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Tuning Intermediates Adsorption and C─N Coupling for Efficient Urea Electrosynthesis Via Doping Ni into Cu

Small methods 2024年第3期8卷 e2300811页

作者： Yangyang Zhang Yajun Zhao Marshet Getaye Sendeku Fuhua Li Jinjie Fang Yuan Wang Zhongbin Zhuang Yun Kuang Bin Liu Xiaoming Sun State Key Lab of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 P. R. China. School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University 62 Nanyang Drive Singapore 639798 Singapore. Ocean Hydrogen Energy R&D Center Research Institute of Tsinghua University in Shenzhen Shenzhen 518057 P. R. China. Department of Materials Science and Engineering City University of Hong Kong China Hong Kong SAR 999077 P. R. China.

Simultaneous electrochemical reduction of nitrite and carbon dioxide (CO ) under mild reaction conditions offers a new sustainable and low-cost approach for urea synthesis. However, the development of urea electrosynthesis thus far still suffers from low selectivity due to the high energy barrier of CO formation and the subsequent C─N coupling. In this work, a highly active dendritic Cu Ni catalyst is developed to enable the highly selective electrosynthesis of urea from co-reduction of nitrite and CO , reaching a urea Faradaic efficiency (FE) and production rate of 39.8% and 655.4 µg h cm , respectively, at -0.7 V versus reversible hydrogen electrode (RHE). In situ Fourier-transform infrared spectroscopy (FT-IR) measurements together with density functional theory (DFT) calculations demonstrate that Ni doping into Cu can significantly enhance the adsorption energetics of the key reaction intermediates and facilitate the C─N coupling. This work not only provides a new strategy to design efficient electrocatalysts for urea synthesis but also offers deep insights into the mechanism of C─N coupling during the co-reduction of nitrite and CO .

关键词： CO2 reduction C─N coupling Ni doping nitrite reduction urea synthesis

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Well-defined N3C1-anchored Single-Metal-Sites for Oxygen Reduction Reaction

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Angewandte Chemie 2023年第1期136卷

作者： Senhe Huang Dr. Diana Tranca Dr. Fermin Rodríguez-Hernández Dr. Jichao Zhang Dr. Chenbao Lu Dr. Jinhui Zhu Prof. Hai-Wei Liang Prof. Xiaodong Zhuang The Soft2D Lab State Key Laboratory of Metal Matrix Composites Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing School of Chemistry and Chemical Engineering Shanghai Jiao Tong University Shanghai 200240 China Shanghai Synchrotron Radiation Facility Zhangjiang Laboratory Shanghai Advanced Research Institute Chinese Academy of Sciences 239 Zhangheng Road Shanghai 201204 China College of Chemistry Zhengzhou University Zhengzhou 450001 Henan China Department of Chemistry University of Science and Technology of China Jinzhai Road 96 Hefei 230026 China Frontiers Science Center for Transformative Molecules Zhang Jiang Institute for Advanced Study Shanghai Jiao Tong University Shanghai 201203 China

N-, C-, O-, S-coordinated single-metal-sites (SMSs) have garnered significant attention due to the potential for significantly enhanced catalytic capabilities resulting from charge redistribution. However, significant challenges persist in the precise design of well-defined such SMSs, and the fundamental comprehension has long been impeded in case-by-case reports using carbon materials as investigation targets. In this work, the well-defined molecular catalysts with N 3 C 1 -anchored SMSs, i.e., N-confused metalloporphyrins (NCPor-Ms), are calculated for their catalytic oxygen reduction activity. Then, NCPor-Ms with corresponding N 4 -anchored SMSs (metalloporphyrins, Por-Ms), are synthesized for catalytic activity evaluation. Among all, NCPor-Co reaches the top in established volcano plots. NCPor-Co also shows the highest half-wave potential of 0.83 V vs. RHE, which is much better than that of Por-Co (0.77 V vs. RHE). Electron-rich, low band gap and regulated d -band center contribute to the high activity of NCPor-Co. This study delves into the examination of well-defined asymmetric SMS molecular catalysts, encompassing both theoretical and experimental facets. It serves as a pioneering step towards enhancing the fundamental comprehension and facilitating the development of high-performance asymmetric SMS catalysts.

