 h) on a 3D-printed substrate. Electron paramagnetic resonance demonstrated higher ·OH-, ·O2- and hole production of irradiated 25CgCN, attributed to crystallinity and homojunction interaction. Thus, electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.
Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides. Leveraging intrinsic heptazine/triazine phase and face-to-face contact, crystalline C3N5 (CC3N5) was combined with protonated g-C3N4 (pgCN) through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces. The highest photocatalytic performance was obtained through crystallinity and homojunction engineering, by controlling the pgCN:CC3N5 ratio. The 25:100 pgCN:CC3N5 homojunction (25CgCN) had the highest hydrogen production (1409.51 μmol h-1) and apparent quantum efficiency (25.04%, 420 nm), 8-fold and 180-fold higher than CC3N5 and pgCN, respectively. This photocatalytic homojunction improves benzaldehyde and hydrogen production activity, retaining 89% performance after 3 cycles (12 h) on a 3D-printed substrate. Electron paramagnetic resonance demonstrated higher ·OH-, ·O2- and hole production of irradiated 25CgCN, attributed to crystallinity and homojunction interaction. Thus, electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.
2025, 10(10): 1981-1989.
doi: 10.1016/j.gee.2024.09.001
Abstract:
Covalent organic frameworks (COFs) are newly developed crystalline substances that are garnering growing interest because of their ultra-high porosity, crystalline nature, and easy-modified architecture, showing promise in the field of photocatalysis. However, it is difficult for pure COFs materials to achieve excellent photocatalytic hydrogen production due to their severe carrier recombination problems. To mitigate this crucial issue, establishing heterojunction is deemed an effective approach. Nonetheless, many of the metal-containing materials that have been used to construct heterojunctions with COFs own a number of drawbacks, including small specific surface area and rare active sites (for inorganic semiconductor materials), wider bandgaps and higher preparation costs (for MOFs). Therefore, it is necessary to choose metal-free materials that are easy to prepare. Red phosphorus (RP), as a semiconductor material without metal components, with suitable bandgap, moderate redox potential, relatively minimal toxicity, is affordable and readily available. Herein, a range of RP/TpPa-1-COF (RP/TP1C) composites have been successfully prepared through solvothermal method. The two-dimensional structure of the two materials causes strong interactions between the materials, and the construction of heterojunctions effectively inhibits the recombination of photogenic charge carriers. As a consequence, the 9% RP/TP1C composite, with the optimal photocatalytic ability, achieves a photocatalytic H2 evolution rate of 6.93 mmol g-1 h-1, demonstrating a 10.19-fold increase compared to that of bare RP and a 4.08-fold improvement over that of pure TP1C. This article offers a novel and innovative method for the advancement of efficient COF-based photocatalysts.
Covalent organic frameworks (COFs) are newly developed crystalline substances that are garnering growing interest because of their ultra-high porosity, crystalline nature, and easy-modified architecture, showing promise in the field of photocatalysis. However, it is difficult for pure COFs materials to achieve excellent photocatalytic hydrogen production due to their severe carrier recombination problems. To mitigate this crucial issue, establishing heterojunction is deemed an effective approach. Nonetheless, many of the metal-containing materials that have been used to construct heterojunctions with COFs own a number of drawbacks, including small specific surface area and rare active sites (for inorganic semiconductor materials), wider bandgaps and higher preparation costs (for MOFs). Therefore, it is necessary to choose metal-free materials that are easy to prepare. Red phosphorus (RP), as a semiconductor material without metal components, with suitable bandgap, moderate redox potential, relatively minimal toxicity, is affordable and readily available. Herein, a range of RP/TpPa-1-COF (RP/TP1C) composites have been successfully prepared through solvothermal method. The two-dimensional structure of the two materials causes strong interactions between the materials, and the construction of heterojunctions effectively inhibits the recombination of photogenic charge carriers. As a consequence, the 9% RP/TP1C composite, with the optimal photocatalytic ability, achieves a photocatalytic H2 evolution rate of 6.93 mmol g-1 h-1, demonstrating a 10.19-fold increase compared to that of bare RP and a 4.08-fold improvement over that of pure TP1C. This article offers a novel and innovative method for the advancement of efficient COF-based photocatalysts.
2025, 10(10): 1990-2001.
doi: 10.1016/j.gee.2025.05.003
Abstract:
1T-MoS2 nanosheets, with metallic conductivity and high capacity, hold great potential for lithium-ion capacitors (LICs), but suffer from sluggish reaction kinetics due to dense stacking. Herein, 1T-MoS2 nanosheets with enlarged interlayer spacing, vertically bonded to reduced graphene oxide (rGO) (1T-MoS2/rGO), were designed using a hydrothermal-assisted dispersion and intercalation strategy. The active nitrogen species derived from N, N-dimethylformamide (DMF) not only bridge the rGO and MoS2 through strong Mo-N-C bonds to promote the formation of dispersed MoS2 nanosheets, but also intercalate into the MoS2 structure, further enlarging the interlayer spacing. This unique structure synergistically enhances meso- and microscale mass transfer outside and inside of the few-layered nanosheets, significantly improving electrochemical reaction kinetics and reducing the kinetic mismatch between the anode and cathode. Consequently, the resulting-1T-MoS2/rGO achieves a capacity of 500 mAh g-1 after 500 cycles at 5 A g-1 and a high rate performance of 587 mAh g-1 at a high rate of 10 A g-1. Moreover, the assembled 3D vertical 1T-MoS2/rGO//AC LIC delivers a high energy density of 100.3 Wh kg-1 at a power density of 1.0 kW kg-1, and long cycle stability with capacity retention as high as 91.02% after 5000 cycles at 2 A g-1. This work provides a generalizable strategy for engineering two-dimensional material-based electrodes, offering new insights into high-performance energy storage systems.
1T-MoS2 nanosheets, with metallic conductivity and high capacity, hold great potential for lithium-ion capacitors (LICs), but suffer from sluggish reaction kinetics due to dense stacking. Herein, 1T-MoS2 nanosheets with enlarged interlayer spacing, vertically bonded to reduced graphene oxide (rGO) (1T-MoS2/rGO), were designed using a hydrothermal-assisted dispersion and intercalation strategy. The active nitrogen species derived from N, N-dimethylformamide (DMF) not only bridge the rGO and MoS2 through strong Mo-N-C bonds to promote the formation of dispersed MoS2 nanosheets, but also intercalate into the MoS2 structure, further enlarging the interlayer spacing. This unique structure synergistically enhances meso- and microscale mass transfer outside and inside of the few-layered nanosheets, significantly improving electrochemical reaction kinetics and reducing the kinetic mismatch between the anode and cathode. Consequently, the resulting-1T-MoS2/rGO achieves a capacity of 500 mAh g-1 after 500 cycles at 5 A g-1 and a high rate performance of 587 mAh g-1 at a high rate of 10 A g-1. Moreover, the assembled 3D vertical 1T-MoS2/rGO//AC LIC delivers a high energy density of 100.3 Wh kg-1 at a power density of 1.0 kW kg-1, and long cycle stability with capacity retention as high as 91.02% after 5000 cycles at 2 A g-1. This work provides a generalizable strategy for engineering two-dimensional material-based electrodes, offering new insights into high-performance energy storage systems.
