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Journal of Energy Chemistry 2025年第1期100卷 760-769页

作者： Lin Peng Yu Bai Hang Li Meixiu Qu Zhenhua Wang Kening Sun Advanced Research Institute of Multidisciplinary Science Beijing Institute of Technology Beijing Key Laboratory of chemical Power Source and Green Catalysis School of Chemistry and Chemical Engineering Beijing Institute of Technology

Lithium-sulfur （Li-S） batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox ***,we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P （Vp-B-Ni2P）,thereby enhancing the bidirectional sulfur *** study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides （LiPSs） as well as expediting the bidirectional conversion kinetics of sulfur ***,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation ***,the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 m A h g-1at 5 C and high areal capacity of 8.03 mA h cm-2under E/S of 5μL mg-1and sulfur loading of 7.20 mg *** work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.

关键词： Lithium sulfur batteries

High-temperature-tolerant flexible supercapacitors: Gel polymer electrolytes and electrode materials

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Journal of Energy Chemistry 2025年第1期100卷 426-457页

作者： Chong Peng Xinyi Huang Mingwei Zhao Shuling Liao Quanhong Yang Nianjun Yang Siyu Yu School of Chemistry & chemical engineering Southwest University Nanoyang Group Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage School of Chemical Engineering and Technology and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin University Department of Chemistry & IMO-IMOMEC Hasselt University

The development of flexible supercapacitors(FSCs) capable of operating at high temperatures is crucial for expanding the application areas and operating conditions of supercapacitors. Gel polymer electrolytes and electrode materials stand as two key components that significantly impact the efficacy of hightemperature-tolerant FSCs(HT-FSCs). They should not only exhibit high electrochemical performance and excellent flexibility, but also withstand intense thermal stress. Considerable efforts have been devoted to enhancing their thermal stability while maintaining high electrochemical and mechanical performance. In this review, the fundamentals of HT-FSCs are outlined. A comprehensive overview of state-of-the-art progress and achievements in HT-FSCs, with a focus on thermally stable gel polymer electrolytes and electrode materials is provided. Finally, challenges and future perspectives regarding HT-FSCs are discussed, alongside strategies for elevating operational temperatures and *** review offers both theoretical foundations and practical guidelines for designing and manufacturing HT-FSCs, further promoting their widespread adoption across diverse fields.

关键词： Polymer membrane electrodes

Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key Laboratory of Green chemical engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology Key Laboratory of Pesticide & chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Oxygen evolution reaction

Mechanistic insight into the synergy between nickel single atoms and nanoparticles on N-doped carbon for electroreduction of CO2

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Journal of Energy Chemistry 2025年第1期100卷 327-336页

作者： Mingdong Sun Wenwen Guan Cailing Chen Chao Wu Xiaoling Liu Biao Meng Tao Chen Yu Han Jun Wang Shibo Xi Yu Zhou State Key Laboratory of Materials-Oriented chemical engineering College of Chemical Engineering Nanjing Tech University Advanced Membranes and Porous Materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Institute of Sustainability for chemicals Energy and Environment A*STAR (Agency for Science Technology and Research) College of Materials Science and engineering Sichuan University

The synergy of single atoms （SAs） and nanoparticles （NPs） has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction （CO2RR）;however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst ***,a Ni2+-loaded porous poly（ionic liquids）(PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing *** catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO2into *** Ni K-edge X-ray absorption near-edge structure （XANES） spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and *** charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active *** the electroreduction of CO2,the coexistence of Ni SAs and NPs strengthened the CO2activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO2→*COOH step,and therefore promoted the catalysis efficiency.