关键词： Asymmetric Single-Atom Catalysts DFT Calculation Molecular Catalysts N-Confused Porphyrin Volcano Plot

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Hydrogen Electrocatalysis: Self‐Assembly of Large‐Area 2D Polycrystalline Transition Metal Carbides for Hydrogen Electrocatalysis (Adv. Mater. 50/2018)

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advanced Materials 2018年第50期30卷

作者： Xining Zang Wenshu Chen Xiaolong Zou J. Nathan Hohman Lujie Yang Buxuan Li Minsong Wei Chenhui Zhu Jiaming Liang Mohan Sanghadasa Jiajun Gu Liwei Lin Research Laboratory of Electronics Massachusetts Institute of Technology Cambridge MA 02139 USA Mechanical Engineering University of California Berkley Berkeley CA 94704 USA State Key Laboratory of Metal Matrix Composites Shanghai Jiao Tong University Shanghai 200240 China Tsinghua–Berkeley Shenzhen Institute Shenzhen 518055 China The Molecular Foundry Lawrence Berkeley National Lab Berkeley CA 94704 USA Advanced Light Source Lawrence Berkeley National Lab Berkeley CA 94704 USA U.S. Army RDECOM AMRDEC Redstone Arsenal AL 35898 USA

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Rational Design of Single Molybdenum Atoms Anchored on N‐Doped Carbon for Effective Hydrogen Evolution Reaction

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Angewandte Chemie 2017年第50期129卷

作者： Wenxing Chen Jiajing Pei Chun‐Ting He Jiawei Wan Hanlin Ren Youqi Zhu Yu Wang Juncai Dong Shubo Tian Weng‐Chon Cheong Siqi Lu Lirong Zheng Xusheng Zheng Wensheng Yan Zhongbin Zhuang Chen Chen Qing Peng Dingsheng Wang Yadong Li Department of Chemistry Tsinghua University Beijing 100084 China State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 China MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-Sen University Guangzhou 510275 China Shanghai Synchrontron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Science Shanghai 201800 China Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing China National Synchrotron Radiation Laboratory (NSRL) University of Science and Technology of China Hefei Anhui 230029 China

The highly efficient electrochemical hydrogen evolution reaction (HER) provides a promising pathway to resolve energy and environment problems. An electrocatalyst was designed with single Mo atoms (Mo‐SAs) supported on N‐doped carbon having outstanding HER performance. The structure of the catalyst was probed by aberration‐corrected scanning transmission electron microscopy (AC‐STEM) and X‐ray absorption fine structure (XAFS) spectroscopy, indicating the formation of Mo‐SAs anchored with one nitrogen atom and two carbon atoms (Mo 1 N 1 C 2 ). Importantly, the Mo 1 N 1 C 2 catalyst displayed much more excellent activity compared with Mo 2 C and MoN, and better stability than commercial Pt/C. Density functional theory (DFT) calculation revealed that the unique structure of Mo 1 N 1 C 2 moiety played a crucial effect to improve the HER performance. This work opens up new opportunities for the preparation and application of highly active and stable Mo‐based HER catalysts.

关键词： Einzelatomkatalysatoren Elektrokatalyse Molybdän N-dotierter Kohlenstoff Wasserstoffentwicklung

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Publisher Correction: Atomically engineering activation sites onto metallic 1T-MoS2 catalysts for enhanced electrochemical hydrogen evolution

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Nature communications 2020年第1期11卷 2878页

