2024 Vol. 9, No. 6

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Short Communication
Construction of Pd-doped RuO2 nanosheets for efficient and stable acidic water oxidation
Yibo Liu, Xing Hu, Chenxi Liu, Shan Zhu, Kezhu Jiang, Feng Liu, Shijian Zheng
2024, 9(6): 937-948. doi: 10.1016/j.gee.2023.12.003
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RuO2 has been considered a potential alternative to commercial IrO2 for the oxygen evolution reaction (OER) due to its superior intrinsic activity. However, its inherent structure dissolution in acidic environments restricts its commercial applications. In this study, we report a novel Pd-doped ruthenium oxide (Pd-RuO2) nanosheet catalyst that exhibits improved activity and stability through a synergistic effect of Pd modulation of Ru electronic structure and the two-dimensional structure. The catalyst exhibits excellent performance, achieving an overpotential of only 204 mV at a current density of 10 mA cm-2. Impressively, after undergoing 8000 cycles of cyclic voltammetry testing, the overpotential merely decreased by 5 mV. The PEM electrolyzer with Pd0.08Ru0.92O2 as an anode catalyst survived an almost 130 h operation at 200 mA cm-2. To elucidate the underlying mechanisms responsible for the enhanced stability, we conducted an X-ray photoelectron spectroscopy (XPS) analysis, which reveals that the electron transfer from Pd to Ru effectively circumvents the over-oxidation of Ru, thus playing a crucial role in enhancing the catalyst's stability. Furthermore, density functional theory (DFT) calculations provide compelling evidence that the introduction of Pd into RuO2 effectively modulates electron correlations and facilitates the electron transfer from Pd to Ru, thereby preventing the over-oxidation of Ru. Additionally, the application of the two-dimensional structure effectively inhibited the aggregation and growth of nanoparticles, further bolstering the structural integrity of the catalyst.
Review article
Advantageous properties of halide perovskite quantum dots towards energy-efficient sustainable applications
Qian Zhao, Shuo Wang, Young-Hoon Kim, Shekhar Mondal, Qingqing Miao, Simiao Li, Danya Liu, Miao Wang, Yaxin Zhai, Jianbo Gao, Abhijit Hazarika, Guo-Ran Li
2024, 9(6): 949-965. doi: 10.1016/j.gee.2023.04.001
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As lead halide perovskite (LHP) semiconductors have shown tremendous promise in many application fields, and particularly made strong impact in the solar photovoltaic area, low dimensional quantum dot forms of these perovskites are showing the potential to make distinct marks in the fields of electronics, optoelectronics and photonics. The so-called perovskite quantum dots (PQDs) not only possess the most important features of LHP materials, i.e., the unusual high defect tolerance, but also demonstrate clear quantum size effects, along with exhibiting desirable optoelectronic properties such as near perfect photoluminescent quantum yield, multiple exciton generation and slow hot-carrier cooling. Here, we review the advantageous properties of these nanoscale perovskites and survey the prospects for diverse applications which include light-emitting devices, solar cells, photocatalysts, lasers, detectors and memristors, emphasizing the distinct superiorities as well as the challenges.
