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Formulating the Electrolyte Towards High-Energy and Safe Rechargeable Lithium–Metal Batteries

Angewandte Chemie 2021年第30期133卷

作者： Qiang Ma Dr. Junpei Yue Min Fan Shuang-Jie Tan Dr. Juan Zhang Dr. Wen-Peng Wang Dr. Yuan Liu Yi-Fan Tian Dr. Quan Xu Prof. Ya-Xia Yin Prof. Ya You Prof. An Luo Prof. Sen Xin Prof. Xiong-Wei Wu Prof. Yu-Guo Guo College of Electrical and Information Engineering Hunan University Changsha Hunan 410082 P. R. China School of Chemistry and Materials Science College of Agronomy Hunan Agricultural University Changsha Hunan 410128 P. R. China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular Sciences Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences (CAS) Beijing 100190 P. R. China Nanozyme Medical Center School of Basic Medical Sciences Zhengzhou University Zhengzhou 450001 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei P. R. China

Rechargeable lithium–metal batteries with a cell-level specific energy of >400 Wh kg −1 are highly desired for next-generation storage applications, yet the research has been retarded by poor electrolyte–electrode compatibility and rigorous safety concerns. We demonstrate that by simply formulating the composition of conventional electrolytes, a hybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li-metal anode and the nickel-rich layered oxide cathodes. By employing the new electrolyte, Li∥LiNi 0.6 Co 0.2 Mn 0.2 O 2 cells show favorable cycling and rate performance, and a 10 Ah Li∥LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell demonstrates a practical specific energy of >450 Wh kg −1 . Our findings shed light on reasonable design principles for electrolyte and electrode/electrolyte interfaces toward practical realization of high-energy rechargeable batteries.

关键词： hybrid electrolytes in situ polymerization interfacial chemistry rechargeable lithium–metal batteries

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Three-dimensionally ordered macroporous materials for photo/electrocatalytic sustainable energy conversion, solar cell and energy storage

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EnergyChem 2022年第4期4卷

作者： Yang Ding Chunhua Wang Runtian Zheng Soumyajit Maitra Genwei Zhang Tarek Barakat Subhasis Roy Bao-Lian Su Li-Hua Chen Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium Department of Chemistry KU Leuven Celestijnenlaan 200F B-3001 Leuven Belgium Department of Chemical Engineering University of Calcutta 92 APC Road Kolkata West Bengal 700009 India Department of Chemistry Fudan University 2005 Songhu Road 200438 Shanghai China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Clare Hall University of Cambridge Cambridge CB2 1EW UK

Three-dimensionally ordered macroporous (3DOM) materials have aroused tremendous interest in solar light to energy conversion, sustainable and renewable products generation, and energy storage fields owing to their convenient mass transfer channels, high surface area, enhanced interaction between matter and light, plentiful reactive sites as well as tunable composition. In this review, the state-of-the-art 3DOM materials as well as their preparation methods and the relevant applications including photo/electrocatalytic sustainable energy conversion, solar cells, Li ion batteries and supercapacitor are thoroughly outlined. Meanwhile, the unique merits and mechanisms for 3DOM materials in various applications are revealed and discussed in depth. Moreover, the strategies for designing 3DOM materials and the enhanced performance for applications are correlated, which can be significantly valuable to help readers to promptly acquire the comprehensive knowledge and to inspire some new ideas in developing 3DOM materials for further improved performances. Finally, the challenges and perspectives of 3DOM materials for sustainable energy conversion/production, solar cells and energy storage fields are outlooked. We sincerely look forward to that this critical review can facilitate the fast developments in designing highly efficient 3DOM materials and the relevant applications.

