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Poly(ethylenimine)-assisted synthesis of hollow carbon spheres comprising multi-sized Ni species for CO_(2)electroreduction

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Chinese Journal of Catalysis 2024年第9期64卷 66-76页

作者： Kaining Li Yasutaka Kuwahara Hiromi Yamashita division of Materials and Manufacturing Science Graduate School of EngineeringOsaka University2‐1 Yamada‐okaOsaka 565‐0871Japan Innovative Catalysis Science division Institute for Open and Transdisciplinary Research Initiatives(OTRI)Osaka University2‐1 Yamada‐okaSuitaOsaka 565‐0871Japan

Electrochemical CO_(2)reduction to produce value-added chemicals and fuels is one of the research hotspots in the field of energy *** development of efficient catalysts with high conductivity and readily accessible active sites for CO_(2)electroreduction remains challenging yet *** this work,a reliable poly(ethyleneimine)(PEI)-assisted strategy is developed to prepare a hollow carbon nanocomposite comprising a single-site Ni-modified carbon shell and confined Ni nanoparticles(NPs)(denoted as Ni@NHCS),where PEI not only functions as a mediator to induce the highly dispersed growth of Ni NPs within hollow carbon spheres,but also as a nitrogen precursor to construct highly active atomically-dispersed Ni-Nx *** from the unique structural properties of Ni@NHCS,the aggregation and exposure of Ni NPs can be effectively prevented,while the accessibility of abundant catalytically active Ni-Nx sites can be *** a result,Ni@NHCS exhibits a high CO partial current density of 26.9 mA cm^(-2)and a Faradaic efficiency of 93.0%at-1.0 V ***,outperforming those of its PEI-free *** from the excellent activity and selectivity,the shell confinement effect of the hollow carbon sphere endows this catalyst with long-term *** findings here are anticipated to help understand the structure-activity relationship in Ni-based carbon catalyst systems for electrocatalytic CO_(2)***,the PEI-assisted synthetic concept is potentially applicable to the preparation of high-performance metal-based nanoconfined materials tailored for diverse energy conversion applications and beyond.

关键词： Hollow carbon sphere Ni nanoparticle CO_(2)reduction Electrocatalysis Single-atom catalyst

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High-silica faujasite zeolite-tailored metal encapsulation for the low-temperature production of pentanoic biofuels

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Journal of Energy Chemistry 2024年第1期88卷 552-560,I0012页

作者： Wenhao Cui Yuanshuai Liu Pengfei Guo Zhijie Wu Liqun Kang Huawei Geng Shengqi Chu Linying Wang Dong Fan Zhenghao Jia Haifeng Qi Wenhao Luo Peng Tian Zhongmin Liu National Engineering research Center of Lower-carbon Catalysis Technology Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101ShandongChina College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina State Key Laboratory of Heavy Oil Processing and Key Laboratory of Catalysis of CNPC China University of PetroleumBeijing 102249China Department of Inorganic Spectroscopy Max Planck Institute for Chemical Energy ConversionMülheim an der Ruhr 45470Germany Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China division of Energy research Resources Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Leibniz-Institut für Katalyse Albert-Einstein-Straβe 29aRostock 18059Germany

Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable ***,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant ***,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal *** with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.

关键词： High-silica zeolite Y Metal encapsulation Bifunctional catalysis Hydrodeoxygenation Biofuels

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Roadmap for rechargeable batteries:present and beyond

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Science China Chemistry 2024年第1期67卷 13-42页

作者： Sen Xin Xu Zhang Lin Wang Haijun Yu Xin Chang Yu-Ming Zhao Qinghai Meng Pan Xu Chen-Zi Zhao Jiahang Chen Huichao Lu Xirui Kong Jiulin Wang Kai Chen Gang Huang Xinbo Zhang Yu Su Yao Xiao Shu-Lei Chou Shilin Zhang Zaiping Guo Aobing Du Guanglei Cui Gaojing Yang Qing Zhao Liubing Dong Dong Zhou Feiyu Kang Hu Hong Chunyi Zhi Zhizhang Yuan Xianfeng Li Yifei Mo Yizhou Zhu Dongfang Yu Xincheng Lei Jianxiong Zhao Jiayi Wang Dong Su Yu-Guo Guo Qiang Zhang Jun Chen Li-Jun Wan CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences.Beijing 100049 China Institute of Advanced Battery Materials and Devices Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Key Laboratory of Advanced Functional Materials Ministry of EducationBeijing University of TechnologyBeijing 100124China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China State Key Laboratory of Chemistry and Utilization of carbon-Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830046China Department of Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChangchun 130022China Institute for carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaide 5000Australia Qingdao Industrial Energy Storage research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China Frontiers Science Center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China College of Chemistry and Materials Science Jinan UniversityGuangzhou 511443China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhen 518055China Department of Materials Science and Engineering City University of Hong KongHong Kong 999077China division of Energy Storage Dalian National Laboratory for Clean Energy(DNL)Dalian Institute of Chem

Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate *** to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable *** efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow *** the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a *** roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable *** computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.

