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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

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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

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Overview of in-situ oxygen production technologies for lunar resources

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 233-255页

作者： Youpeng Xu Sheng Pang Liangwei Cong Guoyu Qian Dong Wang Laishi Li Yusheng Wu Zhi Wang College of Materials Science and Engineering Shenyang University of TechnologyShenyang 110870China CAS Key Laboratory of green Process and Engineering National Engineering Research Center for Green Recycling of Strategic Metal ResourcesInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Innovation Academy for green Manufacture Chinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

The rich resources and unique environment of the Moon make it an ideal location for human expansion and the utilization of extraterrestrial ***,crucial for supporting human life on the Moon,can be extracted from lunar regolith,which is highly rich in oxygen and contains polymetallic *** oxygen and metal extraction can be achieved using existing metallurgical ***,the ample reserves of water ice on the Moon offer another means for oxygen *** paper offers a detailed overview of the leading technologies for achieving oxygen production on the Moon,drawing from an analysis of lunar resources and environmental *** delves into the principles,processes,advantages,and drawbacks of water-ice electrolysis,two-step oxygen production from lunar regolith,and one-step oxygen production from lunar *** two-step methods involve hydrogen reduction,carbothermal reduction,and hydrometallurgy,while the one-step methods encompass fluorination/chlorination,high-temperature decomposition,molten salt electrolysis,and molten regolith electrolysis(MOE).Following a thorough comparison of raw materials,equipment,technology,and economic viability,MOE is identified as the most promising approach for future in-situ oxygen production on the *** the corrosion characteristics of molten lunar regolith at high temperatures,along with the Moon's low-gravity environment,the development of inexpensive and stable inert anodes and electrolysis devices that can easily collect oxygen is critical for promoting MOE technology on the *** review significantly contributes to our understanding of in-situ oxygen production technologies on the Moon and supports upcoming lunar exploration initiatives.

关键词： lunar resources in-situ oxygen production space metallurgy molten lunar regolith electrolysis

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Potential dependence in electrocatalysis: a theoretical perspective

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Science China Chemistry 2025年第1期68卷 21-25页

作者： Leyu Liu Zhaoming Xia Zeyu Wang Yinjuan Chen Hai Xiao Department of Chemistry Tsinghua University Fundamental Science center of Rare Earths Ganjiang Innovation Academy Chinese Academy of Sciences Key Laboratory of Advanced Catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation Center Changzhou University

Electrocatalysis is a key technology for the new energy era and sustainable development, serving as the interface for interconversion of electrical and chemical energies, which spans a wide spectrum of applications in sustainable energy and environmental engineering. Electrocatalytic reactions including electrochemical CO2reduction reaction （eCO2RR）, hydrogen evolution reaction （HER）, and oxygen evolution/reduction reactions （OER/ORR）, hold essential promise for renewable energy technologies as well as complement the biogeochemical carbon and oxygen cycles.

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Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries

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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

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Electrocatalytic selective synthesis and tandem utilization of hydroxylamine

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Science China Chemistry 2025年

作者： Yuxuan Lu Hengquan Yang Engineering research center of Ministry of Education for Fine Chemicals School of Chemistry and Chemical Engineering Shanxi Key Laboratory of Green Catalytic Synthesis of Coal-based High Value Chemicals Shanxi University

The transformation of renewable nitrogen feedstock to nitrogenous chemicals plays a significant role in our modern society,considering the crucial impact of nitrogenous chemicals on life sciences,biomedicine,agriculture,and *** （NH2OH）,a typical nucleophile,has been widely served as the nitrogenous feedstock to produce nitrogenous *** NH2OH synthesis methods rely on harsh reaction conditions,leading to an unfavorable environmental *** contrast,nitric oxide electroreduction promises to produce NH2OH powered by renewable *** achievements have revealed the possibility of this process,but have also identified significant *** activity and selectivity are fundamentally limited by competing hydrogenation reactions,while the performance evaluation with high accuracy and reproducibility is ***,this review aims to provide insight into the mechanism of NH2OH electrosynthesis,especially regarding understanding reaction pathways and the design principle towards efficient ***,the performance evaluation parameters and standard measurement methods for NH2OH synthesis are summarized to screen efficient ***,the prospects and emerging opportunities to synthesize nitrogen-containing organic compounds by tandem reaction are *** review aims to provide a guide for evaluating and exploring efficient electrocatalytic systems for NH2OH production and utilization technology.

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Trinuclear gold-catalyzed site-selective alkylation of peptides

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Science China Chemistry 2025年第1期68卷 249-256页

作者： Qing-Yun Fang Chengyihan Gu Yinghan Chen Wencheng Yan Yong Liang Weipeng Li Chengjian Zhu Jie Han Jin Xie State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic Materials Chemistry and Biomedicine Innovation Center (Chem BIC) School of Chemistry and Chemical Engineering Nanjing University green Catalysis center College of Chemistry Zhengzhou University State Key Laboratory of Natural Medicines China Pharmaceutical University

Selective modification of peptides has always been a challenging issue. The selective alkylation of peptides can alter the biological activity and physical properties of molecules, and it has gained significant research interest. We herein disclose an intriguing gold-catalyzed alkylation of peptides using bench-stable unactivated alkyl bromides under photoredox catalysis. A wide range of structurally diverse primary, secondary and tertiary alkyl bromides serve as effective coupling partners to precisely connect with the α-C(sp3)–H in glycine residue of peptides. This protocol demonstrates an exceptionally broad scope for alkyl halides and excellent tolerance for a wide range of useful functional groups. A series of relay transformations to construct cyclic peptides, to proceed click reaction and to realize peptide fluorescence labeling further enhance its synthetic practicality. In addition, mechanistic studies and density functional theory(DFT) calculations reveal an inner-sphere and subsequent outersphere single electron transfer(SET) mechanism.