关键词： Activation energy

Fluorinated poly(p-triphenylene isatin) anion exchange membranes based on hydrophilic hydroxyl side chain modulation for fuel cells

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Journal of Energy Chemistry 2025年第1期100卷 702-709页

作者： Yiman Gu Yanchao Zhang Zhanyu Li Yijia Lei Baozeng Sun Xiaoyu Yu Zhe Wang College of Chemistry and Life Science Changchun University of Technology College of chemical engineering Changchun University of Technology School of Materials Science and engineering Changchun University of Technology Key Laboratory of Advanced Functional Polymer Membrane Materials of Jilin Province

The development of alkaline fuel cells is moving forward at an accelerated pace,and the application of ether-free bonded polymers to anion exchange membranes （AEMs） has been widely ***,the question of the“trade-off”between AEM ionic conductivity and dimensional stability remains *** strategy of inducing microphase separation to improve the performance of AEM has attracted much attention recently,but the design of optimal molecular structures is still being ***,this work introduced different ratios of 3-bromo-1,1,1-trifluoroacetone （x=40,50,and 60） into the main chain of poly（p-terphenylene isatin）.Because fluorinated groups have excellent hydrophobicity,hydrophilic hydroxyl-containing side chains are introduced to jointly adjust the formation of phase separation *** results show that PTI-PTF50-NOH AEM with the appropriate fluorinated group ratio has the best ionic conductivity and alkali stability under the combined effect of *** has an ionic conductivity of 133.83 mS cm-1at 80°*** addition,the OH-conductivity remains at 89%of the initial value at 80°C and 3 M KOH for 1056 h of *** cell polarization curve based on PTI-PTF50-NOH shows a power density of 734.76 mW cm-2at a current density of 1807.7 mA cm-2.

关键词： Potassium hydroxide

Precise gradient separation of nanoparticles using reduced graphene oxide-polyoxomolybdate membranes

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Science China Chemistry 2025年第01期 209-216页

作者： Yixin Yang Wanlei Zhao Ruoxuan Zheng Hongqiang Li Wei Chen Yu-Fei Song State Key Laboratory of chemical Resource engineering Beijing University of Chemical Technology Quzhou Institute for Innovation in Resource chemical engineering

The purification and size sieving of nanoparticles （NPs） represents a significant scientific ***,the r GO-polyoxometalates (POMs=PMo12,Mo132and Mo368) membranes were fabricated successfully via a simple and scalable POMsassisted in-situ photoreduction *** the mass ratio of r GO to PMo12was 1:30,the resultant r GO-PMo12membranes with highly ordered and uniform nanochannels of 1.0 nm can be obtained,which showed an accurate carbon quantum dots（CQDs） separation with a cut-off size approximately 1.0 *** increase of the size of the interlayered POMs from PMo12（1.0 nm）,{Mo132}（2.9 nm） to{Mo368}（3.8 nm）,the resultant r GO-PMo12,r GO-Mo132and r GO-Mo368exhibited precise gradient separation of CQDs and Au nanoparticles by size exclusion *** results pave a promising way to construct new twodimensional （2D） membranes for highly efficient size-selective separation.

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Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang State Key Laboratory of Fine chemicals School of Chemical Engineering Dalian University of Technology State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： Aspect ratio

Maximizing biomass utilization: An integrated strategy for coproducing multiple chemicals

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Journal of Energy Chemistry 2025年第1期100卷 180-191页

作者： Byeongchan Ahn Sua Jo Jonggeol Na J.Jay Liu Young-Ju Kim Wangyun Won Department of chemical and Biological engineering Korea University Department of chemical engineering (Integrated process) Kyung Hee University Department of chemical engineering and Materials Science Ewha Womans University Department of chemical engineering Pukyong National University Resources engineering Plant Research Department Korea Institute of Geoscience and Mineral Resources

