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2025 Vol. 10, No. 10

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Nanocatalysis: Towards high-performance energy and environmental materials for achieving circular carbon economy
Heterointerface of nickel-ferric hydroxide/cobalt-phosphide-boride boosting hydrazine-assisted water electrolysis
Jiayi Wang, Shaojun Qing, Xili Tong, Ting Xiang, Guangnan Luo, Kun Zhang, Liangji Xu
2025, 10(10): 1957-1967. doi: 10.1016/j.gee.2024.10.003
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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.
2D/2D homojunction-mediated charge separation: Synergistic effect of crystalline C3N5 and g-C3N4 via electrostatic self-assembly for photocatalytic hydrogen and benzaldehyde production
Sue-Faye Ng, Joel Jie Foo, Peipei Zhang, Steven Hao Wan Kok, Lling-Lling Tan, Binghui Chen, Wee-Jun Ong
2025, 10(10): 1968-1980. doi: 10.1016/j.gee.2024.06.008
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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.
Construction of two-dimensional heterojunctions based on metal-free semiconductor materials and Covalent Organic Frameworks for exceptional solar energy catalysis
Haijun Hu, Daming Feng, Kailai Zhang, Hui Li, Hongge Pan, Hongwei Huang, Xiaodong Sun, Tianyi Ma
2025, 10(10): 1981-1989. doi: 10.1016/j.gee.2024.09.001
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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.
1T-MoS2 nanosheets with enlarged interlayer spacing vertically bonded on rGO for high-performance lithium-ion capacitors
Wenjun Zhu, Bofeng Zhang, Fanxing Bu, Minghai Zhao, Xinyong Tao, Keli Liu, Yuwen Fang, Wei Luo
2025, 10(10): 1990-2001. doi: 10.1016/j.gee.2025.05.003
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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.
Lattice sulfur-induced disordered and electron-deficient Pd-based nanosheets enabling selective electrocatalytic semi-hydrogenation of alkynes
Hongyao Luo, Haochuan Jing, Bing Zhang, Nailiang Yang, Tao Sun, Chuntian Qiu, Yangsen Xu, Peng Yang, Xiang Ling
2025, 10(10): 2002-2013. doi: 10.1016/j.gee.2025.07.003
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The semi-hydrogenation of alkynes to alkenes is of great significance in the industrial production of pharmaceutical and fine chemicals. Electrochemical semi-hydrogenation (ECSH) has emerged as a promising alternative to conventional thermochemical hydrogenation. However, its practical application is hindered by low reaction rate and competing hydrogen evolution reaction (HER). In this work, the controllable incorporation of sulfur into the lattice of Pd nanostructures is proposed to develop disordered and electron-deficient Pd-based nanosheets on Ni foam and enhance their ECSH performance of alkynes. Mechanistic investigations demonstrate that the electronic and geometric structures of Pd sites are optimized by lattice sulfur, which tunes the competitive adsorption of H* and alkynes, inherently inhibits the H* coupling and weakens alkene adsorption, thereby promotes the semi-hydrogenation of alkynes and prevents the over-hydrogenation of alkenes. The optimized Pd-based nanosheets exhibit efficient electrocatalytic semi-hydrogenation performance in an H-cell, achieving 97% alkene selectivity, 94% Faradaic efficiency, and a reaction rate of 303.7 μmol mgcatal-1. h-1 using 4-methoxyphenylacetylene as the model substrate. Even in a membrane electrode assembly (MEA) configuration, the optimized Pd-based nanosheets achieves a single-cycle alkyne conversion of 96% and an alkene selectivity of 97%, with continuous production of alkene at a rate of 1901.1 μmol mgcatal-1. h-1. The potential- and time-independent selectivity, good substrate universality with excellent tolerance to active groups (C-Br/Cl/C＝O, etc.) further highlight the potential of this strategy for advanced catalysts design and green chemistry.