2023, 8(1): 10-114.
doi: 10.1016/j.gee.2022.07.003
摘要：
In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future, lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock. This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels. Following a brief introduction on the structure, major resources and pretreatment methods of lignocellulosic biomass, the catalytic conversion of three main components, i.e., cellulose, hemicellulose and lignin, into various compounds are comprehensively discussed. Either in separate steps or in one-pot, cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF, furfural, polyols, and organic acids, or even nitrogen-containing chemicals such as amino acids. On the other hand, lignin is first depolymerized into phenols, catechols, guaiacols, aldehydes and ketones, and then further transformed into hydrocarbon fuels, bioplastic precursors and bioactive compounds. The review then introduces the transformations of whole biomass via catalytic gasification, catalytic pyrolysis, as well as emerging strategies. Finally, opportunities, challenges and prospective of woody biomass valorization are highlighted.
In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future, lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock. This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels. Following a brief introduction on the structure, major resources and pretreatment methods of lignocellulosic biomass, the catalytic conversion of three main components, i.e., cellulose, hemicellulose and lignin, into various compounds are comprehensively discussed. Either in separate steps or in one-pot, cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF, furfural, polyols, and organic acids, or even nitrogen-containing chemicals such as amino acids. On the other hand, lignin is first depolymerized into phenols, catechols, guaiacols, aldehydes and ketones, and then further transformed into hydrocarbon fuels, bioplastic precursors and bioactive compounds. The review then introduces the transformations of whole biomass via catalytic gasification, catalytic pyrolysis, as well as emerging strategies. Finally, opportunities, challenges and prospective of woody biomass valorization are highlighted.
2019, 4(2): 95-115.
doi: 10.1016/j.gee.2019.01.012
摘要：
Biomass is renewable, abundant, cheap, biocompatible, and biodegradable materials and has been used to produce chemicals, materials, energy, and fuels. However, most of the biomass, especially most of the biomass polymers are not soluble in common solvents, which hinders their pretreatment and conversion. Deep eutectic solvents (DESs) are environmental-friendly, cheap, and highly tunable, with high solubility, which renders them potential applications in biomass pretreatment and conversion. They could be used as solvents or catalysts and so on. This paper intends to review the application of DESs for the pretreatment of biomass and conversion of biomass to value-added products. We focus on the following topics related to biomass and DESs: (1) DESs for the pretreatment of biomass; (2) DESs for the dissolution and separation of biomass or extraction of chemicals from biomass; (3) DESs for biomass conversion; (4) Drawbacks, and recyclability of DESs for pretreatment and conversion of biomass.
Biomass is renewable, abundant, cheap, biocompatible, and biodegradable materials and has been used to produce chemicals, materials, energy, and fuels. However, most of the biomass, especially most of the biomass polymers are not soluble in common solvents, which hinders their pretreatment and conversion. Deep eutectic solvents (DESs) are environmental-friendly, cheap, and highly tunable, with high solubility, which renders them potential applications in biomass pretreatment and conversion. They could be used as solvents or catalysts and so on. This paper intends to review the application of DESs for the pretreatment of biomass and conversion of biomass to value-added products. We focus on the following topics related to biomass and DESs: (1) DESs for the pretreatment of biomass; (2) DESs for the dissolution and separation of biomass or extraction of chemicals from biomass; (3) DESs for biomass conversion; (4) Drawbacks, and recyclability of DESs for pretreatment and conversion of biomass.
2020, 5(1): 8-21.
doi: 10.1016/j.gee.2019.03.002
摘要：
This review divides the acidic deep eutectic solvents (ADES) into Brønsted and Lewis DES according to their diversity of acidic character. The hydrogen bond donors and halide salts for formulating an ADES are classified, the synthesis methods are described, and the physicochemical properties including freezing point, acidity, density, viscosity and conductivity are presented. Furthermore, the applications of Brønsted acidic deep eutectic solvents (BADES) and Lewis acidic deep eutectic solvents (LADES) are overviewed, respectively, covering the fields in dissolution, extraction, organic reaction and metal electrodeposition. It is expected that the ADES has great potential to replace the pollutional mineral acid, expensive and unstable solid acid, and costly ionic liquid in many acid-employed chemical processes, thus meeting the demands of green chemistry.
This review divides the acidic deep eutectic solvents (ADES) into Brønsted and Lewis DES according to their diversity of acidic character. The hydrogen bond donors and halide salts for formulating an ADES are classified, the synthesis methods are described, and the physicochemical properties including freezing point, acidity, density, viscosity and conductivity are presented. Furthermore, the applications of Brønsted acidic deep eutectic solvents (BADES) and Lewis acidic deep eutectic solvents (LADES) are overviewed, respectively, covering the fields in dissolution, extraction, organic reaction and metal electrodeposition. It is expected that the ADES has great potential to replace the pollutional mineral acid, expensive and unstable solid acid, and costly ionic liquid in many acid-employed chemical processes, thus meeting the demands of green chemistry.
2017, 2(3): 218-245.
doi: 10.1016/j.gee.2017.05.003
摘要：
Metal organic frameworks (MOFs) represent a class of porous material which is formed by strong bonds between metal ions and organic linkers. By careful selection of constituents, MOFs can exhibit very high surface area, large pore volume, and excellent chemical stability. Research on synthesis, structures and properties of various MOFs has shown that they are promising materials for many applications, such as energy storage, gas storage, heterogeneous catalysis and sensing. Apart from direct use, MOFs have also been used as support substrates for nanomaterials or as sacrificial templates/precursors for preparation of various functional nanostructures. In this review, we aim to present the most recent development of MOFs as precursors for the preparation of various nanostructures and their potential applications in energy-related devices and processes. Specifically, this present survey intends to push the boundaries and covers the literatures from the year 2013 to early 2017, on supercapacitors, lithium ion batteries, electrocatalysts, photocatalyst, gas sensing, water treatment, solar cells, and carbon dioxide capture. Finally, an outlook in terms of future challenges and potential prospects towards industrial applications are also discussed.