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Kinetics Controlled Perovskite Crystallization for High Performance Solar Cells

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Angewandte Chemie 2024年第14期136卷

作者： Jinghao Ge Ran Chen Yabin Ma Yunfan Wang Yingjie Hu Lu Zhang Fengzhu Li Xiaokang Ma Sai-Wing Tsang Jiaxue You Alex K. Y. Jen Shengzhong Frank Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology International Joint Research Center of Shaanxi Province for Photoelectric Materials Science Institute for Advanced Energy Materials School of Materials Science and Engineering Shaanxi Normal University No. 620 West Chang'an Avenue Xi'an 710119 China These authors contributed equally. School of Materials Science and Engineering Xi'an University of Science and Technology No. 67 Xiaozhai East Road Xi'an Shaanxi 710054 PR China Department of Materials Science and Engineering Hong Kong Institute for Clean Energy City University of Hong Kong Tat Chee Avenue Kowloon Hong Kong SAR China State Key Laboratory of Solidification Processing Northwestern Polytechnical University No. 127 Laodong West Road Xi'an Shaanxi 710072 PR China Dalian National Laboratory for Clean Energy iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences No.457 Zhongshan Road Shahekou District Dalian 116023 China University of the Chinese Academy of Sciences No. 80 Zhongguancun East Road Beijing 100039 China

The power conversion efficiencies (PCEs) of perovskite solar cells have recently developed rapidly compared to crystalline silicon solar cells. To have an effective way to control the crystallization of perovskite thin films is the key for achieving good device performance. However, a paradox in perovskite crystallization is from the mismatch between nucleation and Oswald ripening. Usually, the large numbers of nucleation sites tend to weak Oswald ripening. Here, we proposed a new mechanism to promote the formation of nucleation sites by reducing surface energy from 44.9 mN/m to 36.1 mN/m, to spontaneously accelerate the later Oswald ripening process by improving the grain solubility through the elastic modulus regulation. The ripening rate is increased from 2.37 Åm ⋅ s −1 to 4.61 Åm ⋅ s −1 during annealing. Finally, the solar cells derived from the optimized films showed significantly improved PCE from 23.14 % to 25.32 %. The long-term stability tests show excellent thermal stability (the optimized device without encapsulation maintaining 82 % of its initial PCE after 800 h aging at 85 °C) and an improved light stability under illumination. This work provides a new method, the elastic modulus regulation, to enhance the ripening process.

关键词： Perovskite solar cells Oswald ripening crystallization kinetics nucleation surface energy

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High-Performance Thermoelectric α-Ag9Ga1−xTe6Compounds with Ultralow Lattice Thermal Conductivity Originating from Ag9Te2Motifs

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Angewandte Chemie 2022年第36期134卷

作者： Yingfei Tang Yimeng Yu Na Zhao Keke Liu Haijie Chen Constantinos C. Stoumpos Yixuan Shi Shuo Chen Lingxiao Yu Jinsong Wu Qingjie Zhang Xianli Su Xinfeng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (equal) Visualization (equal) Writing - original draft (lead) Nanostructure Research Center Wuhan University of Technology Wuhan 430070 China Contribution: Data curation (equal) Software (equal) Visualization (supporting) Contribution: Investigation (equal) Methodology (equal) Contribution: Investigation (equal) Methodology (equal) Visualization (equal) State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional Materials College of Materials Science and Engineering Donghua University Shanghai 201620 China Contribution: Methodology (equal) Visualization (equal) Writing - review & editing (equal) Department of Materials Science and Technology Voutes Campus University of Crete Iraklio Heraklion 70013 Greece Contribution: Methodology (equal) Visualization (equal) Contribution: Investigation (equal) Visualization (equal) Contribution: Conceptualization (equal) Investigation (equal) Contribution: Methodology (equal) Contribution: Conceptualization (equal) Methodology (equal) Contribution: Conceptualization (equal) Investigation (equal) Methodology (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Methodology (equal) Supervision (equal) Writing - review & editing (equal)

We have determined the complex atomic structure of high-temperature α-Ag 9 GaTe 6 phase with a hexagonal lattice ( P 6 3 mc space group, a = b =8.2766 Å, c =13.4349 Å). The structure has outer [GaTe 4 ] 5− tetrahedrons and inner [Ag 9 Te 2 ] 5+ clusters. All of the Ag ions are disorderly distributed in the lattice. Seven types of the Ag atoms constitute the cage-like [Ag 9 Te 2 ] 5+ clusters. The highly disordered Ag ions vibrate in-harmonically, producing strong coupling between low frequency optical phonons and acoustic phonons. This in conjunction with a low sound velocity of 1354 m s −1 leads to an ultralow thermal conductivity of 0.20 W m −1 K −1 at 673 K. Meanwhile, the deficiency of Ga in Ag 9 Ga 1− x Te 6 compounds effectively optimizes the electronic transport properties. Ag 9 Ga 0.91 Te 6 attains a highest power factor of 0.40 mW m −1 K −2 at 673 K. All these contribute to a much-improved ZT value of 1.13 at 623 K for Ag 9 Ga 0.95 Te 6 , which is 41 % higher than that of the pristine Ag 9 GaTe 6 sample.