Reviewing electrochemical stability of ionic liquids-/deep eutectic solvents-based electrolytes in lithium-ion, lithium-metal and post-lithium-ion batteries for green and safe energy
Yu Chen, Shuzi Liu, Zixin Bi, Zheng Li, Fengyi Zhou, Ruifen Shi, Tiancheng Mu
2024, 9(6): 966-991. doi: 10.1016/j.gee.2023.05.002
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Sustainable energy is the key issue for the environment protection, human activity and economic development. Ionic liquids (ILs) and deep eutectic solvents (DESs) are dogmatically regarded as green and sustainable electrolytes in lithium-ion, lithium-metal (e.g., lithium-sulphur, lithium-oxygen) and post-lithium-ion (e.g., sodium-ion, magnesium-ion, and aluminum-ion) batteries. High electrochemical stability of ILs/DESs is one of the prerequisites for green, sustainable and safe energy; while easy electrochemical decomposition of ILs/DESs would be contradictory to the concept of green chemistry by adding the cost, releasing volatile/hazardous by-products and hindering the recyclability. However, (1) are ILs/DESs-based electrolytes really electrochemically stable when they are not used in batteries? (2) are ILs/DESs-based electrolytes really electrochemically stable in real batteries? (3) how to design ILs/DESs-based electrolytes with high electrochemical stability for batteries to achieve sustainability and green development? Up to now, there is no summary on this topic, to the best of our knowledge. Here, we review the effect of chemical structure and non-structural factors on the electrochemical stability of ILs/DESs in simulated conditions. More importantly, electrochemical stability of ILs/DESs in real lithium-ion, lithium-metal and post-lithium-ion batteries is concluded and compared. Finally, the strategies to improve the electrochemical stability of ILs/DESs in lithium-ion, lithium-metal and post-lithium-ion batteries are proposed. This review would provide a guide to design ILs/DESs with high electrochemical stability for lithium-ion, lithium-metal and post-lithium-ion batteries to achieve sustainable and green energy.
Progress of semitransparent emerging photovoltaics for building integrated applications
Zhisheng Zhou, Zhangyu Yuan, Zhipeng Yin, Qifan Xue, Ning Li, Fei Huang
2024, 9(6): 992-1015. doi: 10.1016/j.gee.2023.05.006
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With the rapid development of emerging photovoltaics technology in recent years, the application of building-integrated photovoltaics (BIPVs) has attracted the research interest of photovoltaic communities. To meet the practical application requirements of BIPVs, in addition to the evaluation indicator of power conversion efficiency (PCE), other key performance indicators such as heat-insulating ability, average visible light transmittance (AVT), color properties, and integrability are equally important. The traditional Si-based photovoltaic technology is typically limited by its opaque properties for application scenarios where transparency is required. The emerging PV technologies, such as organic and perovskite photovoltaics are promising candidates for BIPV applications, owing to their advantages such as high PCE, high AVT, and tunable properties. At present, the PCE of semitransparent perovskite solar cells (ST-PSCs) has attained 14% with AVT of 22-25%; for semitransparent organic solar cells (ST-OSCs), the PCE reached 13% with AVT of almost 40%. In this review article, we summarize recent advances in material selection, optical engineering, and device architecture design for high-performance semitransparent emerging PV devices, and discuss the application of optical modeling, as well as the challenges of commercializing these semitransparent solar cells for building-integrated applications.
Research paper
Mapping out the reaction network of humin formation at the initial stage of fructose dehydration in water
Xing Fu, Yexin Hu, Ping Hu, Hui Li, Shuguang Xu, Liangfang Zhu, Changwei Hu
2024, 9(6): 1016-1026. doi: 10.1016/j.gee.2022.09.012
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The formation of humins hampers the large-scale production of 5-hydroxymethylfurfural (HMF) in biorefinery. Here, a detailed reaction network of humin formation at the initial stage of fructose-to-HMF dehydration in water is delineated by combined experimental, spectroscopic, and theoretical studies. Three bimolecular reaction pathways to build up soluble humins are demonstrated. That is, the intermolecular etherification of β-furanose at room temperature initiates the C12 path, whereas the C-C cleavage of α-furanose at 130-150 ℃ leads to C11 path, and that of open-chain fructose at 180 ℃ to C11' path. The successive intramolecular dehydrations and condensations of the as-formed bimolecular intermediates lead to three types of soluble humins. We show that the C12 path could be restrained by using HCl or AlCl3 catalyst, and both the C12 and C11' paths could be effectively inhibited by adding THF as a co-solvent or accelerating heating rate via microwave heating.