Metal organic frameworks (MOFs) represent a class of porous material which is formed by strong bonds between metal ions and organic linkers. By careful selection of constituents, MOFs can exhibit very high surface area, large pore volume, and excellent chemical stability. Research on synthesis, structures and properties of various MOFs has shown that they are promising materials for many applications, such as energy storage, gas storage, heterogeneous catalysis and sensing. Apart from direct use, MOFs have also been used as support substrates for nanomaterials or as sacrificial templates/precursors for preparation of various functional nanostructures. In this review, we aim to present the most recent development of MOFs as precursors for the preparation of various nanostructures and their potential applications in energy-related devices and processes. Specifically, this present survey intends to push the boundaries and covers the literatures from the year 2013 to early 2017, on supercapacitors, lithium ion batteries, electrocatalysts, photocatalyst, gas sensing, water treatment, solar cells, and carbon dioxide capture. Finally, an outlook in terms of future challenges and potential prospects towards industrial applications are also discussed.
2017, 2(3): 246-277.
doi: 10.1016/j.gee.2017.06.006
摘要：
The aluminum–air battery is considered to be an attractive candidate as a power source for electric vehicles (EVs) because of its high theoretical energy density (8100 Wh kg−1), which is significantly greater than that of the state-of-the-art lithium-ion batteries (LIBs). However, some technical and scientific problems preventing the large-scale development of Al–air batteries have not yet to be resolved. In this review, we present the fundamentals, challenges and the recent advances in Al–air battery technology from aluminum anode, air cathode and electrocatalysts to electrolytes and inhibitors. Firstly, the alloying of aluminum with transition metal elements is reviewed and shown to reduce the self-corrosion of Al and improve battery performance. Additionally for the cathode, extensive studies of electrocatalytic materials for oxygen reduction/evolution including Pt and Pt alloys, nonprecious metal catalysts, and carbonaceous materials at the air cathode are highlighted. Moreover, for the electrolyte, the application of aqueous and nonaqueous electrolytes in Al–air batteries are discussed. Meanwhile, the addition of inhibitors to the electrolyte to enhance electrochemical performance is also explored. Finally, the challenges and future research directions are proposed for the further development of Al–air batteries.
The aluminum–air battery is considered to be an attractive candidate as a power source for electric vehicles (EVs) because of its high theoretical energy density (8100 Wh kg−1), which is significantly greater than that of the state-of-the-art lithium-ion batteries (LIBs). However, some technical and scientific problems preventing the large-scale development of Al–air batteries have not yet to be resolved. In this review, we present the fundamentals, challenges and the recent advances in Al–air battery technology from aluminum anode, air cathode and electrocatalysts to electrolytes and inhibitors. Firstly, the alloying of aluminum with transition metal elements is reviewed and shown to reduce the self-corrosion of Al and improve battery performance. Additionally for the cathode, extensive studies of electrocatalytic materials for oxygen reduction/evolution including Pt and Pt alloys, nonprecious metal catalysts, and carbonaceous materials at the air cathode are highlighted. Moreover, for the electrolyte, the application of aqueous and nonaqueous electrolytes in Al–air batteries are discussed. Meanwhile, the addition of inhibitors to the electrolyte to enhance electrochemical performance is also explored. Finally, the challenges and future research directions are proposed for the further development of Al–air batteries.
2018, 3(1): 20-41.
doi: 10.1016/j.gee.2017.10.001
摘要：
Over the past decades, a series of aqueous rechargeable batteries (ARBs) were explored, investigated and demonstrated. Among them, aqueous rechargeable alkali-metal ion (Li+, Na+, K+) batteries, aqueous rechargeable-metal ion (Zn2+, Mg2+, Ca2+, Al3+) batteries and aqueous rechargeable hybrid batteries are standing out due to peculiar properties. In this review, we focus on the fundamental basics of these batteries, and discuss the scientific and/or technological achievements and challenges. By critically reviewing state-of-the-art technologies and the most promising results so far, we aim to analyze the benefits of ARBs and the critical issues to be addressed, and to promote better development of ARBs.
Over the past decades, a series of aqueous rechargeable batteries (ARBs) were explored, investigated and demonstrated. Among them, aqueous rechargeable alkali-metal ion (Li+, Na+, K+) batteries, aqueous rechargeable-metal ion (Zn2+, Mg2+, Ca2+, Al3+) batteries and aqueous rechargeable hybrid batteries are standing out due to peculiar properties. In this review, we focus on the fundamental basics of these batteries, and discuss the scientific and/or technological achievements and challenges. By critically reviewing state-of-the-art technologies and the most promising results so far, we aim to analyze the benefits of ARBs and the critical issues to be addressed, and to promote better development of ARBs.
2020, 5(1): 37-49.
doi: 10.1016/j.gee.2019.09.003
摘要：
The most abundant natural biopolymer on earth, cellulose fiber, may offer a highly efficient, low-cost, and chemical-free option for wastewater treatment. Cellulose is widely distributed in plants and several marine animals. It is a carbohydrate polymer consisting of β-1,4-linked anhydro-D-glucose units with three hydroxyl groups per anhydroglucose unit (AGU). Cellulose-based materials have been used in food, industrial, pharmaceutical, paper, textile production, and in wastewater treatment applications due to their low cost, renewability, biodegradability, and non-toxicity. For water treatment in the oil and gas industry, cellulose-based materials can be used as adsorbents, flocculants, and oil/water separation membranes. In this review, the uses of cellulose-based materials for wastewater treatment in the oil & gas industry are summarized, and recent research progress in the following aspects are highlighted: crude oil spill cleaning, flocculation of solid suspended matter in drilling or oil recovery in the upstream oil industry, adsorption of heavy metal or chemicals, and separation of oil/water by cellulosic membrane in the downstream water treatment.
The most abundant natural biopolymer on earth, cellulose fiber, may offer a highly efficient, low-cost, and chemical-free option for wastewater treatment. Cellulose is widely distributed in plants and several marine animals. It is a carbohydrate polymer consisting of β-1,4-linked anhydro-D-glucose units with three hydroxyl groups per anhydroglucose unit (AGU). Cellulose-based materials have been used in food, industrial, pharmaceutical, paper, textile production, and in wastewater treatment applications due to their low cost, renewability, biodegradability, and non-toxicity. For water treatment in the oil and gas industry, cellulose-based materials can be used as adsorbents, flocculants, and oil/water separation membranes. In this review, the uses of cellulose-based materials for wastewater treatment in the oil & gas industry are summarized, and recent research progress in the following aspects are highlighted: crude oil spill cleaning, flocculation of solid suspended matter in drilling or oil recovery in the upstream oil industry, adsorption of heavy metal or chemicals, and separation of oil/water by cellulosic membrane in the downstream water treatment.