关键词： α-Ag9GaTe6 Crystal Structure Ga Deficiency Thermoelectrics Ultralow Lattice Thermal Conductivity

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[email protected] 2 hybrid microcapsules with high in vivo biocompatibility and stability for cell therapy

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Colloids and Surfaces B: Biointerfaces 2021年 203卷

作者： Grégory Leroux Myriam Neumann Christophe F. Meunier Virginie Voisin Isabelle Habsch Nathalie Caron Carine Michiels Li Wang Bao-Lian Su Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Molecular Physiology Research Unit (URPhyM) Namur Research Institute for Life Sciences (NARILIS) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Laboratory of Biochemistry and Cell Biology (URBC) Namur Research Institute for Life Sciences (NARILIS) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Luoshi Road 122 Wuhan 430070 China

Designing new materials to encapsulate living therapeutic cells for the treatment of the diseases caused by protein or hormone deficiencies is a great challenge. The desired materials need to be biocompatible towards both entrapped cells and host organisms, have long-term in vivo stability after implantation, allow the diffusion of nutrients and metabolites, and ensure perfect immune-isolation. The current work investigates the in vivo biocompatibility and stability of [email protected] 2 hybrid microcapsules and the immune-isolation of entrapped HepG2 cells, to assess their potential for cell therapy. A comparison was made with alginate-silica hybrid microcapsules (ASA). These two hybrid microcapsules are implanted subcutaneously in female Wistar rats. The inflammatory responses of the rats are monitored by the histological examination of the implants and the surrounding tissues, to indicate their in vivo biocompatibility towards the hosts. The in vivo stability of the microcapsules is evaluated by the recovery rate of the intact microcapsules after implantation. The immune-isolation of the entrapped cells is assessed by their morphology, membrane integrity and intracellular enzymatic activity. The results show high viability of the entrapped cells and insignificant inflammation of the hosts, suggesting the excellent biocompatibility of [email protected] 2 and ASA microcapsules towards both host organisms and entrapped cells. Compared to the ASA microcapsules, more intact [email protected] 2 hybrid microcapsules are recovered 2-day and 2-month post-implantation and more cells remain alive, proving their better in vivo biocompability, stability, and immune-isolation. The present study demonstrates that the [email protected] 2 hybrid microcapsule is a highly promising implantation material for cell therapy.

关键词： Hybrid hydrogels Cell encapsulation In vivo biocompatibility In vivo stability Immune isolation

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Engineering a Local Free Water Enriched Microenvironment for Surpassing Platinum Hydrogen Evolution Activity

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Angewandte Chemie 2022年第35期134卷

作者： Qunlei Wen Junyuan Duan Wenbin Wang Dr. Danji Huang Dr. Youwen Liu Dr. Yongliang Shi Prof. JiaKun Fang Prof. Anmin Nie Prof. Huiqiao Li Prof. Tianyou Zhai State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Conceptualization (equal) Investigation (lead) Writing - original draft (lead) Contribution: Formal analysis (equal) Investigation (equal) Contribution: Investigation (supporting) Writing - original draft (supporting) State Key Lab of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Conceptualization (lead) Formal analysis (lead) Writing - review & editing (lead) Center for Spintronics and Quantum Systems State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and Engineering Xi'an Jiaotong University Xi'an Shanxi 710049 P. R. China Contribution: Investigation (lead) Writing - review & editing (equal) Contribution: Conceptualization (supporting) Formal analysis (equal) Investigation (equal) Writing - review & editing (equal) Center for High Pressure Science State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao Hebei 066004 P. R. China Contribution: Formal analysis (equal) Contribution: Writing - review & editing (equal) Contribution: Conceptualization (supporting) Project administration (lead) Supervision (equal) Writing - review & editing (equal)