An efficient recycling strategy to eliminate the residual “impurities” while heal the damaged structure of spent graphite anodes
Dan Yang, Ying Yang, Haoran Du, Yongsheng Ji, Mingyuan Ma, Yujun Pan, Xiaoqun Qi, Quan Sun, Kaiyuan Shi, Long Qie
2024, 9(6): 1027-1034. doi: 10.1016/j.gee.2022.11.003
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The recycling of graphite from spent lithium-ion batteries (LIBs) is overlooked due to its relatively low added value and the lack of efficient recovering methods. To reuse the spent graphite anodes, we need to eliminate their useless components (mainly the degraded solid electrolyte interphase, SEI) and reconstruct their damaged structure. Herein, a facile and efficient strategy is proposed to recycle the spent graphite on the basis of the careful investigation of the composition of the cycled graphite anodes and the rational design of the regeneration processes. The regenerated graphite, which is revitalized by calcination treatment and acid leaching, delivers superb rate performance and a high specific capacity of 370 mAh g-1 (∼99% of its theoretical capacity) after 100 cycles at 0.1 C, superior to the commercial graphite anodes. The improved electrochemical performance could be attributed to unchoked Li+ transport channels and enhanced charge transfer reaction due to the effective destruction of the degraded SEI and the full recovery of the damaged structure of the spent graphite. This work clarifies that the electrochemical performance of the regenerated graphite could be deteriorated by even a trace amount of the residual “impurity” and provides a facile method for the efficient regeneration of graphite anodes.
Reversible solid-liquid conversion enabled by self-capture effect for stable non-flow zinc-bromine batteries
Xixi Zhang, Xiaoke Wang, Guangmeng Qu, Tairan Wang, Xiliang Zhao, Jun Fan, Cuiping Han, Xijin Xu, Chunyi Zhi, Hongfei Li
2024, 9(6): 1035-1044. doi: 10.1016/j.gee.2022.11.007
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Non-flow aqueous zinc-bromine batteries without auxiliary components (e.g., pumps, pipes, storage tanks) and ion-selective membranes represent a cost-effective and promising technology for large-scale energy storage. Unfortunately, they generally suffer from serious diffusion and shuttle of polybromide (Br-, Br3-) due to the weak physical adsorption between soluble polybromide and host carbon materials, which results in low energy efficiency and poor cycling stability. Here, we develop a novel self-capture organic bromine material (1,1'-bis [3-(trimethylammonio)propyl]-4,4'-bipyridinium bromine, NVBr4) to successfully realize reversible solid complexation of bromide components for stable non-flow zinc-bromine battery applications. The quaternary ammonium groups (NV4+ ions) can effectively capture the soluble polybromide species based on strong chemical interaction and realize reversible solid complexation confined within the porous electrodes, which transforms the conventional “liquid-liquid” conversion of soluble bromide components into “liquid-solid” model and effectively suppresses the shuttle effect. Thereby, the developed non-flow zinc-bromide battery provides an outstanding voltage platform at 1.7 V with a notable specific capacity of 325 mAh g-1 (1 A g-1), excellent rate capability (200 mAh g-1 at 20 A g-1), outstanding energy density of 469.6 Wh kg-1 and super-stable cycle life (20,000 cycles with 100% Coulombic efficiency), which outperforms most of reported zinc-halogen batteries. Further mechanism analysis and DFT calculations demonstrate that the chemical interaction of quaternary ammonium groups and bromide species is the main reason for suppressing the shuttle effect. The developed strategy can be extended to other halogen batteries to obtain stable charge storage.
Understanding the failure mechanism towards developing high-voltage single-crystal Ni-rich Co-free cathodes
Jixue Shen, Bao Zhang, Changwang Hao, Xiao Li, Zhiming Xiao, Xinyou He, Xing Ou
2024, 9(6): 1045-1057. doi: 10.1016/j.gee.2022.11.006
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Benefited from its high process feasibility and controllable costs, binary-metal layered structured LiNi0.8Mn0.2O2 (NM) can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles (EVs) sales, which is considered as the most promising next-generation cathode material for lithium-ion batteries (LIBs). However, the lack of deep understanding on the failure mechanism of NM has seriously hindered its application, especially under the harsh condition of high-voltage without sacrifices of reversible capacity. Herein, single-crystal LiNi0.8Mn0.2O2 is selected and compared with traditional LiNi0.8Co0.1Mn0.1O2 (NCM), mainly focusing on the failure mechanism of Co-free cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic characteristic. Specifically, the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition, which exacerbates the distortion of the lattice, mechanical strain changes and exhibits poor electrochemical performance, especially under the high cutoff voltage. Furthermore, the reaction kinetic of NM is impaired due to the absence of Co element, especially at the single-crystal architecture. Whereas, the negative influence of Li/Ni antisite defect is controllable at low current densities, owing to the attenuated polarization. Notably, Co-free NM can exhibit better safety performance than that of NCM cathode. These findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials, providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.