关键词： energy storage rechargeable batteries battery materials electrochemistry

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Fine-tuning electronic structure of N-doped graphitic carbon-supported Co-and Fe-incorporated Mo_(2)C to achieve ultrahigh electrochemical water oxidation activity

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carbon Energy 2024年第7期6卷 134-149页

作者： Md.Selim Arif Sher Shah Hyeonjung Jung Vinod K.Paidi Kug-Seung Lee Jeong Woo Han Jong Hyeok Park Department of Chemical and Biomolecular Engineering Yonsei UniversitySeoulRepublic of Korea Department of Chemistry University of North BengalRaja RammohunpurDarjeelingWest BengalIndia Department of Materials Science and Engineering Research Institute of Advanced MaterialsSeoul National UniversitySeoulRepublic of Korea Pohang Accelerator Laboratory Beamline DivisionPohangRepublic of Korea European Synchrotron Radiation Facility France

Mo_(2)C is an excellent electrocatalyst for hydrogen evolution reaction(HER).However,Mo_(2)C is a poor electrocatalyst for oxygen evolution reaction(OER).Herein,two different elements,namely Co and Fe,are incorporated in Mo_(2)C that,therefore,has a finely tuned electronic structure,which is not achievable by incorporation of any one of the ***,the resulting electrocatalyst Co_(0.8)Fe_(0.2)-Mo_(2)C-80 displayed excellent OER catalytic performance,which is evidenced by a low overpotential of 214.0(and 246.5)mV to attain a current density of 10(and 50)mA cm^(-2),an ultralow Tafel slope of 38.4 mV dec^(-1),and longterm stability in alkaline *** data demonstrates that Co_(0.8)Fe_(0.2)-Mo_(2)C-80 requires the lowest overpotential(1.00 V)for OER and Co centers to be the active *** ultrahigh catalytic performance of the electrocatalyst is attributed to the excellent intrinsic catalytic activity due to high Brunauer-Emmett-Teller specific surface area,large electrochemically active surface area,small Tafel slope,and low chargetransfer resistance.

关键词： fine-tuning electronic structures heteronanostructures Mo_(2)C multimetal(Co/Fe) oxygen evolution reaction

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Technical alternatives for coke oven gas utilization in China: A comparative analysis of environment-economic-strategic perspectives

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Environmental Science and Ecotechnology 2024年第5期21卷 168-177页

作者： Zichen Di Feixia Lei Jiankai Jing Hao Peng Xi Lu Fangqin Cheng Institute of Resources and Environmental Engineering Shanxi UniversityTaiyuan030006PR China School of Environment State Key Joint Laboratory of Environment Simulation and Pollution ControlTsinghua UniversityBeijing100084PR China Institute for carbon Neutrality Tsinghua UniversityBeijing100084PR China

China is the largest coke producer and *** is a pressing need to address the high emissions of air pollutants and carbon dioxide associated with traditional coking *** the nation pursues a transition towards carbon neutrality,expanding supply chains for coking plants to produce hydrogen,methanol,and other green alternatives has garnered significant ***,the relative advantages of these strategies have remained *** this study,we integrate a life cycle assessmenteconomic analysis-scenario analysis model to evaluate various coke oven gas(COG)utilization routes(COGtM:COG-to-methanol,COGtLNG:COG-to-liquefied natural gas,COGtSA:COG-to-synthetic ammonia,and COGtH:COG-to-hydrogen).The results indicate that COGtSA emerges as the preferred option for balancing environmental and economic ***,COGtM demonstrates economic viability but is associated with higher environmental *** being recognized as a significant strategic direction under carbon neutrality initiatives,COGtH faces economic feasibility and risk resilience *** encounters both financial and environmental challenges,necessitating strategic development from an energy security *** projected coking capacity is anticipated to experience a slight increase in the mid-term yet a significant decline in the long term,influenced by steel production *** potential future markets,COGtM is estimated to potentially capture a maximum market share of 16e34%in the methanol ***,against the backdrop of continuously expanding potential demand for hydrogen,COGtH holds advantages as a transitional solution,but in the long run,it can only meet a small portion of the *** can meet 7e14%of market demand and emerges as the most viable pathway from the viewpoint of balancing environmental and economic aspects and covering future markets.