作者： Yichao Huang Yuanhui Sun Xueli Zheng Toshihiro Aoki Brian Pattengale Jier Huang Xin He Wei Bian Sabrina Younan Nicholas Williams Jun Hu Jingxuan Ge Ning Pu Xingxu Yan Xiaoqing Pan Lijun Zhang Yongge Wei Jing Gu Key Lab of Organic Optoelectronics & Molecular Engineering of Ministry of Education Department of Chemistry Tsinghua University Beijing 100084 P. R. China. Department of Chemistry and Biochemistry San Diego State University 5500 Campanile Drive San Diego CA 92182-1030 USA. State Key Laboratory of Superhard Materials Key Laboratory of Automobile Materials of MOE and School of Materials Science and Engineering Jilin University Changchun 130012 P. R. China. Department of Materials Science and Engineering Stanford University Stanford CA 94305 USA. UC Irvine Materials Research Institute (IMRI) University of California - Irvine Irvine CA 92697 USA. Department of Chemistry Marquette University Milwaukee WI 53201-1881 USA. Collaborative Innovation Center of Advanced Nuclear Energy Technology Institute of Nuclear and New Energy Technology Tsinghua University Beijing 100084 P.R. China. Department of Materials Science and Engineering University of California - Irvine Irvine CA 92697 USA. Department of Physics and Astronomy University of California - Irvine Irvine CA 92697 USA. State Key Laboratory of Superhard Materials Key Laboratory of Automobile Materials of MOE and School of Materials Science and Engineering Jilin University Changchun 130012 P. R. China. lijun_zhang@***. Key Lab of Organic Optoelectronics & Molecular Engineering of Ministry of Education Department of Chemistry Tsinghua University Beijing 100084 P. R. China. yonggewei@***. Department of Chemistry and Biochemistry San Diego State University 5500 Campanile Drive San Diego CA 92182-1030 USA. jgu@sdsu.edu.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

关键词： Catalyst synthesis Electrocatalysis Hydrogen fuel Two-dimensional materials

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Programming of Supercrystals Using Replicable DNA-Functionalized Colloids

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Angewandte Chemie 2024年第22期136卷

作者： Xiaoyun Sun Dr. Wenqiang Hua Xiaoyu Liu Dr. Jing Jin Dr. Jianing Zhang Dr. Jie Tian Prof. Bin Zheng Prof. Wei Jiang Dr. Dongbao Yao Prof. Haojun Liang Hefei National Research Center for Physical Sciences at the Microscale Department of Polymer Science and Engineering School of Chemistry and Materials Science Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) University of Science and Technology of China Hefei Anhui 230026 China Shanghai Synchrotron Radiation Facility Zhangjiang Laboratory Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China State Key Laboratory of Polymer Physics and Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun Jilin 130022 China Material Test and Analysis Lab Engineering and Materials Science Experiment Center University of Science and Technology of China Hefei Anhui 230026 China School of Chemistry and Chemical Engineering Hefei Normal University Hefei Anhui 230061 China deceased (February 11 2022)

The development of self-replicating systems is of great importance in research on the origin of life. As the most iconic molecules, nucleic acids have provided prominent examples of the fabrication of self-replicating artificial nanostructures. However, it is still challenging to construct sophisticated synthetic systems that can create large-scale or three-dimensionally ordered nanomaterials using self-replicating nanostructures. By integrating a template system containing DNA-functionalized colloidal seeds with a simplified DNA strand-displacement circuit programmed subsystem to produce DNA-functionalized colloidal copies, we developed a facile enthalpy-mediated strategy to control the replication and catalytic assembly of DNA-functionalized colloids in a time-dependent manner. The replication efficiency and crystal quality of the resulting superlattice structures can be effectively increased by regulating the molar ratio of the template to the copy colloids. By constructing binary systems from two types of gold nanoparticles (or proteins), superlattice structures with different crystal symmetries can be obtained through the replication and catalytic assembly processes. This programmable enthalpy-mediated approach was easily leveraged to achieve the phase transformation and catalytic amplification of colloidal crystals starting from different initial template crystals. This work offers a potential way to construct self-replicating artificial systems that exhibit complicated phase behaviors and can produce large-scale superlattice nanomaterials.

关键词： DNA-functionalized colloids replication DNA strand-displacement circuit colloidal crystal catalytic assembly

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A Dynamic Metal-Organic Radical Emission System

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Angewandte Chemie 2024年第12期137卷

作者： Xiang Li Prof. Yuan Wang Prof. Glib V. Baryshnikov Ihor Sahalianov Prof. Hans Ågren Yuri Tanuma Prof. Zhiyun Zhang Prof. Cheng Qian Dr. Muyu Cong Prof. Tao Yi Prof. Hongwei Wu State Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Lab of Science and Technology of Eco-Textile Ministry of Education College of Chemistry and Chemical Engineering Donghua University Shanghai 201620 China Beijing National Laboratory of Molecular Sciences and CAS Key Laboratory of Colloid Interface and Thermodynamics Institute of Chemistry Chinese Academy of Sciences North First Street 2 Zhongguancun Beijing 100190 China Laboratory of Organic Electronics Department of Science and Technology Linköping University SE-60174 Norrköping Sweden Wallenberg Initiative Materials Science for Sustainability Department of Science and Technology Linköping University SE-60174 Norrköping Sweden Department of Physics and Astronomy Uppsala University Uppsala SE-751 20 Sweden Jožef Stefan Institute Jamova 39 1000 Ljubljana Slovenia Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Center for Materiobiology and Dynamic Chemistry East China University of Science & Technology Shanghai 200237 P. R. China