Biomimetic MXene membranes with negatively thermo-responsive switchable 2D nanochannels for graded molecular sieving
Yi Wang, Yangyang Wang, Chang Liu, Dongjian Shi, Weifu Dong, Baoliang Peng, Liangliang Dong, Mingqing Chen
2024, 9(6): 1058-1067. doi: 10.1016/j.gee.2023.01.004
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Negatively thermo-responsive 2D membranes, which mimic the stomatal opening/closing of plants, have drawn substantial interest for tunable molecular separation processes. However, these membranes are still restricted significantly on account of low water permeability and poor dynamic tunability of 2D nanochannels under temperature stimulation. Here, we present a biomimetic negatively thermo-responsive MXene membrane by covalently grafting poly (N-isopropylacrylamide) (PNIPAm) onto MXene nanosheets. The uniformly grafted PNIPAm polymer chains can enlarge the interlayer spacings for increasing water permeability while also allowing more tunability of 2D nanochannels for enhancing the capability of gradually separating multiple molecules of different sizes. As expected, the constructed membrane exhibits ultrahigh water permeance of 95.6 L m-2 h-1 bar-1 at 25 ℃, which is eight-fold higher than the state-of-the-art negatively thermo-responsive 2D membranes. Moreover, the highly temperature-tunable 2D nanochannels enable the constructed membrane to perform excellent graded molecular sieving for dye- and antibiotic-based ternary mixtures. This strategy provides new perspectives in engineering smart 2D membrane and expands the scope of temperature-responsive membranes, showing promising applications in micro/nanofluidics and molecular separation.
Towards carbon neutrality of calcium carbide-based acetylene production with sustainable biomass resources
Peng Jiang, Guanhan Zhao, Hao Zhang, Tuo Ji, Liwen Mu, Xiaohua Lu, Jiahua Zhu
2024, 9(6): 1068-1078. doi: 10.1016/j.gee.2022.12.004
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Acetylene is produced from the reaction between calcium carbide (CaC2) and water, while the production of CaC2 generates significant amount of carbon dioxide not only because it is an energy-intensive process but also the raw material for CaC2 synthesis is from coal. Here, a comprehensive biomass-to-acetylene process was constructed that integrated several units including biomass pyrolysis, oxygen-thermal CaC2 fabrication and calcium looping. For comparison, a coal-to-acetylene process was also established by using coal as feedstock. The carbon efficiency, energy efficiency and environmental impacts of the bio-based calcium carbide acetylene (BCCA) and coal-based calcium carbide acetylene (CCCA) processes were systematically analyzed. Moreover, the environmental impacts were further evaluated by applying thermal integration at system level and energy substitution in CaC2 furnace. Even though the BCCA process showed lower carbon efficiency and energy efficiency than that of the CCCA process, life cycle assessment demonstrated the BCCA (1.873 kgCO2eq kg-prod-1) a lower carbon footprint process which is 0.366 kgCO2eq kg-prod-1 lower compared to the CCCA process. With sustainable energy (biomass power) substitution in CaC2 furnace, an even lower GWP value of 1.377 kgCO2eq kg-prod-1 can be achieved in BCCA process. This work performed a systematic analysis on integrating biomass into industrial acetylene production, and revealed the positive role of biomass as raw material (carbon) and energy supplier.

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