关键词： Coke oven gas Life cycle assessment Economic analysis Comprehensive benefits Transformation strategy

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Salt-assisted vapor-liquid-solid growth of high-quality ultrathin nickel oxide flakes for artificial synapses in image recognition applications

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Nano research 2024年第5期17卷 4622-4630页

作者： Hui Zhang Zongjie Shen Alei Li Lin Wang Qinan Wang Yunfei Li Yunlei Zhong Juntong Zhu Yong Zhang Mengjiao Han Dan Tian Chun Zhao Lixing Kang Qingwen Li School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China division of Advanced Materials Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China College of Energy Soochow Institute for Energy and Materials Innovationsand Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou 215123China Songshan Lake Materials Laboratory Dongguan 523808China School of Advanced Technology Xi’an Jiaotong-Liverpool UniversitySuzhou 215123China College of Materials Science and Engineering Co-Innovation Center of Efficient Processing and Utilization of Forest ResourcesNanjing Forestry UniversityNanjing 210037China

Transition metal oxides have attracted intense interest owing to their abundant physical and chemical *** controlled preparation of large-area,high-quality two-dimensional crystals is essential for revealing their inherent properties and realizing high-performance ***,fabricating two-dimensional(2D)transition metal oxides using a general approach still presents substantial ***,we successfully achieve highly crystalline nickel oxide(NiO)flakes with a thickness as thin as 3.3 nm through the salt-assisted vapor-liquid-solid(VLS)growth method,which demonstrated exceptional stability under ambient *** explore the great potential of the NiO crystal in this work,an artificial synapse based on the NiO-flake resistive switching(RS)layer is ***-term and long-term synaptic behaviors are obtained with external *** artificial synaptic performance provides the foundation of the neuromorphic application,including handwriting number recognition based on artificial neuron network(ANN)and the virtually unsupervised learning capability based on generative adversarial network(GAN).This pioneering work not only paves new paths for the synthesis of 2D oxides in the future but also demonstrates the substantial potential of oxides in the field of neuromorphic computing.

关键词： nickel oxide(NiO)flakes vapor-liquid-solid(VLS)growth memristor synapse generative adversarial network(GAN)

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Elucidating regulatory processes of intense physical activity by multi-omics analysis

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Military Medical research 2024年第4期11卷 479-499页

作者： Ernesto S.Nakayasu Marina A.Gritsenko Young-Mo Kim Jennifer E.Kyle Kelly G.Stratton Carrie D.Nicora Nathalie Munoz Kathleen M.Navarro Daniel Claborne Yuqian Gao Karl K.Weitz Vanessa L.Paurus Kent J.Bloodsworth Kelsey A.Allen Lisa M.Bramer Fernando Montes Kathleen A.Clark Grant Tietje Justin Teeguarden Kristin E.Burnum-Johnson Biological Sciences division Pacific Northwest National LaboratoryRichlandWA 99352USA Environmental and Molecular Sciences division Pacific Northwest National LaboratoryRichlandWA 99352USA Centers for Disease Control and Prevention National Institute for Occupational Safety and HealthWestern States DivisionDenverCO 80204USA Computational Analytics division Pacific Northwest National LaboratoryRichlandWA 99352USA National Security Directorate Pacific Northwest National LaboratoryRichlandWA 99352USA Los Angeles County Fire Department Los AngelesCA 90063USA Centers for Disease Control and Prevention National Institute for Occupational Safety and HealthRespiratory Health DivisionMorgantownWV 26505USA Environmental and Molecular Toxicology Oregon State UniversityCorvallisOR 97331USA

Background:Physiological and biochemical processes across tissues of the body are regulated in response to the high demands of intense physical activity in several occupations,such as firefighting,law enforcement,military,and sports.A better understanding of such processes can ultimately help improve human performance and prevent illnesses in the work ***:To study regulatory processes in intense physical activity simulating real-life conditions,we performed a multi-omics analysis of 3 biofluids(blood plasma,urine,and saliva)collected from 11 wildland firefighters before and after a 45 min,intense exercise *** profiles ***-exercise were compared by Student’s t-test followed by pathway analysis and comparison between the different omics ***:Our multi-omics analysis identified and quantified 3835 proteins,730 lipids and 182 metabolites combining the 3 different types of *** blood plasma analysis revealed signatures of tissue damage and acute repair response accompanied by enhanced carbon metabolism to meet energy *** urine analysis showed a strong,concomitant regulation of 6 out of 8 identified proteins from the renin-angiotensin system supporting increased excretion of catabolites,reabsorption of nutrients and maintenance of fluid *** saliva,we observed a decrease in 3 pro-inflammatory cytokines and an increase in 8 antimicrobial peptides.A systematic literature review identified 6 papers that support an altered susceptibility to respiratory ***:This study shows simultaneous regulatory signatures in biofluids indicative of homeostatic maintenance during intense physical activity with possible effects on increased infection susceptibility,suggesting that caution against respiratory diseases could benefit workers on highly physical demanding jobs.

