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engineering nanoparticle structure at synergistic Ru-Na interface for integrated CO2 capture and hydrogenation

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Journal of Energy Chemistry 2025年第1期100卷 779-791页

作者： Hanzi Liu Ling Cen Xinlin Xie Lei Liu Zhao Sun Zhiqiang Sun Hunan engineering Research center of Clean and Low-Carbon Energy Technology School of Energy Science and Engineering Central South University

The development of dual functional material for cyclic CO2capture and hydrogenation is of great significance for converting diluted CO2into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and ***,we engineered a series of RuNa/γ-Al2O3materials,varying the size of ruthenium from single atoms to clusters/*** coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic *** findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°*** Ru-Na interfacial sites facilitate CO2migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and ***-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO2.

关键词： Carbon capture and utilization

Highly conductive and stable iodine doped argyrodite electrolyte for all-solid-state lithium batteries

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Journal of Energy Chemistry 2025年第1期100卷 50-58页

作者： Gaozhan Liu Jing Zhang Jing Yang Jinghui Chen Xingyue Xiao Xiayin Yao Ningbo Institute of Materials Technology and engineering Chinese Academy of Sciences center of Materials science and Optoelectronics engineering University of Chinese Academy of Sciences

Lithium argyrodites with high ionic conductivity and low cost are considered as one of the most prospective solid electrolytes for all-solid-state lithium ***,the poor chemical stability and compatibility with lithium metal limit their ***,Li5.4PS4.4Cl1.4I0.2solid electrolyte with high ionic conductivity of 11.49 m S cm-1and improved chemical stability is synthesized by iodine *** ultra-thin Li5.4PS4.4Cl1.4I0.2membrane with thickness of 10μm can be obtained by wet coating process,exhibiting a high ionic conductivity of 2.09 mS cm-1and low areal resistance of 1.17Ω***,iodine doping could in-situ form LiI at the lithium/electrolyte interface and improve the critical current density of Li5.4PS4.4Cl1.6from 0.8 to 1.35 mA *** resultant LiCoO2/Li5.4PS4.4Cl1.4I0.2/Li battery shows excellent cycling stability at 1 C,with a reversible specific capacity of 110.1 mA h g-1and a retention of 80.5% after 1000 *** addition,the assembled LiCoO2/Li5.4PS4.4Cl1.4I0.2membrane/Li pouch cell delivers an initial discharge capacity of 110.4 mA h g-1and 80.5% capacity retention after 100 cycles.

关键词： Solid-State Batteries

Prominent cycling reversibility and kinetics enabled by CaTiO3 protective layer on Zn metal for aqueous Zn-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 245-258页

作者： Gaeun Lee Yong Nam Ahn Seongjoon So Chanwoo Park Jong-Seong Bae Taehyun Park Il Tae Kim Jaehyun Hur School of Chemical Biological and Battery Engineering Gachon University Seongnam Busan center Korea Basic Science Institute

Aqueous Zn-ion batteries （AZIBs） have received considerable attention owing to their various advantages such as safety,low cost,simple battery assembly conditions,and high ionic ***,they still suffer from serious problems,including uncontrollable dendrite growth,corrosion,hydrogen evolution reaction （HER） from water decomposition,electrode passivation,and unexpected *** creation of a uniform artificial nanocrystal layer on the Zn anode surface is a promising strategy for resolving these ***,we propose the use of a perovskite CaTiO3（CTO） protective layer on Zn（CTO@Zn） as a promising approach for improving the performance of *** CTO artificial layer provides an efficient pathway for Zn ion diffusion towards the Zn metal because of the high dielectric constant （εr=180） and ferroelectric characteristics that enable the alignment of dipole moments and redistribute the Zn2+ions in the CTO *** avoiding the direct contact of the Zn anode with the electrolyte solution,the uneven dendrite growth,corrosion,parasitic side reactions,and HER are mitigated,while CTO retains its mechanical and chemical robustness during ***,CTO@Zn demonstrates an improved lifespan in a symmetric cell configuration compared with bare ***@Zn shows steady overpotential （～68 m V） for 1500 h at 1 mA cm-2/0.5 mA h cm-2,excelling bare ***,when paired with the V2O5-C cathode,the CTO@Zn//V2O5-C full battery delivers 148.4 mA h g-1（based on the mass of the cathode） after 300 *** study provides new insights into Zn metal anodes and the development of high-performance AZIBs.

关键词： Perovskite

Optimizing electronic structure through point defect engineering for enhanced electrocatalytic energy conversion

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Green Energy & Environment 2025年第1期10卷 109-131页

作者： Wei Ma Jiahao Yao Fang Xie Xinqi Wang Hao Wan Xiangjian Shen Lili Zhang Menggai Jiao Zhen Zhou Interdisciplinary Research center for Sustainable Energy science and engineering(IRC4SE2) School of Chemical EngineeringZhengzhou UniversityHenan450001China

Point defect engineering endows catalysts with novel physical and chemical properties,elevating their electrocatalytic *** introduction of defects emerges as a promising strategy,effectively modifying the electronic structure of active *** optimization influences the adsorption energy of intermediates,thereby mitigating reaction energy barriers,altering paths,enhancing selectivity,and ultimately improving the catalytic efficiency of *** elucidate the impact of defects on the electrocatalytic process,we comprehensively outline the roles of various point defects,their synthetic methodologies,and characterization ***,we consolidate insights into the relationship between point defects and catalytic activity for hydrogen/oxygen evolution and CO_(2)/O_(2)/N_(2) reduction reactions by integrating mechanisms from diverse *** underscores the pivotal role of point defects in enhancing catalytic *** last,the principal challenges and prospects associated with point defects in current electrocatalysts are proposed,emphasizing their role in advancing the efficiency of electrochemical energy storage and conversion materials.

