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Tailoring Second Coordination Sphere for Tunable Solid–Liquid Interfacial Charge Transfer toward Enhanced Photoelectrochemical H2Production

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Angewandte Chemie 2024年第22期136卷

作者： Dr. Yangguang Hu Dr. Wu Zhou Dr. Wanbing Gong Prof. Chao Gao Prof. Shaohua Shen Prof. Tingting Kong Prof. Yujie Xiong Anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular Solids Ministry of Education College of Chemistry and Materials Science Anhui Normal University 241002 Wuhu Anhui China Hefei National Laboratory for Physical Sciences at the Microscale School of Chemistry and Materials Science University of Science and Technology of China 230026 Hefei Anhui China These authors equally contributed to this work International Research Centre for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University 710049 Xi'an Shaanxi China

The recombination of photogenerated charge carriers severely limits the performance of photoelectrochemical (PEC) H 2 production. Here, we demonstrate that this limitation can be overcome by optimizing the charge transfer dynamics at the solid–liquid interface via molecular catalyst design. Specifically, the surface of a p-Si photocathode is modulated using molecular catalysts with different metal atoms and organic ligands to improve H 2 production performance. Co(pda-SO 3 H) 2 is identified as an efficient and durable catalyst for H 2 production through the rational design of metal centers and first/second coordination spheres. The modulation with Co(pda-SO 3 H) 2 , which contains an electron-withdrawing −SO 3 H group in the second coordination sphere, elevates the flat-band potential of the polished p-Si photocathode and nanoporous p-Si photocathode by 81 mV and 124 mV, respectively, leading to the maximized energy band bending and the minimized interfacial carrier transport resistance. Consequently, both the two photocathodes achieve the Faradaic efficiency of more than 95 % for H 2 production, which is well maintained during 18 h and 21 h reaction, respectively. This work highlights that the band-edge engineering by molecular catalysts could be an important design consideration for semiconductor–catalyst hybrids toward PEC H 2 production.

关键词： PEC H2 production molecular catalyst coordination sphere surface modulation charge transfer

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Cover Image, Volume 4, Number 1, January 2022

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Carbon Energy 2022年第1期4卷

作者： Chengyong Shu Qiang Tan Chengwei Deng Wei Du Zhuofan Gan Yan Liu Chao Fan Hui Jin Wei Tang Xiao-dong Yang Xiaohua Yang Yuping Wu School of Chemical Engineering and Technology Xi'an Jiaotong University Xi'an China State Key Laboratory for Mechanical Behavior of Materials School of Material Science and Engineering Xi'an Jiaotong University Xi'an China State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power Sources Shanghai China State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an China Xiao-dong Yang College of Materials Science and Engineering Huaqiao University 361021 Xiamen China. Xiaohua Yang Institute of Quantum and Sustainable Technology (IQST) School of Chemistry and Chemical Engineering Jiangsu University 212013 Zhenjiang China. Yuping Wu State Key Laboratory of Materials-Oriented Chemical Engineering School of Energy Science and Engineering and Institute of Advanced Materials Nanjing Tech University 211800 Nanjing China. College of Materials Science and Engineering Huaqiao University Xiamen China Institute of Quantum and Sustainable Technology (IQST) School of Chemistry and Chemical Engineering Jiangsu University Zhenjiang China State Key Laboratory of Materials-Oriented Chemical Engineering School of Energy Science and Engineering and Institute of Advanced Materials Nanjing Tech University Nanjing China

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Dynamic Pore-Scale Dissolution by CO2-Saturated Brine in Carbonates: Impact of Homogeneous Versus Fractured Versus Vuggy Pore Structure

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Water Resources Research 2020年第4期56卷 e2019WR026112-e2019WR026112页

作者： Yongfei Yang Yingwen Li Jun Yao Stefan Iglauer Linda Luquot Kai Zhang Hai Sun Lei Zhang Wenhui Song Zhiyu Wang Key Laboratory of Unconventional Oil and Gas Development China University of Petroleum (East China) Ministry of Education Qingdao China Research Center of Multiphase Flow in Porous Media School of Petroleum Engineering China University of Petroleum (East China) Qingdao China School of Engineering Petroleum Engineering Discipline Edith Cowan University Joondalup Western Australia Australia Université Montpellier CNRS Geosciences Montpellier Laboratory Montpellier France