2022, 7(1): 3-15.
doi: 10.1016/j.gee.2020.12.023
摘要：
In recent years, an increasing amount of interest has been dedicated to the synthesis and application of ZIF-67-based materials due to their exceptionally high surface area, tunable porosity, and excellent thermal and chemical stabilities. This review summarizes the latest strategies of synthesizing ZIF-67-based materials by exploring the prominent examples. Then, the recent progress in the applications of ZIF-67-based materials in heterogeneous catalysis, including catalysis of the redox reactions, addition reactions, esterification reactions, Knoevenagel condensations, and hydrogenation-dehydrogenation reactions, has been elaborately discussed. Finally, we end this work by shedding some light on the large-scale industrial production of ZIF-67-based materials and their applications in the future.
In recent years, an increasing amount of interest has been dedicated to the synthesis and application of ZIF-67-based materials due to their exceptionally high surface area, tunable porosity, and excellent thermal and chemical stabilities. This review summarizes the latest strategies of synthesizing ZIF-67-based materials by exploring the prominent examples. Then, the recent progress in the applications of ZIF-67-based materials in heterogeneous catalysis, including catalysis of the redox reactions, addition reactions, esterification reactions, Knoevenagel condensations, and hydrogenation-dehydrogenation reactions, has been elaborately discussed. Finally, we end this work by shedding some light on the large-scale industrial production of ZIF-67-based materials and their applications in the future.
2022, 7(4): 578-605.
doi: 10.1016/j.gee.2021.04.006
摘要：
As an aromatic polymer in nature, lignin has recently attracted gross attention because of its advantages of high carbon content, low cost and bio-renewability. However, most lignin is directly burnt for power generation to satisfy the energy demand of the pulp mills. As a result, only a handful of isolated lignin is used as a raw material. Thus, increasing value addition on lignin to expand its scope of applications is currently a challenge demanding immediate attention. Many efforts have been made in the valorization of lignin, including the preparation of precursors for carbon fibers. However, its complex structure and diversity significantly restrict the spinnability of lignin. In this review, we provide elaborate knowledge on the preparation of lignin-based carbon fibers ranging from the relationships among chemical structures, formation conditions and properties of fibers, to their potential applications. Specifically, control procedures for different spinning methods of lignin, including melt spinning, solution spinning and electrospinning, together with stabilization and carbonization are deeply discussed to provide an overall understanding towards the formation of lignin-based carbon fibers. We also offer perspectives on the challenges and new directions for future development of lignin-based carbon fibers.
As an aromatic polymer in nature, lignin has recently attracted gross attention because of its advantages of high carbon content, low cost and bio-renewability. However, most lignin is directly burnt for power generation to satisfy the energy demand of the pulp mills. As a result, only a handful of isolated lignin is used as a raw material. Thus, increasing value addition on lignin to expand its scope of applications is currently a challenge demanding immediate attention. Many efforts have been made in the valorization of lignin, including the preparation of precursors for carbon fibers. However, its complex structure and diversity significantly restrict the spinnability of lignin. In this review, we provide elaborate knowledge on the preparation of lignin-based carbon fibers ranging from the relationships among chemical structures, formation conditions and properties of fibers, to their potential applications. Specifically, control procedures for different spinning methods of lignin, including melt spinning, solution spinning and electrospinning, together with stabilization and carbonization are deeply discussed to provide an overall understanding towards the formation of lignin-based carbon fibers. We also offer perspectives on the challenges and new directions for future development of lignin-based carbon fibers.
2023, 8(4): 972-988.
doi: 10.1016/j.gee.2022.02.002
摘要：
Developing multifunctional energy storage systems with high specific energy, high specific power and long cycling life has been the one of the most important research directions. Compared to batteries and traditional capacitors, supercapacitors possess more balanced performance with both high specific power and long cycle-life. Nevertheless, regular supercapacitors can only achieve energy storage without harvesting energy and the energy density is still not very high compared to batteries. Therefore, combining high specific energy and high specific power, long cycle-life and even fast self-charging into one cell has been a promising direction for future energy storage devices. The multifunctional hybrid supercapacitors like asymmetric supercapacitors, batteries/supercapacitors hybrid devices and self-charging hybrid supercapacitors have been widely studied recently. Carbon based electrodes are common materials used in all kinds of energy storage devices due to their fabulous electrical and mechanical properties. In this survey, the research progress of all kinds of hybrid supercapacitors using multiple effects and their working mechanisms are briefly reviewed. And their advantages and disadvantages are discussed. The hybrid supercapacitors have great application potential for portable electronics, wearable devices and implantable devices in the future.
Developing multifunctional energy storage systems with high specific energy, high specific power and long cycling life has been the one of the most important research directions. Compared to batteries and traditional capacitors, supercapacitors possess more balanced performance with both high specific power and long cycle-life. Nevertheless, regular supercapacitors can only achieve energy storage without harvesting energy and the energy density is still not very high compared to batteries. Therefore, combining high specific energy and high specific power, long cycle-life and even fast self-charging into one cell has been a promising direction for future energy storage devices. The multifunctional hybrid supercapacitors like asymmetric supercapacitors, batteries/supercapacitors hybrid devices and self-charging hybrid supercapacitors have been widely studied recently. Carbon based electrodes are common materials used in all kinds of energy storage devices due to their fabulous electrical and mechanical properties. In this survey, the research progress of all kinds of hybrid supercapacitors using multiple effects and their working mechanisms are briefly reviewed. And their advantages and disadvantages are discussed. The hybrid supercapacitors have great application potential for portable electronics, wearable devices and implantable devices in the future.
2024, 9(9): 1366-1383.
doi: 10.1016/j.gee.2023.10.002
Abstract:
2017, 2(3): 246-277.
doi: 10.1016/j.gee.2017.06.006
Abstract:
2024, 9(9): 1459-1465.
doi: 10.1016/j.gee.2023.09.002
Abstract:
2023, 8(2): 351-353.
doi: 10.1016/j.gee.2022.06.002
Abstract:
2023, 8(1): 10-114.
doi: 10.1016/j.gee.2022.07.003
Abstract:
In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future, lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock. This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels. Following a brief introduction on the structure, major resources and pretreatment methods of lignocellulosic biomass, the catalytic conversion of three main components, i.e., cellulose, hemicellulose and lignin, into various compounds are comprehensively discussed. Either in separate steps or in one-pot, cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF, furfural, polyols, and organic acids, or even nitrogen-containing chemicals such as amino acids. On the other hand, lignin is first depolymerized into phenols, catechols, guaiacols, aldehydes and ketones, and then further transformed into hydrocarbon fuels, bioplastic precursors and bioactive compounds. The review then introduces the transformations of whole biomass via catalytic gasification, catalytic pyrolysis, as well as emerging strategies. Finally, opportunities, challenges and prospective of woody biomass valorization are highlighted.