关键词： Multi-omics analysis Intense exercise Human performance Biofluids Metabolism Immunity

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Perspective of alkaline zinc-based flow batteries

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Science China Chemistry 2024年第1期67卷 260-275页

作者： Zhizhang Yuan Xianfeng Li division of Energy Storage Dalian National Laboratory for Clean Energy(DNL)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 110623China

Energy storage technologies have been identified as the key in constructing new electric power systems and achieving carbon neutrality,as they can absorb and smooth the renewables-generated *** zinc-based flow batteries are well suitable for stationary energy storage applications,since they feature the advantages of high safety,high cell voltage and low ***,many alkaline zinc-based flow batteries have been proposed and developed,e.g.,the alkaline zinc–iron flow battery and alkaline zinc–nickel flow *** development and application are closely related to advanced materials and battery *** this perspective,we will first provide a brief introduction and discussion of alkaline zinc-based flow *** we focus on these batteries from the perspective of their current status,challenges and *** bottlenecks for these batteries are briefly *** with the practical requirements and development trends of alkaline zinc-based flow battery technologies,their future development and research direction will be summarized.

关键词： energy storage alkaline zinc-based flow batteries advanced materials battery structure

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Advances in bio-inspired electrocatalysts for clean energy future

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Nano research 2024年第2期17卷 515-533页

作者： Jing-Wen Duan Mu Min-Rui Gao division of Nanomaterials&Chemistry Hefei National Laboratory for Physical Sciences at the MicroscaleDepartment of ChemistryUniversity of Science and Technology of ChinaHefei 230026China

Electrocatalysis can enable efficient energy storage and conversion and thus is an effective way to achieve carbon *** unique structure and function of organisms can offer many ideas for the design of electrocatalysts,which has become one of the most promising research ***,the understanding of the mechanism of bio-inspired electrocatalysis has become clearer,which has promoted the design of bio-inspired catalysts and catalytic *** bio-inspired catalysts(enzyme-like catalysts,layered porous catalysts,superhydrophobic/superhydrophilic surfaces,and so on)have been developed to enable efficient electrocatalytic ***,we discuss the key advances in the field of bio-inspired electrocatalysts progressed in recent ***,the role of bio-inspiration in increasing the intrinsic activity and number of active sites of catalysts is ***,the structure and mechanism of layered porous catalytic systems that mimic biological transport systems are comprehensively ***,the design of three-phase interfaces from micro-nanoscale to atomic scale is highlighted,including the wettability of the electrode surface and the transport system near the *** conclude the review by identifying challenges in bio-inspired electrocatalysts and providing insights into future prospects for the exciting research field.

关键词： bio-inspired electrocatalysts active sites layered porous structure three-phase interface

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Greenhouse gas emissions during the COVID-19 pandemic from agriculture in China

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Frontiers of Agricultural Science and Engineering 2024年第3期11卷 409-427页

作者： Jianing TIAN Chuanhui GU Yanchao BAI division of Natural and Applied Sciences Duke Kunshan UniversityKunshan 215316China Environmental research Center Duke Kunshan UniversityKunshan 215311China College of Environmental Science and Engineering Yangzhou UniversityYangzhou 225009China

To study the impact of the COVID-19 pandemic on agricultural carbon emissions in China,the greenhouse gas emissions generated by crop and livestock production,and agricultural material and energy inputs in China from 2019 to 2021 were systematically *** was found that from 2019 to 2021,Net greenhouse gas emissions(NGHGE)from agriculture in China had an increasing *** emissions ranked first in NGHGE,with an annual proportion exceeding 65%and an increasing annual ***_(4)emissions were primarily influenced by enteric fermentation and rice *** oxide emissions accounted for around 22%of annual NGHGE and decreased from 2019 to *** main sources of N_(2)O emissions were the use of nitrogen fertilizers and manure *** dioxide emissions accounted for about 18%annually,with diesel and agricultural electricity use contributing to over 60%of CO_(2)*** carbon sequestration represented about a 6.1%lowering of *** combined proportion of CH4 emissions from enteric fermentation and rice production accounted for over 50%of total GHG *** changes in NGHGE were mainly caused by disturbance of the livestock industry during the pandemic.

关键词： Agricultural systems emission factors greenhouse gases soil carbon sequestration

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