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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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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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Corrigendum to “Experimental study of liquid sodium flow and heat transfer characteristics along a hexagonal 7-rod bundle” [Appl. Therm. Eng. 149 (2019) 578–587.]

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Applied Thermal engineering 2019年 159卷

作者： Yandong Hou Liu Wang Mingjun Wang Kui Zhang Xisi Zhang Wenjun Hu Yingwei Wu Wenxi Tian Suizheng Qiu G.H. Su State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong University 28 Xianning West Road Xi’an 710049 China Shaanxi Key Lab. of Advanced Nuclear Energy and Technology School of Nuclear Science and Technology Xi’an Jiaotong University 28 Xianning West Road Xi’an 710049 China China Institute of Atomic Energy P.O. Box 275-95 Beijing 102413 China

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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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Impressive computational acceleration by using machine learning for 2-dimensional super-lubricant materials discovery

arXiv

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arXiv 2019年

作者： Fronzi, Marco Ghazaleh, Mutaz Abu Isayev, Olexandr Winkler, David A. Shapter, Joe Ford, Michael J. International Research Centre for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an Shaanxi710049 China School of Mathematical and Physical Science University of Technology Sydney UltimoNSW2007 Australia Laboratory for Molecular Modeling Division of Chemical Biology and Medicinal Chemistry UNC Eshelman School of Pharmacy University of North Carolina Chapel HillNC27599 United States Manufacturing Commonwealth Scientific and Industrial Research Organization Bag 10 Clayton South MDCVIC3169 Australia Monash Institute of Pharmaceutical Sciences Monash University 381 Royal Parade ParkvilleVIC3052 Australia Latrobe Institute for Molecular Science La Trobe University Kingsbury Drive BundooraVIC3086 Australia School of Pharmacy University of Nottingham NottinghamNG7 2RD United Kingdom Australian Institute for Bioengineering and Nanotechnology University of Queensland St Lucia BrisbaneQLD4072 Australia College of Science and Engineering Flinders University Bedford Park AdelaideSA5042 Australia

The screening of novel materials is an important topic in the field of materials science. Although traditional computational modelling, especially first-principles approaches, is a very useful and accurate tool to predict the properties of novel materials, it still demands extensive and expensive state-of-the-art computational resources. Additionally, they can be often extremely time consuming. We describe a time and resource efficient machine learning approach to create a large dataset of structural properties of van der Waals layered structures. In particular, we focus on the interlayer energy and the elastic constant of layered materials composed of two different 2-dimensional (2D) structures, that are important for novel solid lubricant and super-lubricant materials. We show that machine learning models can recapitulate results of computationally expansive approaches (i.e. density functional theory) with high accuracy. Copyright © 2019, The Authors. All rights reserved.

关键词： Large dataset

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Current-Density Regulating Lithium Metal Directional Deposition for Long Cycle-Life Li Metal Batteries

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Angewandte Chemie 2021年第35期133卷

作者： Heng Mao Wei Yu Zhuanyun Cai Guixian Liu Limin Liu Rui Wen Yaqiong Su Huari Kou Kai Xi Benqiang Li Hongyang Zhao Xinyu Da Hu Wu Wei Yan Shujiang Ding Xi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Xi'an Jiaotong University & Shaanxi Quantong Joint Research Institute of New Energy Vehicles Power Xi'an Jiaotong University Xi'an 710049 China Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) State Key Laboratory of Physical Chemistry of Solid Surfaces Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China Key Laboratory of Molecular Nanostructure and Nanotechnology Beijing National Laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China Department of Mechanical Engineering University of Michigan-Dearborn Dearborn MI 48128 USA Department of Environmental Science and Engineering State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China

Uncontrolled dendrite formation in the high energy density of lithium (Li) metal batteries (LMBs) may pose serious safety risks. While numerous studies have attempted to protect separators, these proposed methods fail to effectively inhibit upward dendrite growth that punctures through the separator. Here, we introduce a novel “orientated-growth” strategy that transfers the main depositional interface to the anode/current collector interface from the anode/separator interface. We placed a layer of cellulose/graphene carbon composite aerogel (CCA) between the current collector and the anode (LCL-bottom). This layer works as a charge organizer that induces a high current density and encourages Li to deposit at the anode/current collector interface. Both in situ and ex situ images of the electrode demonstrate that the anode part of the cell has been flipped; with the newly deposited particles facing the current collector and the smooth surface facing the separator. The electrode in half and full cells showed outstanding cyclic stability and rate capability, with the LCL-bottom/LFP full cell capable of maintaining 94 % of its initial capacity after 1000 cycles.