In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future, lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock. This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels. Following a brief introduction on the structure, major resources and pretreatment methods of lignocellulosic biomass, the catalytic conversion of three main components, i.e., cellulose, hemicellulose and lignin, into various compounds are comprehensively discussed. Either in separate steps or in one-pot, cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF, furfural, polyols, and organic acids, or even nitrogen-containing chemicals such as amino acids. On the other hand, lignin is first depolymerized into phenols, catechols, guaiacols, aldehydes and ketones, and then further transformed into hydrocarbon fuels, bioplastic precursors and bioactive compounds. The review then introduces the transformations of whole biomass via catalytic gasification, catalytic pyrolysis, as well as emerging strategies. Finally, opportunities, challenges and prospective of woody biomass valorization are highlighted.
2019, 4(2): 95-115.
doi: 10.1016/j.gee.2019.01.012
Abstract:
Biomass is renewable, abundant, cheap, biocompatible, and biodegradable materials and has been used to produce chemicals, materials, energy, and fuels. However, most of the biomass, especially most of the biomass polymers are not soluble in common solvents, which hinders their pretreatment and conversion. Deep eutectic solvents (DESs) are environmental-friendly, cheap, and highly tunable, with high solubility, which renders them potential applications in biomass pretreatment and conversion. They could be used as solvents or catalysts and so on. This paper intends to review the application of DESs for the pretreatment of biomass and conversion of biomass to value-added products. We focus on the following topics related to biomass and DESs: (1) DESs for the pretreatment of biomass; (2) DESs for the dissolution and separation of biomass or extraction of chemicals from biomass; (3) DESs for biomass conversion; (4) Drawbacks, and recyclability of DESs for pretreatment and conversion of biomass.
Biomass is renewable, abundant, cheap, biocompatible, and biodegradable materials and has been used to produce chemicals, materials, energy, and fuels. However, most of the biomass, especially most of the biomass polymers are not soluble in common solvents, which hinders their pretreatment and conversion. Deep eutectic solvents (DESs) are environmental-friendly, cheap, and highly tunable, with high solubility, which renders them potential applications in biomass pretreatment and conversion. They could be used as solvents or catalysts and so on. This paper intends to review the application of DESs for the pretreatment of biomass and conversion of biomass to value-added products. We focus on the following topics related to biomass and DESs: (1) DESs for the pretreatment of biomass; (2) DESs for the dissolution and separation of biomass or extraction of chemicals from biomass; (3) DESs for biomass conversion; (4) Drawbacks, and recyclability of DESs for pretreatment and conversion of biomass.
2020, 5(1): 8-21.
doi: 10.1016/j.gee.2019.03.002
Abstract:
This review divides the acidic deep eutectic solvents (ADES) into Brønsted and Lewis DES according to their diversity of acidic character. The hydrogen bond donors and halide salts for formulating an ADES are classified, the synthesis methods are described, and the physicochemical properties including freezing point, acidity, density, viscosity and conductivity are presented. Furthermore, the applications of Brønsted acidic deep eutectic solvents (BADES) and Lewis acidic deep eutectic solvents (LADES) are overviewed, respectively, covering the fields in dissolution, extraction, organic reaction and metal electrodeposition. It is expected that the ADES has great potential to replace the pollutional mineral acid, expensive and unstable solid acid, and costly ionic liquid in many acid-employed chemical processes, thus meeting the demands of green chemistry.
This review divides the acidic deep eutectic solvents (ADES) into Brønsted and Lewis DES according to their diversity of acidic character. The hydrogen bond donors and halide salts for formulating an ADES are classified, the synthesis methods are described, and the physicochemical properties including freezing point, acidity, density, viscosity and conductivity are presented. Furthermore, the applications of Brønsted acidic deep eutectic solvents (BADES) and Lewis acidic deep eutectic solvents (LADES) are overviewed, respectively, covering the fields in dissolution, extraction, organic reaction and metal electrodeposition. It is expected that the ADES has great potential to replace the pollutional mineral acid, expensive and unstable solid acid, and costly ionic liquid in many acid-employed chemical processes, thus meeting the demands of green chemistry.
2017, 2(3): 218-245.
doi: 10.1016/j.gee.2017.05.003
Abstract:
Metal organic frameworks (MOFs) represent a class of porous material which is formed by strong bonds between metal ions and organic linkers. By careful selection of constituents, MOFs can exhibit very high surface area, large pore volume, and excellent chemical stability. Research on synthesis, structures and properties of various MOFs has shown that they are promising materials for many applications, such as energy storage, gas storage, heterogeneous catalysis and sensing. Apart from direct use, MOFs have also been used as support substrates for nanomaterials or as sacrificial templates/precursors for preparation of various functional nanostructures. In this review, we aim to present the most recent development of MOFs as precursors for the preparation of various nanostructures and their potential applications in energy-related devices and processes. Specifically, this present survey intends to push the boundaries and covers the literatures from the year 2013 to early 2017, on supercapacitors, lithium ion batteries, electrocatalysts, photocatalyst, gas sensing, water treatment, solar cells, and carbon dioxide capture. Finally, an outlook in terms of future challenges and potential prospects towards industrial applications are also discussed.
Metal organic frameworks (MOFs) represent a class of porous material which is formed by strong bonds between metal ions and organic linkers. By careful selection of constituents, MOFs can exhibit very high surface area, large pore volume, and excellent chemical stability. Research on synthesis, structures and properties of various MOFs has shown that they are promising materials for many applications, such as energy storage, gas storage, heterogeneous catalysis and sensing. Apart from direct use, MOFs have also been used as support substrates for nanomaterials or as sacrificial templates/precursors for preparation of various functional nanostructures. In this review, we aim to present the most recent development of MOFs as precursors for the preparation of various nanostructures and their potential applications in energy-related devices and processes. Specifically, this present survey intends to push the boundaries and covers the literatures from the year 2013 to early 2017, on supercapacitors, lithium ion batteries, electrocatalysts, photocatalyst, gas sensing, water treatment, solar cells, and carbon dioxide capture. Finally, an outlook in terms of future challenges and potential prospects towards industrial applications are also discussed.