Review articles
Advancements in catalytic hydrogenation of nitrocyclohexane to cyclohexanone oxime
Jinzhi Lu, Tongxin Song, Weiping Ding, Yan Zhu
2025, 10(10): 2014-2028. doi: 10.1016/j.gee.2025.05.007
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Cyclohexanone oxime serves as a crucial intermediate in the synthesis of caprolactam, which is an essential precursor for manufacturing nylon fibers, high-performance engineering plastics, and specialized plastic films. Catalytic hydrogenation of nitrocyclohexane to cyclohexanone oxime has been documented to be an atom-economical, green and environmentally friendly process. In this review, we first introduce the current design rules of catalysts for catalytic hydrogenation of nitrocyclohexane in terms of both active metals and supports. Secondly, we discuss the influence of solvent effects on the cyclohexanone oxime from the nitrocyclohexane conversion. In addition, we concisely discuss typically proposed reaction pathways for the hydrogenation of nitrocyclohexane to produce cyclohexanone oxime. Finally, we provide our perspectives on some issues for catalytic conversion of nitrocyclohexane to cyclohexanone oxime in the future.
Recent advances in cellulose-based separators for zinc-based batteries: Performances, mechanism and perspectives
Zekun Zhang, Yongjun Li, Xuejing Yin, Siwen Li, Bin Li, Ningning Zhao, Jing Zhu, Lei Dai, Ling Wang, Zhangxing He, Zemin Feng
2025, 10(10): 2029-2046. doi: 10.1016/j.gee.2025.03.010
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Zinc-based batteries have attracted widespread attention due to their inherent safety, notable cost-effectiveness and consistent performance, etc. However, the advancement of zinc-based battery technology encounters significant challenges, including the formation of zinc dendrites and irreversible side reactions. Separators are vital in batteries due to their role in preventing electrode contact and facilitating rapid movement of ions within the electrolyte. The incorporation of cellulose in batteries enables uniform ion transport and a stable electric field, attributed to its excellent hydrophilicity, strong mechanical strength, and abundant active sites. Herein, the latest research progress of cellulose-based separators on various zinc-based batteries is systematically summarized. To begin with, the accomplishments and inherent limitations of traditional separators are clarified. Next, it underscores the advantages of cellulose-based materials in battery technology, thoroughly examining their utilization and merits as separators in zinc-based batteries. Lastly, the review offers prospective insights into the future trajectory of cellulose-based separators in zinc-based batteries. Through a comprehensive analysis of the present landscape, the review establishes a framework for the future design and enhancement of cellulose-based separators, thereby fostering the progression of associated industries.
Factors affecting the performance of membranes for H2/CH4 separation from the perspective of separation mechanisms
Shiyin Sun, Shuangde Li, Yunfa Chen
2025, 10(10): 2047-2070. doi: 10.1016/j.gee.2025.04.002
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The production of high-purity H2 is the building block of hydrogen economy, which can greatly promote the construction of related technologies and infrastructure. Efficient H2/CH4 separation is a necessary unit in producing high-purity energy and reducing greenhouse gas emissions, which can meet the industrial demand and help to address the energy issue and achieve global carbon neutrality goals. Membrane separation technology, as a promising strategy for H2 purification, has attracted much attention due to its high efficiency, energy conservation and versatile applications. This article reviews the latest research advances in the high-performance membranes for H2/CH4 separation, and elucidates the effect of membrane materials, preparation methods and membrane structure on separation performance from the perspective of separation mechanisms. It also summarized the essential aspects of membrane design, such as microstructural regulation, multiphase coupling, the optimal usage conditions and simple analysis of economic benefits. Finally, the current challenges and future directions of membranes for H2/CH4 separation were discussed, intending to provide in-depth reference and inspiration for the theoretical research and practical application of membrane separation technology.
Research papers
Constructing S-scheme 3D Zn3In2S6/ReS2 heterojunction photocatalyst for simultaneous organic pollutants degradation and hydrogen production
Qi Gao, Tiantian Wang, Liangmeng Ni, Zhenrui Li, Xia Du, Shaowen Rong, Hui Wang, Liquan Jing, Zhijia Liu, Jinguang Hu
2025, 10(10): 2071-2085. doi: 10.1016/j.gee.2025.04.007
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Controlling efficient interfacial charge transfer is crucial for developing advanced photocatalysts. This study successfully developed a bifunctional photocatalyst with an S-scheme heterojunction by incorporating ReS2 into the Zn3In2S6 (ZIS) nanoflower structure, enabling the organic pollutants degradation and synergistic hydrogen production. The optimized ZIS/ReS2-1% exhibited exceptional photocatalytic efficiency, reaching a 97.7% degradation rate of ibuprofen (IBP) within 2 h, along with a hydrogen generation rate of 1.84 mmol/g/h. The degradation efficiency and hydrogen generation rate were 1.78 and 5.75 times greater than those of Zn3In2S6, respectively. Moreover, ZIS/ReS2-1% demonstrated excellent catalytic degradation abilities for various organic pollutants such as ciprofloxacin, amoxicillin, norfloxacin, levofloxacin, ofloxacin, sulfamethoxazole, and tetracycline, while also showing good synergistic hydrogen production efficiency. Electron spin resonance and radical scavenging experiments verified that h+, ·O2-, and ·OH were the primary reactive species responsible for IBP degradation. The superior photocatalytic performance of the ZIS/ReS2-1% was mainly attributed to its broad and intense absorption of visible light, effective separation of charge carriers, and enhanced redox capabilities. The degradation pathway of IBP was unveiled through Fukui function and liquid chromatography-mass spectrometry, and the toxicity of the degradation intermediates was also examined. In-situ XPS and density functional theory (DFT) calculations confirmed the existence of S-scheme heterojunction. This study provided a new pathway for simultaneously achieving organic pollutant treatment and energy conversion.