关键词： anode/separator interface depositional interface transfer lithium metal battery long cycles

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Atomically Dispersed Janus Nickel Sites on Red Phosphorus for Photocatalytic Overall Water Splitting

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Angewandte Chemie 2022年第29期134卷

作者： Menglong Wang Shuai Xu Prof. Zhaohui Zhou Prof. Chung-Li Dong Dr. Xu Guo Jeng-Lung Chen Dr. Yu-Cheng Huang Prof. Shaohua Shen Prof. Yubin Chen Prof. Liejin Guo Prof. Clemens Burda International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Shaanxi 710049 China Chemical Engineering and Technology School of Water and Environment Key Laboratory of Subsurface Hydrology and Ecological Effects in Arid Region Ministry of Education Chang'an University Xi'an 710064 China Department of Physics Tamkang University New Taipei City 25137 Taiwan National Synchrotron Radiation Research Center Hsinchu 30076 Taiwan Department of Chemistry Case Western Reserve University Cleveland OH 44106 USA

Single-atom nickel catalysts hold great promise for photocatalytic water splitting due to their plentiful active sites and cost-effectiveness. Herein, we adopt a reactive-group guided strategy to prepare atomically dispersed nickel catalysts on red phosphorus. The hydrothermal treatment of red phosphorus leads to the formation of P−H and P−OH groups, which behave as the reactive functionalities to generate the dual structure of single-atom P−Ni and P−O−Ni catalytic sites. The produced single-atom sites provide two different functions: P−Ni for water reduction and P−O−Ni for water oxidation. Benefitting from this specific Janus structure, Ni-red phosphorus shows an elevated hydrogen evolution rate compared to Ni nanoparticle-modified red phosphorus under visible-light irradiation. The hydrogen evolution rate was additionally enhanced with increased reaction temperature, reaching 91.51 μmol h −1 at 70 °C, corresponding to an apparent quantum efficiency of 8.9 % at 420 nm excitation wavelength.

关键词： Nickel Photocatalysis Red Phosphorus Single-Atom Catalysts Water Splitting

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Insights into Charge Transfer at an Atomically Precise Nanocluster/Semiconductor Interface

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Angewandte Chemie 2020年第20期132卷

作者： Yu Wang Xiao‐He Liu Qiankun Wang Martin Quick Sergey A. Kovalenko Qing‐Yun Chen Norbert Koch Nicola Pinna Institut für Chemie and IRIS Adlershof Humboldt-Universität zu Berlin Brook-Taylor-Strasse 2 12489 Berlin Germany International Research Center for Renewable Energy (IRCRE) and State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power Engineering Xi'an Jiaotong University Xi'an 710049 P. R. China Institut für Physik and IRIS Adlershof Humboldt-Universität zu Berlin Brook-Taylor-Strasse 6 12489 Berlin Germany

The deposition of an atomically precise nanocluster, for example, Ag 44 (SR) 30 , onto a large‐band‐gap semiconductor such as TiO 2 allows a clear interface to be obtained to study charge transfer at the interface. Changing the light source from visible light to simulated sunlight led to a three orders of magnitude enhancement in the photocatalytic H 2 generation, with the H 2 production rate reaching 7.4 mmol h −1 g catalyst −1 . This is five times higher than that of TiO 2 modified with Ag nanoparticles and even comparable to that of TiO 2 modified with Pt nanoparticles under similar conditions. Energy band alignment and transient absorption spectroscopy reveal that the role of the metal clusters is different from that of both organometallic complexes and plasmonic nanoparticles: A type II heterojunction charge‐transfer route is achieved under UV/Vis irradiation, with the cluster serving as a small‐band‐gap semiconductor. This results in the clusters acting as co‐catalysts rather than merely photosensitizers.

关键词： Ladungstransfer Cokatalysatoren Photosensibilisator Silber-Nanocluster

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Photothermal Synergistic Effect Induces Bimetallic Cooperation to Modulate Product Selectivity of CO2Reduction on Different CeO2Crystal Facets

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Angewandte Chemie 2024年第46期136卷

作者： Yuqi Ren Yitao Si Mingyue Du Changjun You Chunyang Zhang Yuan-Hao Zhu Prof. Zhenkun Sun Prof. Kai Huang Prof. Maochang Liu Prof. Lunbo Duan Prof. Naixu Li School of Chemistry and Chemical Engineering Southeast University No.2 Dongnandaxue Road Nanjing 211189 Jiangsu P.R. China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University No.28 Xianning West Road Xi'an Shaanxi 710049 P.R. China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and Environment No.2 Dongnandaxue Road Nanjing 210096 Jiangsu P.R. China

Product selectivity of solar-driven CO 2 reduction and H 2 O oxidation reactions has been successfully controlled by tuning the spatial distance between Pt/Au bimetallic active sites on different crystal facets of CeO 2 catalysts. The replacement depth of Ce atoms by monatomic Pt determines the distance between bimetallic sites, while Au clusters are deposited on the surface. This space configuration creates a favourable microenvironment for the migration of active hydrogen species (*H). The *H is generated via the activation of H 2 O on monatomic Pt sites and migrate towards Au clusters with a strong capacity for CO 2 adsorption. Under concentrated solar irradiation, selectivity of the (100) facet towards CO is 100 %, and the selectivity of the (110) and (111) facets towards CH 4 is 33.5 % and 97.6 %, respectively. Notably, the CH 4 yield on the (111) facet is as high as 369.4 μmol/g/h, and the solar-to-chemical energy efficiency of 0.23 % is 33.8 times higher than that under non-concentrated solar irradiation. The impacts of high-density flux photon and thermal effects on carriers and *H migration at the microscale are comprehensively discussed. This study provides a new avenue for tuning the spatial distance between active sites to achieve optimal product selectivity.

关键词： Photothermal catalysis CO2 reduction Product selectivity Bimetallic active sites Spatial distance

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