2017, 2(3): 246-277.
doi: 10.1016/j.gee.2017.06.006
Abstract:
The aluminum–air battery is considered to be an attractive candidate as a power source for electric vehicles (EVs) because of its high theoretical energy density (8100 Wh kg−1), which is significantly greater than that of the state-of-the-art lithium-ion batteries (LIBs). However, some technical and scientific problems preventing the large-scale development of Al–air batteries have not yet to be resolved. In this review, we present the fundamentals, challenges and the recent advances in Al–air battery technology from aluminum anode, air cathode and electrocatalysts to electrolytes and inhibitors. Firstly, the alloying of aluminum with transition metal elements is reviewed and shown to reduce the self-corrosion of Al and improve battery performance. Additionally for the cathode, extensive studies of electrocatalytic materials for oxygen reduction/evolution including Pt and Pt alloys, nonprecious metal catalysts, and carbonaceous materials at the air cathode are highlighted. Moreover, for the electrolyte, the application of aqueous and nonaqueous electrolytes in Al–air batteries are discussed. Meanwhile, the addition of inhibitors to the electrolyte to enhance electrochemical performance is also explored. Finally, the challenges and future research directions are proposed for the further development of Al–air batteries.
The aluminum–air battery is considered to be an attractive candidate as a power source for electric vehicles (EVs) because of its high theoretical energy density (8100 Wh kg−1), which is significantly greater than that of the state-of-the-art lithium-ion batteries (LIBs). However, some technical and scientific problems preventing the large-scale development of Al–air batteries have not yet to be resolved. In this review, we present the fundamentals, challenges and the recent advances in Al–air battery technology from aluminum anode, air cathode and electrocatalysts to electrolytes and inhibitors. Firstly, the alloying of aluminum with transition metal elements is reviewed and shown to reduce the self-corrosion of Al and improve battery performance. Additionally for the cathode, extensive studies of electrocatalytic materials for oxygen reduction/evolution including Pt and Pt alloys, nonprecious metal catalysts, and carbonaceous materials at the air cathode are highlighted. Moreover, for the electrolyte, the application of aqueous and nonaqueous electrolytes in Al–air batteries are discussed. Meanwhile, the addition of inhibitors to the electrolyte to enhance electrochemical performance is also explored. Finally, the challenges and future research directions are proposed for the further development of Al–air batteries.
2018, 3(1): 20-41.
doi: 10.1016/j.gee.2017.10.001
Abstract:
Over the past decades, a series of aqueous rechargeable batteries (ARBs) were explored, investigated and demonstrated. Among them, aqueous rechargeable alkali-metal ion (Li+, Na+, K+) batteries, aqueous rechargeable-metal ion (Zn2+, Mg2+, Ca2+, Al3+) batteries and aqueous rechargeable hybrid batteries are standing out due to peculiar properties. In this review, we focus on the fundamental basics of these batteries, and discuss the scientific and/or technological achievements and challenges. By critically reviewing state-of-the-art technologies and the most promising results so far, we aim to analyze the benefits of ARBs and the critical issues to be addressed, and to promote better development of ARBs.
Over the past decades, a series of aqueous rechargeable batteries (ARBs) were explored, investigated and demonstrated. Among them, aqueous rechargeable alkali-metal ion (Li+, Na+, K+) batteries, aqueous rechargeable-metal ion (Zn2+, Mg2+, Ca2+, Al3+) batteries and aqueous rechargeable hybrid batteries are standing out due to peculiar properties. In this review, we focus on the fundamental basics of these batteries, and discuss the scientific and/or technological achievements and challenges. By critically reviewing state-of-the-art technologies and the most promising results so far, we aim to analyze the benefits of ARBs and the critical issues to be addressed, and to promote better development of ARBs.
2020, 5(1): 37-49.
doi: 10.1016/j.gee.2019.09.003
Abstract:
The most abundant natural biopolymer on earth, cellulose fiber, may offer a highly efficient, low-cost, and chemical-free option for wastewater treatment. Cellulose is widely distributed in plants and several marine animals. It is a carbohydrate polymer consisting of β-1,4-linked anhydro-D-glucose units with three hydroxyl groups per anhydroglucose unit (AGU). Cellulose-based materials have been used in food, industrial, pharmaceutical, paper, textile production, and in wastewater treatment applications due to their low cost, renewability, biodegradability, and non-toxicity. For water treatment in the oil and gas industry, cellulose-based materials can be used as adsorbents, flocculants, and oil/water separation membranes. In this review, the uses of cellulose-based materials for wastewater treatment in the oil & gas industry are summarized, and recent research progress in the following aspects are highlighted: crude oil spill cleaning, flocculation of solid suspended matter in drilling or oil recovery in the upstream oil industry, adsorption of heavy metal or chemicals, and separation of oil/water by cellulosic membrane in the downstream water treatment.
The most abundant natural biopolymer on earth, cellulose fiber, may offer a highly efficient, low-cost, and chemical-free option for wastewater treatment. Cellulose is widely distributed in plants and several marine animals. It is a carbohydrate polymer consisting of β-1,4-linked anhydro-D-glucose units with three hydroxyl groups per anhydroglucose unit (AGU). Cellulose-based materials have been used in food, industrial, pharmaceutical, paper, textile production, and in wastewater treatment applications due to their low cost, renewability, biodegradability, and non-toxicity. For water treatment in the oil and gas industry, cellulose-based materials can be used as adsorbents, flocculants, and oil/water separation membranes. In this review, the uses of cellulose-based materials for wastewater treatment in the oil & gas industry are summarized, and recent research progress in the following aspects are highlighted: crude oil spill cleaning, flocculation of solid suspended matter in drilling or oil recovery in the upstream oil industry, adsorption of heavy metal or chemicals, and separation of oil/water by cellulosic membrane in the downstream water treatment.
2022, 7(1): 3-15.
doi: 10.1016/j.gee.2020.12.023
Abstract:
In recent years, an increasing amount of interest has been dedicated to the synthesis and application of ZIF-67-based materials due to their exceptionally high surface area, tunable porosity, and excellent thermal and chemical stabilities. This review summarizes the latest strategies of synthesizing ZIF-67-based materials by exploring the prominent examples. Then, the recent progress in the applications of ZIF-67-based materials in heterogeneous catalysis, including catalysis of the redox reactions, addition reactions, esterification reactions, Knoevenagel condensations, and hydrogenation-dehydrogenation reactions, has been elaborately discussed. Finally, we end this work by shedding some light on the large-scale industrial production of ZIF-67-based materials and their applications in the future.