Developing new organic radical emission systems and regulating their luminescence properties presents a significant challenge. Herein, we build dynamic and multi-emission band radical luminescence systems by co-assembling inorganic metal salts with carbonyl compounds in ionic liquids. After the assembling, dual-band, and excitation wavelength-dependent emission was observed upon ultraviolet light irradiation, one emission band originates from carbonyl radical after light irradiation, the other band from the ligand-metal charge transfer (LMCT) state, which benefits from the charge transfer from the radicals to the metal salts. The dual emission centers also introduce excitation wavelength-dependent properties for the molecules. In addition, three-band emission covering the visible and near-infrared regions can be shown when two or three kinds of metal ions are simultaneously doped into the radical system driven by the ligand-metal-metal charge transfer (LMMCT). Interestingly, visible light can quickly quench the radical emission of systems, thus realizing a dynamic luminescence. The LMMCT effect and strong supramolecular interactions significantly improve the photoluminescence quantum yield by up to 67.2 %. Moreover, such materials can be successfully used for detecting radioactive metal ions and information encryption. This study develops a platform for manufacturing various metal-organic radical emission systems with diverse properties.

关键词： metal-organic radical multi-band emission dynamic luminescence supramolecular interactions information encryption

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Publisher Correction:Vertical‑Aligned and Ordered‑Active Architecture of Heterostructured Fibers for High Electrochemical Capacitance

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advanced Fiber Materials 2024年第6期6卷 1992-1992页

作者： Xiaolin Zhu Hui Qiu Yang Zhang Zengming Man Wangyang Lu Ningzhong Bao Guan Wu National Engineering Lab for Textile Fiber Materials and Processing Technology Zhejiang Sci-Tech UniversityHangzhou 310018People’s Republic of China Zhejiang Provincial Innovation Center of Advanced Textile Technology Shaoxing 312000People’s Republic of China State Key Laboratory of Materials‑Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009People’s Republic of China

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Author Correction: Ampere-hour-scale soft-package potassium-ion hybrid capacitors enabling 6-minute fast-charging

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Nature communications 2024年第1期15卷 374页

作者： Huanxin Li Yi Gong Haihui Zhou Jing Li Kai Yang Boyang Mao Jincan Zhang Yan Shi Jinhai Deng Mingxuan Mao Zhongyuan Huang Shuqiang Jiao Yafei Kuang Yunlong Zhao Shenglian Luo State Key Laboratory for Chemo/Biosensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University 410082 Changsha Hunan China. Department of Engineering University of Cambridge 9 JJ Thomson Avenue Cambridge CB3 0FA UK. Department of Chemistry Physical & Theoretical Chemistry Laboratory University of Oxford South Parks Road Oxford OX1 3QZ UK. Electrochemical Innovation Lab Department of Chemical Engineering University College London London WC1E 7JE UK. Dyson School of Design Engineering Imperial College London London SW7 2BX UK. Advanced Technology Institute University of Surrey Guildford Surrey GU2 7XH UK. State Key Laboratory for Chemo/Biosensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University 410082 Changsha Hunan China. haihuizh@***. Department of Chemical & Process Engineering University of Surrey Guildford GU2 7XH UK. College of Materials and Metallurgy Guizhou University 550025 Guiyang China. King's College London London SE1 1UL UK. Department of Electrical and Electronic Engineering Imperial College London London SW7 2AZ UK. State Key Laboratory of Advanced Metallurgy University of Science and Technology Beijing 100083 Beijing China. sjiao@***. Dyson School of Design Engineering Imperial College London London SW7 2BX UK. yunlong.zhao@imperial.ac.uk. State Key Laboratory for Chemo/Biosensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University 410082 Changsha Hunan China. sllou@***.