Limestone pore structure strongly influences dissolution and associated reactive transport. These effects are critical in limestone diagenesis and but also in engineering operations such as carbon capture and storage (CCS). However, detailed studies on how CO 2 -enriched (acidic) brine changes this pore structure at relevant reservoir storage conditions are very limited. Thus, to provide further quantitative information and more fundamental understanding about these key processes, we studied the dissolution patterns of a homogeneous, a fractured, and a vuggy limestone when flooded with CO 2 -saturated brine at representative storage conditions. The pore structured of these limestones showed drastically different responses to the acidic brine flood. As such, preferential channels surrounded by branched channels were formed in the homogeneous sample, while fractures became the main flow path in the fractured sample. In contrast, only one dominant channel formed in the vuggy sample, which resulted in a sharp permeability increase. These dissolution patterns reflect the associated Damköhler number, which significantly lower in the homogeneous, representing uniform dissolution. However, after injecting sufficient reactive fluid (1,000 PV), this uniform dissolution pattern transformed into a single preferential channel growth. Moreover, we conclude that increasing complexity of the pore geometry leads to more nonuniform dissolution. These dissolution patterns indicate the effect of initial pore structure on preferential channel growth and reaction transport. Our work provides key fundamental data for further quantifying limestone dissolution patterns in CCS, indicating that the CO 2 injection may cause the reactivation of geological faults and damage around wellbore, thus aids in the implementation of industrial-scale CCS. The impact of limestone pore structure on reactive transport was analyzed experimentally and computationally The dissolution patterns of homogeneous, f

关键词： Carbonate dissolution pattern Carbon storage Pore-scale Micro-CT Permeability changes Pe -Da distribution

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Cover Feature: Hollow Carbon Sphere-Modified Graphitic Carbon Nitride for Efficient Photocatalytic H2Production (Chem. Eur. J. 68/2021)

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Chemistry – A European Journal 2021年第68期27卷

作者： Dr. Jinghua Li Dr. Lunqiao Xiong Dr. Bing Luo Prof. Dengwei Jing Dr. Jiamei Cao Prof. Junwang Tang International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an Shaanxi 710049 P. R. China Department of Chemical Engineering University College London London WC1E 7JE UK School of Chemical Engineering and Technology Xi'an Jiaotong University Xi'an Shaanxi 710049 P. R. China

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Correction: Epoxide ring-opening reaction promoted by ionic liquid reactivity: interplay of experimental and theoretical studies

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Catalysis Science & Technology 2019年第22期9卷 6532-6532页

作者： Shengxin Chen Guixiang Zeng Yingwei Li Bin He Ruixia Liu Suojiang Zhang Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Beijing 100190 P. R. China Kuang Yaming Honors School Nanjing University Nanjing 210023 P. R. China University of Chinese Academy of Sciences Beijing 100049 P.R. China

Correction for ‘Epoxide ring-opening reaction promoted by ionic liquid reactivity: interplay of experimental and theoretical studies’ by Shengxin Chen et al., Catal. Sci. Technol., 2019, DOI: 10.1039/c9cy00953a.

Correction for ‘Epoxide ring-opening reaction promoted by ionic liquid reactivity: interplay of experimental and theoretical studies’ by Shengxin Chen et al., Catal. Sci. Technol., 2019, DOI: 10.1039/c9cy00953a.

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Carbon-Confined Indium Oxides for Efficient Carbon Dioxide Reduction in a Solid-state Electrolyte flow Cell

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Angewandte Chemie 2022年第21期134卷

作者： Zhitong Wang Yansong Zhou Dongyu Liu Ruijuan Qi Chenfeng Xia Prof. Mingtao Li Prof. Bo You Prof. Bao Yu Xia School of Chemistry and Chemical Engineering Key Laboratory of Material Chemistry for Energy Conversion and Storage Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure Hubei Engineering Research Center for Biomaterials and Medical Protective Materials Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology (HUST) 1037 Luoyu Rd Wuhan 430074 China International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE) Xi'an Jiaotong University (XJTU) 28 Xianning West Road Xi'an 710049 China HSE University 101000 Moscow Russia Key Laboratory of Polar Materials and Devices (MOE) Department of Electronics School of Physics and Electronic Science East China Normal University Shanghai 200241 China

Developing robust electrocatalysts and advanced devices is important for electrochemical carbon dioxide (CO 2 ) reduction toward the generation of valuable chemicals. We present herein a carbon-confined indium oxide electrocatalyst for stable and efficient CO 2 reduction. The reductive corrosion of oxidative indium to the metallic state during electrolysis could be prevented by carbon protection, and the applied carbon layer also optimizes the reaction intermediate adsorption, which enables both high selectivity and activity for CO 2 reduction. In a liquid-phase flow cell, the formate selectivity exceeds 90 % in a wide potential window from −0.8 V to −1.3 V vs. RHE. The continuous production of ca. 0.12 M pure formic acid solution is further demonstrated at a current density of 30 mA cm −2 in a solid-state electrolyte mediated reactor. This work provides significant concepts in the parallel development of electrocatalysts and devices for carbon-neutral technologies.