In recent years, an increasing amount of interest has been dedicated to the synthesis and application of ZIF-67-based materials due to their exceptionally high surface area, tunable porosity, and excellent thermal and chemical stabilities. This review summarizes the latest strategies of synthesizing ZIF-67-based materials by exploring the prominent examples. Then, the recent progress in the applications of ZIF-67-based materials in heterogeneous catalysis, including catalysis of the redox reactions, addition reactions, esterification reactions, Knoevenagel condensations, and hydrogenation-dehydrogenation reactions, has been elaborately discussed. Finally, we end this work by shedding some light on the large-scale industrial production of ZIF-67-based materials and their applications in the future.
2022, 7(4): 578-605.
doi: 10.1016/j.gee.2021.04.006
Abstract:
As an aromatic polymer in nature, lignin has recently attracted gross attention because of its advantages of high carbon content, low cost and bio-renewability. However, most lignin is directly burnt for power generation to satisfy the energy demand of the pulp mills. As a result, only a handful of isolated lignin is used as a raw material. Thus, increasing value addition on lignin to expand its scope of applications is currently a challenge demanding immediate attention. Many efforts have been made in the valorization of lignin, including the preparation of precursors for carbon fibers. However, its complex structure and diversity significantly restrict the spinnability of lignin. In this review, we provide elaborate knowledge on the preparation of lignin-based carbon fibers ranging from the relationships among chemical structures, formation conditions and properties of fibers, to their potential applications. Specifically, control procedures for different spinning methods of lignin, including melt spinning, solution spinning and electrospinning, together with stabilization and carbonization are deeply discussed to provide an overall understanding towards the formation of lignin-based carbon fibers. We also offer perspectives on the challenges and new directions for future development of lignin-based carbon fibers.
As an aromatic polymer in nature, lignin has recently attracted gross attention because of its advantages of high carbon content, low cost and bio-renewability. However, most lignin is directly burnt for power generation to satisfy the energy demand of the pulp mills. As a result, only a handful of isolated lignin is used as a raw material. Thus, increasing value addition on lignin to expand its scope of applications is currently a challenge demanding immediate attention. Many efforts have been made in the valorization of lignin, including the preparation of precursors for carbon fibers. However, its complex structure and diversity significantly restrict the spinnability of lignin. In this review, we provide elaborate knowledge on the preparation of lignin-based carbon fibers ranging from the relationships among chemical structures, formation conditions and properties of fibers, to their potential applications. Specifically, control procedures for different spinning methods of lignin, including melt spinning, solution spinning and electrospinning, together with stabilization and carbonization are deeply discussed to provide an overall understanding towards the formation of lignin-based carbon fibers. We also offer perspectives on the challenges and new directions for future development of lignin-based carbon fibers.
2023, 8(4): 972-988.
doi: 10.1016/j.gee.2022.02.002
Abstract:
Developing multifunctional energy storage systems with high specific energy, high specific power and long cycling life has been the one of the most important research directions. Compared to batteries and traditional capacitors, supercapacitors possess more balanced performance with both high specific power and long cycle-life. Nevertheless, regular supercapacitors can only achieve energy storage without harvesting energy and the energy density is still not very high compared to batteries. Therefore, combining high specific energy and high specific power, long cycle-life and even fast self-charging into one cell has been a promising direction for future energy storage devices. The multifunctional hybrid supercapacitors like asymmetric supercapacitors, batteries/supercapacitors hybrid devices and self-charging hybrid supercapacitors have been widely studied recently. Carbon based electrodes are common materials used in all kinds of energy storage devices due to their fabulous electrical and mechanical properties. In this survey, the research progress of all kinds of hybrid supercapacitors using multiple effects and their working mechanisms are briefly reviewed. And their advantages and disadvantages are discussed. The hybrid supercapacitors have great application potential for portable electronics, wearable devices and implantable devices in the future.
Developing multifunctional energy storage systems with high specific energy, high specific power and long cycling life has been the one of the most important research directions. Compared to batteries and traditional capacitors, supercapacitors possess more balanced performance with both high specific power and long cycle-life. Nevertheless, regular supercapacitors can only achieve energy storage without harvesting energy and the energy density is still not very high compared to batteries. Therefore, combining high specific energy and high specific power, long cycle-life and even fast self-charging into one cell has been a promising direction for future energy storage devices. The multifunctional hybrid supercapacitors like asymmetric supercapacitors, batteries/supercapacitors hybrid devices and self-charging hybrid supercapacitors have been widely studied recently. Carbon based electrodes are common materials used in all kinds of energy storage devices due to their fabulous electrical and mechanical properties. In this survey, the research progress of all kinds of hybrid supercapacitors using multiple effects and their working mechanisms are briefly reviewed. And their advantages and disadvantages are discussed. The hybrid supercapacitors have great application potential for portable electronics, wearable devices and implantable devices in the future.
2024, 9(9): 1366-1383.
doi: 10.1016/j.gee.2023.10.002
Abstract:
The increasing atmospheric carbon dioxide (CO2) concentration has exposed a series of crises in the earth's ecological environment. How to effectively fix and convert carbon dioxide into products with added value has attracted the attention of many researchers. Cell-free enzyme catalytic system coupled with electrical and light have been a promising attempt in the field of biological carbon fixation in recent years. In this review, the research progresses of photoenzyme catalysis, electroenzyme catalysis and photo-electroenzyme catalysis for converting carbon dioxide into chemical products in cell-free systems are systematically summarized. We focus on reviewing and comparing various coupling methods and principles of photoenzyme catalysis and electroenzyme catalysis in cell-free systems, especially the materials used in the construction of the coupling system, and analyze and point out the characteristics and possible problems of different coupling methods. Finally, we discuss the major challenges and prospects of coupling physical signals and cell-free enzymatic catalytic systems in the field of CO2 fixation, suggesting possible strategies to improve the carbon sequestration capacity of such systems.
The increasing atmospheric carbon dioxide (CO2) concentration has exposed a series of crises in the earth's ecological environment. How to effectively fix and convert carbon dioxide into products with added value has attracted the attention of many researchers. Cell-free enzyme catalytic system coupled with electrical and light have been a promising attempt in the field of biological carbon fixation in recent years. In this review, the research progresses of photoenzyme catalysis, electroenzyme catalysis and photo-electroenzyme catalysis for converting carbon dioxide into chemical products in cell-free systems are systematically summarized. We focus on reviewing and comparing various coupling methods and principles of photoenzyme catalysis and electroenzyme catalysis in cell-free systems, especially the materials used in the construction of the coupling system, and analyze and point out the characteristics and possible problems of different coupling methods. Finally, we discuss the major challenges and prospects of coupling physical signals and cell-free enzymatic catalytic systems in the field of CO2 fixation, suggesting possible strategies to improve the carbon sequestration capacity of such systems.