Manipulating the catalyst–electrolyte interface to push reactants into the inner Helmholtz plane (IHP) is highly desirable for efficient electrocatalysts, however, it has rarely been implemented due to the elusive electrochemical IHP and inherent inert catalyst surface. Here, we propose the introduction of local force fields by the surface hydroxyl group to engineer the electrochemical microenvironment and enhance alkaline hydrogen evolution activity. Taking a hydroxyl group immobilized Ni/Ni 3 C heterostructure as a prototype, we reveal that the local hydrogen bond induced by the surface hydroxyl group drags 4-coordinated hydrogen-bonded H 2 O molecules across the IHP to become free H 2 O and thus continuously supply reactants forcatalytic sites catalytic sites. In addition, the hydroxyl group coupled with the Ni/Ni 3 C heterostructure further lowers the water dissociation energy by polarization effects. As a direct outcome, hydroxyl-rich catalysts surpass Pt/C activity at high current density (500 mA cm −2 @ ≈276 mV) in alkaline medium.

关键词： Electrochemical Double Layer High Current Densities Hydrogen Evolution Local Hydrogen Bond Surface Hydroxyl

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Structural Modulation of Nanographenes Enabled by Defects, Size and Doping for Oxygen Reduction Reaction

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Angewandte Chemie 2024年第2期137卷

作者： Dr. Bin Wu Dr. Haibing Meng Xingbao Chen Ying Guo Li Jiang Xiaofeng Shi Dr. Jiexin Zhu Juncai Long Wenliang Gao Feng Zeng Dr. Wen-Jie Jiang Yongfa Zhu Dingsheng Wang Prof. Liqiang Mai Helmholtz-Zentrum Berlin für Materialien und Energie GmbH Albert-Einstein-Straße 15 12489 Berlin Germany Present address School of Materials Science and Engineering Nanyang Technological University 50 Nanyang Avenue 639798 Singapore Singapore Institute of Physics Humboldt University Berlin Newton-Straße 15 12489 Berlin Germany These authors contributed equally to this work College of Chemistry and Chemical Engineering Taiyuan University of Technology 030024 Taiyuan State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Luoshi Road 122 430070 Wuhan China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences (CAS) 100190 Beijing China School of Environment and Safety Engineering North University of China 030051 Taiyuan China College of Chemistry and Chemical Engineering Chongqing University Chongqing 400044 China State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University 211816 Nanjing China Department of Chemical Engineering The University of Melbourne 3010 Melbourne Victoria Department of Chemistry Tsinghua University 100084 Beijing China

Nanographenes are among the fastest-growing materials used for the oxygen reduction reaction (ORR) thanks to their low cost, environmental friendliness, excellent electrical conductivity, and scalable synthesis. The perspective of replacing precious metal-based electrocatalysts with functionalized graphene is highly desirable for reducing costs in energy conversion and storage systems. Generally, the enhanced ORR activity of the nanographenes is typically deemed to originate from the heteroatom doping effect, size effect, defects effect, and/or their synergistic effect. All these factors can efficiently modify the charge distribution on the sp 2 -conjugated carbon framework, bringing about optimized intermediate adsorption and accelerated electron transfer steps during ORR. In this review, the fundamental chemical and physical properties of nanographenes are first discussed about ORR applications. Afterward, the role of doping, size, defects, and their combined influence in boosting nanographenes’ ORR performance is introduced. Finally, significant challenges and essential perspectives of nanographenes as advanced ORR electrocatalysts are highlighted.

关键词： Dopants Size Defects Graphene ORR

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Publisher Correction: Twisted moiré conductive thermal metasurface

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Nature communications 2024年第1期15卷 2876页