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An Early Stage Researcher's Primer on Systems Medicine Terminology

Network and Systems Medicine

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Network and Systems Medicine 2021年第1期4卷 2-50页

作者： Zanin, Massimiliano Aitya, Nadim A.A. Basilio, José Baumbach, Jan Benis, Arriel Behera, Chandan K. Bucholc, Magda Castiglione, Filippo Chouvarda, Ioanna Comte, Blandine Dao, Tien-Tuan Ding, Xuemei Pujos-Guillot, Estelle Filipovic, Nenad Finn, David P. Glass, David H. Harel, Nissim Iesmantas, Tomas Ivanoska, Ilinka Joshi, Alok Boudjeltia, Karim Zouaoui Kaoui, Badr Kaur, Daman Maguire, Liam P. McClean, Paula L. McCombe, Niamh De Miranda, João Luís Moisescu, Mihnea Alexandru Pappalardo, Francesco Polster, Annikka Prasad, Girijesh Rozman, Damjana Sacala, Ioan Sanchez-Bornot, Jose M. Schmid, Johannes A. Sharp, Trevor Solé-Casals, Jordi Spiwok, Vojtěch Spyrou, George M. Stalidzans, Egils Stres, Blaa Sustersic, Tijana Symeonidis, Ioannis Tieri, Paolo Todd, Stephen Van Steen, Kristel Veneva, Milena Wang, Da-Hui Wang, Haiying Wang, Hui Watterson, Steven Wong-Lin, Kongfatt Yang, Su Zou, Xin Schmidt, Harald H.H.W. Centro de Tecnología Biomédica Universidad Politécnica de Madrid Madrid Spain Intelligent Systems Research Centre School of Computing Engineering and Intelligent Systems Ulster University Ulster United Kingdom Center for Physiology and Pharmacology Institute of Vascular Biology and Thrombosis Research Medical University of Vienna Vienna Austria TUM School of Life Sciences Weihenstephan Technical University of Munich Freising Germany Holon Israel CNR National Research Council IAC Institute for Applied Computing Rome Italy Lab of Computing Medical Informatics and Biomedical Imaging Technologies School of Medicine Aristotle University of Thessaloniki Thessaloniki Greece Université Clermont Auvergne INRAE UNH Plateforme d'Exploration du Métabolisme MetaboHUB Clermont Clermont-Ferrand France Université de Technologie de Compiègne Compiègne France Labex MS2T Control of Technological Systems-of-Systems CNRS and Université de Technologie de Compiègne Compiègne France Faculty of Engineering University of Kragujevac Kragujevac Serbia Kragujevac Serbia Steinbeis Advanced Risk Technologies Institute Doo Kragujevac Kragujevac Serbia Pharmacology and Therapeutics School of Medicine Galway Neuroscience Centre National University of Ireland Galway Ireland School of Computing Ulster University Ulster United Kingdom Holon Israel Department of Mathematics and Natural Sciences Kaunas University of Technology Kaunas Lithuania Faculty of Computer Science and Engineering Ss. Cyril and Methodius University Skopje Macedonia Medicine Faculty Université Libre de Bruxelles CHU de Charleroi Charleroi Belgium Northern Ireland Centre for Stratified Medicine Biomedical Sciences Research Institute Ulster University Ulster United Kingdom Escola Superior de Tecnologia e Gestão Instituto Politécnico de Portalegre Portalegre Portugal Instituto Superior Técnico Universidade de Lisboa Lisboa Portugal Faculty of Automatic Control and Computers University Politehnica of B

Background: Systems Medicine is a novel approach to medicine, that is, an interdisciplinary field that considers the human body as a system, composed of multiple parts and of complex relationships at multiple levels, and further integrated into an environment. Exploring Systems Medicine implies understanding and combining concepts coming from diametral different fields, including medicine, biology, statistics, modeling and simulation, and data science. Such heterogeneity leads to semantic issues, which may slow down implementation and fruitful interaction between these highly diverse fields. Methods: In this review, we collect and explain more than100 terms related to Systems Medicine. These include both modeling and data science terms and basic systems medicine terms, along with some synthetic definitions, examples of applications, and lists of relevant references. Results: This glossary aims at being a first aid kit for the Systems Medicine researcher facing an unfamiliar term, where he/she can get a first understanding of them, and, more importantly, examples and references for digging into the topic. © Massimiliano Zanin et al., 2021;Published by Mary Ann Liebert, Inc. 2021.

关键词： Semantics

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