2017, 2(1): 51-57.
doi: 10.1016/j.gee.2017.01.002
Abstract:
In this work, with the purpose to explore the coordination chemistry of calcium complexes which could work as a partial model of manganese–calcium cluster, a spectrophotometric study to evaluate the stability of the complexes: Calcium(II)-1,2-ethylendiamine, Calcium(II)-1,3-propanediamine and Calcium(II)-1,4-butanediamine in acetonitrile, were carried on. By processing the spectrophotometric data with the HypSpec program allows the determination of the formation constants. The logarithmic values of the formation constants obtained for Calcium(II)-1,2-ethylendiamine, Calcium(II)-1,3-propanediamine and Calcium(II)-1,4-butanediamine were log β110 = 4.69, log β110 = 5.25 and log β110 = 4.072, respectively.
In this work, with the purpose to explore the coordination chemistry of calcium complexes which could work as a partial model of manganese–calcium cluster, a spectrophotometric study to evaluate the stability of the complexes: Calcium(II)-1,2-ethylendiamine, Calcium(II)-1,3-propanediamine and Calcium(II)-1,4-butanediamine in acetonitrile, were carried on. By processing the spectrophotometric data with the HypSpec program allows the determination of the formation constants. The logarithmic values of the formation constants obtained for Calcium(II)-1,2-ethylendiamine, Calcium(II)-1,3-propanediamine and Calcium(II)-1,4-butanediamine were log β110 = 4.69, log β110 = 5.25 and log β110 = 4.072, respectively.
2017, 2(3): 246-277.
doi: 10.1016/j.gee.2017.06.006
Abstract:
The aluminum–air battery is considered to be an attractive candidate as a power source for electric vehicles (EVs) because of its high theoretical energy density (8100 Wh kg−1), which is significantly greater than that of the state-of-the-art lithium-ion batteries (LIBs). However, some technical and scientific problems preventing the large-scale development of Al–air batteries have not yet to be resolved. In this review, we present the fundamentals, challenges and the recent advances in Al–air battery technology from aluminum anode, air cathode and electrocatalysts to electrolytes and inhibitors. Firstly, the alloying of aluminum with transition metal elements is reviewed and shown to reduce the self-corrosion of Al and improve battery performance. Additionally for the cathode, extensive studies of electrocatalytic materials for oxygen reduction/evolution including Pt and Pt alloys, nonprecious metal catalysts, and carbonaceous materials at the air cathode are highlighted. Moreover, for the electrolyte, the application of aqueous and nonaqueous electrolytes in Al–air batteries are discussed. Meanwhile, the addition of inhibitors to the electrolyte to enhance electrochemical performance is also explored. Finally, the challenges and future research directions are proposed for the further development of Al–air batteries.
The aluminum–air battery is considered to be an attractive candidate as a power source for electric vehicles (EVs) because of its high theoretical energy density (8100 Wh kg−1), which is significantly greater than that of the state-of-the-art lithium-ion batteries (LIBs). However, some technical and scientific problems preventing the large-scale development of Al–air batteries have not yet to be resolved. In this review, we present the fundamentals, challenges and the recent advances in Al–air battery technology from aluminum anode, air cathode and electrocatalysts to electrolytes and inhibitors. Firstly, the alloying of aluminum with transition metal elements is reviewed and shown to reduce the self-corrosion of Al and improve battery performance. Additionally for the cathode, extensive studies of electrocatalytic materials for oxygen reduction/evolution including Pt and Pt alloys, nonprecious metal catalysts, and carbonaceous materials at the air cathode are highlighted. Moreover, for the electrolyte, the application of aqueous and nonaqueous electrolytes in Al–air batteries are discussed. Meanwhile, the addition of inhibitors to the electrolyte to enhance electrochemical performance is also explored. Finally, the challenges and future research directions are proposed for the further development of Al–air batteries.
2024, 9(9): 1459-1465.
doi: 10.1016/j.gee.2023.09.002
Abstract:
To improve the electrocatalytic transformation of carbon dioxide (CO2) to multi-carbon (C2+) products is of great importance. Here we developed a nitrogen-doped Cu catalyst, by which the maximum C2+ Faradaic efficiency can reach 72.7% in flow-cell system, with the partial current density reaching 0.62 A cm-2. The in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst, thus promoting the *CO utilization in the subsequent C-C coupling step. Simultaneously, the water activation can be well enhanced by N doping on Cu catalyst. Owing to the synergistic effects, the selectivity and activity for C2+ products over the N-deoped Cu catalyst are much improved.
To improve the electrocatalytic transformation of carbon dioxide (CO2) to multi-carbon (C2+) products is of great importance. Here we developed a nitrogen-doped Cu catalyst, by which the maximum C2+ Faradaic efficiency can reach 72.7% in flow-cell system, with the partial current density reaching 0.62 A cm-2. The in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst, thus promoting the *CO utilization in the subsequent C-C coupling step. Simultaneously, the water activation can be well enhanced by N doping on Cu catalyst. Owing to the synergistic effects, the selectivity and activity for C2+ products over the N-deoped Cu catalyst are much improved.
2023, 8(2): 351-353.
doi: 10.1016/j.gee.2022.06.002
Abstract:
Under the context of carbon neutrality of China, it is urgent to shift our energy supply towards cleaner fuels as well as to reduce the greenhouse gas emission. Currently, coal is the main fossil fuel energy source of China. The country is striving hard to replace it with methane, a cleaner fossil fuel. Although China has rich geological resources of methane as coal bed methane (CBM) reserves, it is quite challenging to utilize them due to low concentration. The CBM is however mainly emitted directly to atmosphere during coal mining, causing waste of the resource and huge contribution to greenhouse effect. The recent work by Yang et al. demonstrated a potential solution to extract low concentration methane selectively from CBM through using MOF materials as sorbents. Such kind of materials and associated separation technology are promising to reduce greenhouse gas emission and promote the methane production capability, which would contribute to carbon neutrality in dual pathways.
Under the context of carbon neutrality of China, it is urgent to shift our energy supply towards cleaner fuels as well as to reduce the greenhouse gas emission. Currently, coal is the main fossil fuel energy source of China. The country is striving hard to replace it with methane, a cleaner fossil fuel. Although China has rich geological resources of methane as coal bed methane (CBM) reserves, it is quite challenging to utilize them due to low concentration. The CBM is however mainly emitted directly to atmosphere during coal mining, causing waste of the resource and huge contribution to greenhouse effect. The recent work by Yang et al. demonstrated a potential solution to extract low concentration methane selectively from CBM through using MOF materials as sorbents. Such kind of materials and associated separation technology are promising to reduce greenhouse gas emission and promote the methane production capability, which would contribute to carbon neutrality in dual pathways.
Editor-in-Chief：Buxing Han
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