关键词： gold catalysis peptide alkylation C-C coupling radical

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Design of a cationic accelerator enabling ultrafast ion diffusion kinetics in aqueous zinc-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 377-384页

作者： Yawei Xiao Qianqian Gu Haoyu Li Mengyao Li Yude Wang National center for International research on Photoelectric and Energy Materials School of Materials and Energy Yunnan University Key Laboratory of Ministry of Education for Advanced Materials in Tropical Island Resources School of Chemistry and Chemical Engineering Hainan University College of Chemical Engineering Fuzhou University Yunnan Key Laboratory of Carbon Neutrality and green Low-carbon Technologies Yunnan University

Aqueous zinc-ion batteries are highly favored for grid-level energy storage owing to their low cost and high safety,but their practical application is limited by slow ion *** address this,a strategy has been developed to create a cation-accelerating electric field on the surface of the cathode to achieve ultrafast Zn2+diffusion *** employing electrodeposition to coat MoS2on the surface of BaV6O16·3H2O nanowires,the directional built-in electric field generated at the heterointerface acts as a cation accelerator,continuously accelerating Zn2+diffusion into the active *** optimized Zn2+diffusion coefficient in CC@BaV-6O16·3H2O@MoS2(7.5×10～8cm2s-1) surpasses that of most reported V-based ***,MoS2serving as a cathodic armor extends the cycling life of the Zn-CC@BaV6O16·3H2O@MoS2full batteries to over 10000 *** work provides valuable insights into optimizing ion diffusion kinetics for high-performance energy storage devices.

关键词： Zinc alloys

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Natural and human-induced decline and spatio-temporal differentiation of terrestrial water storage over the Lancang-Mekong River Basin

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Journal of Geographical Sciences 2025年第1期35卷 112-138页

作者： CHEN Junxu WANG Yuan ZHAO Zhifang FAN Yunjiang LUO Xiaochuan YI Lu FENG Siqi YANG Liang Emlyn Yunnan Key Laboratory of Soil Erosion Prevention and green Development Yunnan University International Joint research center for Karstology Yunnan University School of Engineering Westlake University Department of Geography Ludwig Maximilian University of Munich (LMU)

Due to water conflicts and allocation in the Lancang-Mekong River Basin(LMRB), the spatio-temporal differentiation of total water resources and the natural-human influence need to be clarified. This work investigated LMRB's terrestrial water storage anomaly(TWSA) and its spatio-temporal dynamics during 2002–2020. Considering the effects of natural factors and human activities, the respective contributions of climate variability and human activities to terrestrial water storage change(TWSC) were separated. Results showed that:(1) LMRB's TWSA decreased by 0.3158 cm/a.(2) TWSA showed a gradual increase in distribution from southwest of MRB to middle LMRB and from northeast of LRB to middle LMRB. TWSA positively changed in Myanmar while slightly changed in Laos and China. It negatively changed in Vietnam, Thailand and Cambodia.(3) TWSA components decreased in a descending order of soil moisture, groundwater and precipitation.(4) Natural factors had a substantial and spatial differentiated influence on TWSA over the LMRB.(5) Climate variability contributed 79% of TWSC in the LMRB while human activities contributed 21% with an increasing impact after 2008. The TWSC of upstream basin countries was found to be controlled by climate variability while Vietnam and Cambodia's TWSC has been controlled by human activities since 2012.

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Printing perovskite and graphene parallel structure-based optical-mechanical sensors for human-machine interaction

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Science China Technological Sciences 2025年

作者： Sisi CHEN Jiemin ZHANG Nan CHENG Wenbo LI Jing LIU Hongfei XIE Jie ZHANG Yueying CHENG Xiaotong ZHAO Meng SU Yanlin SONG Key Laboratory of green Printing CAS Research/Education Center for Excellence in Molecular Sciences Institute of ChemistryChinese Academy of Sciences (ICCAS) University of Chinese Academy of Sciences Weiyang College Tsinghua University Department of Cardiovascular Surgery First Medical Center PLA General Hospital AECC Beijing Institute of Aeronautical Materials Beijing Institute of Graphene Technology Beijing Engineering research Centre of Graphene Application School of Integrated Circuit & Beijing National research center for Information Science and Technology (BNRist) Tsinghua University

Surgical robots are designed to provide enhanced precision and dexterity compared to manual surgical procedures,which mainly rely on multimodal sensing technologies for the surgeon to seamlessly operate the robotic arms and *** with single-mode sensors, optical and mechanical bi-modal sensors provide improved precision, enhanced safety,and robustness of human-machine interaction systems. Here, the template-guided and pneumatic printing technologies are combined to construct perovskite and graphene parallel structures with both optical and mechanical sensing capabilities. The printed uniformly crystallized perovskite microstructure exhibits fast and sensitive photoelectric response characteristics,enabling shadow recognition functionality. The combination of graphene and elastic rubber endows the great printability to prepare parallel structures near the perovskite arrays for force sensing capabilities. Thus, the printed perovskite and graphene structures possess non-contact optical sensing capabilities to detect hand position by recognizing shadows between the hand and the sensor, as well as contact mechanical sensing capabilities to detect touch force applied by the hand. It provides a synergistic platform for real-time and multidimensional feedback to improve human-machine interaction.

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