Construction of hollow porous lychee-structured Ni/C/ZnFe2O4 microwave-responsive catalysts with rapid efficiently reduction of Cr(VI) ions
Gaoqian Yuan, Ling Zhang, Jingzhe Zhang, Long Dong, Xuefeng Liu, Yage Li, Liang Huang, Faliang Li, Haijun Zhang
2025, 10(10): 2086-2096. doi: 10.1016/j.gee.2025.04.008
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Designing catalysts with high reaction efficiency is essential for reducing heavy metal Cr(VI) ions in wastewater via microwave induction. In this paper, a unique microwave-responsive lychee-like Ni/C/ZnFe2O4 composite catalyst with a double-shell hollow porous heterojunction structure was constructed for the efficient reduction of Cr(VI). Benefiting from the novel hollow porous structure and “carbon nanocage” structure of the Ni/C/ZnFe2O4, coupled with excellent electromagnetic wave absorption ability, the prepared lychee-like Ni/C/ZnFe2O4 composite catalyst could remove up to 98% of Cr(VI) (50 mg L-1, 50 mL) after 40 min of microwave irradiation, even in nearly neutral water conditions. Additionally, density functional theory calculations indicated that the heterojunction interface between Ni/C and ZnFe2O4 enhances electron transfer from ZnFe2O4 to Ni/C, ultimately facilitating the removal of Cr(VI). Furthermore, the incorporation of Ni/C facilitated the acceleration of H ion transfer to *Cr2O72-, thereby expediting the conversion kinetics of the latter. This research aims to establish a theoretical and experimental foundation for the effective and stable microwave-assisted catalytic reduction of heavy metal Cr(VI) ions, presenting new insights and methods to combat heavy metal contamination.
Single-atom Mn-modified biomimetic phthalocyanine covalent organic frameworks with tunable pendant groups for high-efficiency sodium chloride batteries
Jiajun Cui, Zhenzhen Wang, Yongqiang Gu, Ting Xu, Tairan Pang, Chuanling Si, Weiwei Huan, Jie Li
2025, 10(10): 2097-2105. doi: 10.1016/j.gee.2025.06.002
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Rechargeable chlorine-based battery recently emerged as a promising substitute for energy storage systems due to their high average operating voltage (~3.7 V) and large theoretical capacity of ~754.9 mAh g-1. However, insufficient supply of chlorine (Cl2) and sluggish oxidation of NaCl to Cl2 limit its practical application. Covalent Organic Frameworks (COFs) have the potential to be ideal Cl2 host materials as Cl2 adsorbents for their abundant porosity and easily modifiable nature. In this work, the single atom Mn coordinated biomimetic phthalocyanine COFs are used for Cl2 capture and catalyst. The DFT reveals that ASMn and -NH2 significantly change the microenvironment around the active site, effectively promoting the oxidation of NaCl. When applied as the cathode material for Na-Cl2 batteries, the SAMn-COFs-NH2 electrode exhibits large reversible capacities and excellent high-rate cycling performances throughout 200 cycles based on the mechanism of highly reversible NaCl/Cl2 redox reactions. Even at the temperature as low as -40 ℃, the SAMn-COFs-NH2 cathode showed stable discharge capacities at ~1000 mAh g-1 over 50 cycles with a voltage plateau of ~3.3 V. This work may provide new insights for the investigation of chlorine-based electrochemical redox mechanisms and the design of green nanoscaled electrodes for high-property chlorine-based batteries.

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