关键词： Carbon Dioxide Reduction Corrosion-Resistant Electrocatalyst Indium Oxide Solid-state Electrolyte

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Deciphering Ligand Controlled Structural Evolution of Prussian Blue Analogues and Their Electrochemical Activation during Alkaline Water Oxidation

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Angewandte Chemie 2022年第49期134卷

作者： Baghendra Singh Pandian Mannu Yu-Cheng Huang Ravi Prakash Shaohua Shen Chung-Li Dong Arindam Indra Department of Chemistry IIT(BHU) Varanasi UP-221005 India Department of Physics Tamkang University New Taipei City Taiwan School of Material Science and Technology IIT(BHU) Varanasi UP-221005 India International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi An Shi Xi'an 710049 China

Herein, we have demonstrated the control over the structure of precatalysts to tune the properties of the active catalysts and their water oxidation activity. The reaction of K 3 [Fe(CN) 6 ] and Na 2 [Fe(CN) 5 (NO)] with Co(OH) 2 @CC produced precatalysts PC-1 and PC-2, respectively, with distinct structural and electronic features. The replacement of the −CN group with strong π-acceptor −NO modulates the electronic and atomic structure of PC-2. As a result, a facile electrochemical transformation of PC-2 into active catalyst Fe−Co(OH) 2 -Co(O)OH (AC-2) has been attained only in 15 CV cycles while 600 CV cycles are required for the electrochemical activation of PC-1 into AC-1. The X-ray absorption studies reveal the contraction of the Co−O and Fe−O bond in AC-2 because of the presence of a higher amount of Co 3+ and Fe 3+ than in AC-1. The high valent Co 3+ and Fe 3+ modulates the electronic properties of AC-2 and assists in the O−O bond formation, leading to the improved water oxidation activity.

关键词： Electrochemical Reconstruction Oxygen Evolution Reaction Prussian Blue Analogue Ultrathin Nanosheets XAS Studies

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Sa2045 MAGNETIC ANCHORING ASSISTED ENDOSCOPIC IRREVERSIBLE ELECTROPORATION FOR GASTRIC MUCOSAL ABLATION: A PRECLINICAL FEASIBILITY STUDY IN CANINE MODEL

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Gastrointestinal Endoscopy 2020年第6期91卷 AB257-AB257页

作者： Fenggang Ren Qingshan Li Xuyao Gao Yuchi Zhang Jing Zhang Zhuoqun Li Dake Chu Zheng Wu Rongqian Wu Yi Lv National Local Joint Engineering Research Center for Precision Surgery and Regenerative Medicine First Affiliated Hospital of Xi’an Jiaotong University Xi'an China Department of Hepatobiliary Surgery First Affiliated Hospital of Xi’an Jiaotong University Xi'an China State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an China Department of Gastroenterology First Affiliated Hospital of Xi’an Jiaotong University Xi'an China

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Preface

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Fuel Processing Technology 2010年第8期91卷 799-799页

作者： Guangwen Xu Chun-Zhu Li Kinya Sakanishi State Key Laboratory of Multiphase Complex System Institute of Process Engineering Chinese Academy of Sciences China Curtin Centre for Advanced Energy Science and Engineering Curtin University of Technology Australia Biomass Technology Research Center National Institute of Advanced Industrial Science and Technology Japan

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Hydrogele aus amorphem Calciumcarbonat und Polyacrylsäure: bioinspirierte Materialien für “Mineral‐Kunststoffe”

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Angewandte Chemie 2016年第39期128卷

作者： Shengtong Sun Li‐Bo Mao Zhouyue Lei Shu‐Hong Yu Helmut Cölfen Physikalische Chemie Universität Konstanz Universitätsstraße 10 78457 Konstanz Deutschland School of Chemical Engineering State Key Laboratory of Chemical Engineering Shanghai Key Laboratory of Multiphase Materials Chemical Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 Volksrepublik China Division of Nanomaterials and Chemistry Hefei National Laboratory for Physical Sciences at Microscale Department of Chemistry University of Science and Technology of China Hefei Anhui 230026 Volksrepublik China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science Laboratory for Advanced Materials Fudan University Shanghai 200433 Volksrepublik China

Angesichts zunehmender ökologischer Probleme durch die massive Nutzung nicht biologisch abbaubarer, erdölbasierter Kunststoffe ist die Nachfrage nach neuen ökonomischen, umweltverträglichen und recyclierbaren Kunststoffmaterialien hoch. Eine mögliche Alternative stellt die bioinspirierte Synthese mineralbasierter Hybridmaterialien dar. Hier stellen wir ein auf amorphem Calciumcarbonat (ACC) basierendes Hydrogel aus sehr kleinen ACC‐Nanopartikeln vor, die durch Polyacrylsäure physikalisch vernetzt sind. Das Hydrogel ist formbar, dehnbar und selbstheilend. Durch Trocknung lassen sich feste, freistehende und transparente Objekte mit bemerkenswerten mechanischen Eigenschaften erstellen. Der ursprüngliche Hydrogel‐Zustand kann durch Quellen in Wasser vollständig wiederhergestellt werden. Das Material kann auch als Matrix für ein thermochromes Material dienen. Das hier vorgestellte Material ist ein Beispiel für eine neue Klasse von Kunststoffmaterialien, die “Mineral‐Kunststoffe”.

关键词： Amorphes Calciumcarbonat Bioinspirierte Synthesen Organisch-anorganische Hybridkomposite Plastizität Supramolekulare Hydrogele

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