关键词： Point defect engineering Doping Vacancy Electrocatalysis Electronic structure

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

Establishing a new testing protocol of the electrochemical stability window for electric double-layer capacitors

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science China Chemistry 2025年第1期68卷 217-225页

作者： Ruilin Hou Xiaoxi Zhao Tingting Liang Qingyun Dou Shan Xu Xingbin Yan School of Materials science and engineering Sun Yat-sen University Laboratory of Clean Energy Chemistry and Materials Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of engineering and Applied sciences Nanjing University center of Industrial Analysis and Testing Guangdong Academy of Science

The electrochemical stability window(ESW) is crucial for determining the energy density of electric double-layer capacitors(EDLCs). However, current ESW testing protocols of EDLCs are strongly affected by artificial factors, thereby leading to unreliable result. To solve this problem, we first identify the key shortcomings of the traditional protocols by analyzing their test principles. Subsequently, taking an aqueous carbon-based EDLC as an example, we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods. With the aid of this descriptor, we propose a new ESW testing protocol, which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations. The protocol can be extended from the single electrode to the full device. This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.

关键词： electric double-layer capacitors electrochemical stability window testing protocol side reaction descriptor operating limitation

Cyano migration-mediated radical-polar crossover cyclopropanation

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science China Chemistry 2025年第1期68卷 241-248页

作者： Ziqiang Wang Yasu Chen Jie Li Chen Zhu Key Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials ScienceSoochow University Frontiers science center for Transformative Molecules Zhangjiang Institute for Advanced Study and Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Shanghai Jiao Tong University

We report a novel cyano migration-mediated radical-polar crossover process, whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently achieved. This transformation yields a diverse array of multisubstituted cyclopropanes under mild photocatalytic conditions. Mechanistic studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution, leading to the formation of the cyclopropane derivatives.

关键词： cyclopropanation cyano migration radical-polar crossover radical reactions

Aligned Ion Conduction Pathway of Polyrotaxane‑Based Electrolyte with Dispersed Hydrophobic Chains for Solid‑State Lithium–Oxygen Batteries

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Nano-Micro Letters 2025年第2期17卷 169-186页

作者： Bitgaram Kim Myeong‑Chang Sung Gwang‑Hee Lee Byoungjoon Hwang Sojung Seo Ji‑Hun Seo Dong‑Wan Kim Department of Materials science and engineering Korea University145 Anam‑RoSeongbuk‑GuSeoul 02841Republic of Korea School of Civil Environmental and Architectural EngineeringKorea University145 Anam‑RoSeongbuk‑GuSeoul 02841Republic of Korea Materials science and Chemical engineering center Institute for Advanced Engineering(IAE)Yongin 17180Republic of Korea

A critical challenge hindering the practical application of lithium–oxygen batteries(LOBs)is the inevitable problems associated with liquid electrolytes,such as evaporation and safety *** study addresses these problems by proposing a modified polyrotaxane(mPR)-based solid polymer electrolyte(SPE)design that simultaneously mitigates solvent-related problems and improves ***-SPE exhibits high ion conductivity(2.8×10^(−3)S cm^(−1)at 25℃)through aligned ion conduction pathways and provides electrode protection ability through hydrophobic chain *** this mPR-SPE into solid-state LOBs resulted in stable potentials over 300 *** situ Raman spectroscopy reveals the presence of an LiO_(2)intermediate alongside Li_(2)O_(2)during oxygen *** situ X-ray diffraction confirm the ability of the SPE to hinder the permeation of oxygen and moisture,as demonstrated by the air permeability *** present study suggests that maintaining a low residual solvent while achieving high ionic conductivity is crucial for restricting the sub-reactions of solid-state LOBs.

关键词： Solid polymer electrolyte Lithium-oxygen batteries Polyrotaxane ion conductivity Hydrophobic chain

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An NIR-Ⅱ-emissive Ru(Ⅱ) metallacycle for efficient and safe immunotherapy

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science China Chemistry 2025年第1期68卷 5-7页

作者： Chonglu Li Jianbo Zhan Biao Dong Institute of Health Inspection and Testing Hubei Provincial Center for Disease Control and Prevention State Key Laboratory on Integrated Optoelectronics College of Electronic Science and Engineering Jilin University

Immunotherapy, as a groundbreaking cancer treatment, has gained considerable attention for its utilization of the body’s immune system to combat tumors [1]. This therapy induces tumor cell apoptosis, triggering a sustained anti-tumor immune response and effectively preventing tumor recurrence and metastasis [2]. The fundamental principle lies in inducing tumor cell death through specific treatment modalities, leading to the release of a cascade of signaling molecules and antigens, thereby mobilizing the immune system to actively identify and attack tumor cells [3].

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