Lignocellulosic biomass is one of the viable solutions to alleviate the global warming. However, the limited utilization of biomass majorly focused on cellulose and hemicellulose restricts the economic and environmental feasibilities. To cope with this issue, we proposed an integrated process of co-producing 1,6-hexanediol（1,6-HDO） with tetrahydrofuran and adipic acid from biomass, referred to as Strategy A. To compare the impacts of lignin upgrading and feedstock, Strategy B, which co-produces tetrahydrofuran alone, and Strategy C, which is the traditional route to produce 1,6-HDO from fossil fuels, were used. Heat networks are also designed to reduce operating costs and indirect carbon emissions due to energy consumption, saving 87% and 83% of the heat and cooling requirements, respectively, in Strategy A. The market competitiveness of Strategy A was evaluated by determining the minimum selling price through techno-economic analysis, and sustainability was thoroughly investigated by quantifying the environmental impacts through both midpoint and endpoint life-cycle assessments（LCAs）.Strategy A was found to be the most favorable both economically（USRDSCHARDOLLAR3,402/ton） and environmentally（-26.9 kg CO2eq.）. This indicates that lignin valorization is not only economically but also environmentally preferred. Finally, changes in economic and environmental feasibilities depending on economic, process, and environmental parameters were investigated using sensitivity and uncertainty analyses. The results of these analyses provide valuable insight into bio-based chemical production.

关键词： Carbon capture and utilization

Electrocatalytic cleavage of a lignin β-O-4 model compound and coupling with nitrogen-containing aromatics using Prussian blue analogue-derived nickel–cobalt spinel

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Journal of Energy Chemistry 2025年第1期100卷 628-636页

作者： Yi Qi Xueying Chen Bowen Liu Xuliang Lin Xueqing Qiu Yanlin Qin Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology Guangdong Provincial Laboratory of Chemistry and Fine chemical engineering Jieyang Center Guangdong Basic Research Center of Excellence for Ecological Security and Green Development Guangdong University of Technology

Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great *** demonstrate the targeted synthesis and cation modulation of NiCo2O4spinel nanoboxes,synthesized via cation exchange and calcination *** catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds,specifically 2-phenoxy-1-phenylethanol,into nitrogen-containing aromatics,achieving high conversion rates and *** catalysts were synthesized via a cation exchange and calcination oxidation process,using Prussian blue nanocubes as *** porous architecture and polymetallic composition of the NiCo2O4spinel demonstrated superior performance in electrocatalytic oxidative coupling,achieving a 99.2 wt%conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt%for quinoline derivatives and 31.5 wt%for *** innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives,the elucidation of a multistage reaction pathway involving CAO bond cleavage,hydroxyaldol condensation,and CAN bond formation,and a deeper mechanistic understanding derived from DFT *** work establishes a new strategy for lignin valorization,offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions,without the need for additional reagents.

关键词： Spinel Biomass valorization Electrocatalysis Lignin oxidation Coupling

Metal nanoparticles decorated CoFe-(oxy)hydroxysulfides nanosheets fabricated by a general strategy for electrocatalytic water splitting

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Journal of Energy Chemistry 2025年第1期100卷 26-38页

作者： Xiaodong Yang Haochen Shen Xiaoming Xiao Zhichao Li Qi Zhou Wei Yang Bin Jiang Yongli Sun Luhong Zhang Zhenhua Yan School of chemical engineering and technology Tianjin University Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University

This study presents a novel method to fabricate metal-decorated,sulfur-doped layered double hydroxides （M/SLDH） through spontaneous redox and sulfurization *** developed Ag/SLDH and Pt/SLDH catalysts with abundant heterogeneous interfaces and hierarchical nanostructures demonstrated outstanding oxygen evolution reaction （OER） and hydrogen evolution reaction （HER） performance,achieving low overpotentials of 212 and 35 mV at 10 mA cm-2in 1 M KOH,*** both anode and cathode in water splitting,they required only 1.47 V to reach 10 mA cm-2and exhibited high structural robustness,maintaining stability at 1000 mA cm-2for 300 ***-situ Raman analysis revealed that the synergistic effects of metal nanoparticles and S doping significantly promote the transformation into the S-Co1-xFexOOH layer,which serves as the active phase for water ***,ultraviolet photoelectron spectroscopy （UPS） and density functional theory （DFT） analyses indicated that incorporating metal nanoparticles and S doping increase electron density near the Fermi level and reduce reaction energy barriers,thus enhancing intrinsic OER and HER *** study provides a scalable strategy for synthesizing high-performance electrocatalysts for water splitting,with promising potential for broader applications.

关键词： Ultraviolet photoelectron spectroscopy