作者： Huagen Li Dong Wang Guoqiang Xu Kaipeng Liu Tan Zhang Jiaxin Li Guangming Tao Shuihua Yang Yanghua Lu Run Hu Shisheng Lin Ying Li Cheng-Wei Qiu Department of Electrical and Computer Engineering National University of Singapore Kent Ridge 117583 Republic of Singapore. State Key Laboratory of Extreme Photonics and Instrumentation ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University Hangzhou 310027 China. International Joint Innovation Center Key Lab. of Advanced Micro/Nano Electronic Devices & Smart Systems of Zhejiang The Electromagnetics Academy of Zhejiang University Zhejiang University Haining 314400 China. Wuhan National Laboratory for Optoelectronics and State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China. Smart Materials for Architecture Research Lab Innovation Center of Yangtze River Delta Zhejiang University Jiaxing 314100 China. State Key Laboratory of Coal Combustion School of Energy and Power Engineering Huazhong University of Science and Technology Wuhan 430074 China. Chongqing 2D Materials Institute Chongqing 400015 China. State Key Laboratory of Extreme Photonics and Instrumentation ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University Hangzhou 310027 China. eleying@***. International Joint Innovation Center Key Lab. of Advanced Micro/Nano Electronic Devices & Smart Systems of Zhejiang The Electromagnetics Academy of Zhejiang University Zhejiang University Haining 314400 China. eleying@***. Department of Electrical and Computer Engineering National University of Singapore Kent Ridge 117583 Republic of Singapore. chengwei.qiu@nus.edu.sg.

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An Anomalous Electron Configuration Among 3dTransition Metal Atoms

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Angewandte Chemie 2022年第7期135卷

作者： Zhexin Tang Tongtong Shang Han Xu Ting Lin Ang Gao Weiguang Lin Xinyan Li Shiyu Wang Botao Yu Fanqi Meng Qinghua Zhang Xuefeng Wang Dong Su Qingbo Meng Lijun Wu Lin Gu Ce-Wen Nan Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences 100190 Beijing P. R. China School of Physical Sciences University of Chinese Academy of Sciences 100049 Beijing P. R. China State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University 100084 Beijing P. R. China Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials Department of Materials Science and Engineering Tsinghua University 100084 Beijing P. R. China College of Materials Science and Opto-Electronic Technology University of Chinese Academy of Sciences 100049 Beijing P. R. China Condensed Matter Physics and Materials Science Division Brookhaven National Laboratory 11973 Upton NY USA

Physical properties of materials are mainly determined by valence electron configurations, where different valence shells would induce divergent phenomena. In compounds containing Sc 2+ , 3 d electron occupancy is expected, the same as other transition metal atoms like Ti 3+ . But this situation still awaits experimental verification in inorganic materials. Here, we selected ScS to measure the valence electron density and orbital population of Sc 2+ through delicate quantitative convergent-beam electron diffraction. With the absence of 3 d orbital features around Sc-atom sites and the nearly bare population of t 2g orbital, the unintuitive occupation of 4 s orbital in Sc 2+ is concluded. It should be the first time to report such a special electron configuration in a transition metal compound, in which 4 s rather than 3 d orbital is preferred. Our findings reveal the distinct behavior of Sc and probable ways to modulate material properties by controlling electron orbitals.

关键词： Electron Configuration Electron Density Distribution Electron Microscopy Quantitative Convergent-Beam Electron Diffraction Scandium

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Hierarchial Zeolites: Beyond Creation of Mesoporosity: The Advantages of Polymer‐Based Dual‐Function Templates for Fabricating Hierarchical Zeolites (Adv. Funct. Mater. 12/2016)

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advanced Functional materials 2016年第12期26卷

作者： Qiwei Tian Zhaohui Liu Yihan Zhu Xinglong Dong Youssef Saih Jean‐Marie Basset Miao Sun Wei Xu Liangkui Zhu Daliang Zhang Jianfeng Huang Xiangju Meng Feng‐Shou Xiao Yu Han King Abdullah University of Science and Technology (KAUST) Advanced Membranes and Porous Materials Center (AMPMC) Physical Sciences and Engineering Division (PSE) Thuwal 23955‐6900 Saudi Arabia King Abdullah University of Science and Technology (KAUST) KAUST Catalysis Center (KCC) Physical Sciences and Engineering Division (PSE) Thuwal 23955‐6900 Saudi Arabia Cooperate Research and Development Center King Abdullah University of Science and Technology Saudi Aramco Thuwal 23955‐6900 Saudi Arabia Department of Chemistry State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin University Changchun 130012 China Imaging and Characterization Core Laboratory King Abdullah University of Science and Technology Thuwal 23955‐6900 Saudi Arabia Key Lab of Applied Chemistry of Zhejiang Province Department of Chemistry Zhejiang University Hangzhou 310028 P. R. China

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