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Pseudocapacitance: Emergent Pseudocapacitance of 2D Nanomaterials (Adv. Energy Mater. 13/2018)

advanced Energy materials 2018年第13期8卷

作者： Xu Yu Sol Yun Jeong Seok Yeon Pallab Bhattacharya Libin Wang Seung Woo Lee Xianluo Hu Ho Seok Park School of Chemical Engineering Sungkyunkwan University (SKKU) 2066 Seobu‐ro Jangan‐gu Suwon 440‐746 Republic of Korea School of Chemistry and Chemical Engineering Yangzhou University Jiangsu Province Yangzhou 225002 China State Key Laboratory of Materials Processing and Die and Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China George W. Woodruff School of Mechanical Engineering Georgia Institute of Technology Atlanta GA 30332 USA Department of Health Sciences and Technology Samsung Advanced Institute for Health Sciences and Technology (SAIHST) Sungkyunkwan University 2066 Seoburo Jangan‐gu Suwon 440‐746 Republic of Korea

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Tailoring magnetic order via atomically stacking 3d/5d electrons

arXiv

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arXiv 2020年

作者： Huang, Ke Wu, Liang Wang, Maoyu Swain, Nyayabanta Motapothula, M. Luo, Yongzheng Han, Kun Chen, Mingfeng Ye, Chen Yang, Allen Jian Xu, Huan Qi, Dong-Chen N’Diaye, Alpha T. Panagopoulos, Christos Primetzhofer, Daniel Shen, Lei Sengupta, Pinaki Ma, Jing Feng, Zhenxing Nan, Ce-Wen Wang, X. Renshaw Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore637371 Singapore School of Materials Science and Engineering State Key Laboratory of New Ceramics and Fine Processing Tsinghua University Beijing100084 China Department of Physics and Astronomy Rutgers University PiscatawayNJ08854 United States School of Chemical Biological and Environmental Engineering Oregon State University CorvallisOR97331 United States Department of Physics and Astronomy Uppsala University Box 516 UppsalaSE-75120 Sweden Department of Physics SRM University AP Andhra Pradesh Amaravati522-502 India Department of Mechanical Engineering National University of Singapore Singapore117575 Singapore School of Electrical and Electronic Engineering Nanyang Technological University Singapore639798 Singapore ARC Centre of Excellence in Future Low-Energy Electronics Technologies School of Chemistry Physics and Mechanical Engineering Queensland University of Technology BrisbaneQLD4001 Australia Department of Chemistry and Physics La Trobe Institute for Molecular Science La Trobe University MelbourneVIC3086 Australia Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States

The ability to tune magnetic orders, such as magnetic anisotropy and topological spin texture, is desired in order to achieve high-performance spintronic devices. A recent strategy has been to employ interfacial engineering techniques, such as the introduction of spin-correlated interfacial coupling, to tailor magnetic orders and achieve novel magnetic properties. We chose a unique polar-nonpolar LaMnO3/SrIrO3 superlattice because Mn (3d)/Ir (5d) oxides exhibit rich magnetic behaviors and strong spin-orbit coupling through the entanglement of their 3d and 5d electrons. Through magnetization and magnetotransport measurements, we found that the magnetic order is interface-dominated as the superlattice period is decreased. We were able to then effectively modify the magnetization, tilt of the ferromagnetic easy axis, and symmetry transition of the anisotropic magnetoresistance of the LaMnO3/SrIrO3 superlattice by introducing additional Mn (3d) and Ir (5d) interfaces. Further investigations using in-depth first-principles calculations and numerical simulations revealed that these magnetic behaviors could be understood by the 3d/5d electron correlation and Rashba spin-orbit coupling. The results reported here demonstrate a new route to synchronously engineer magnetic properties through the atomic stacking of different electrons, contributing to future applications. Copyright © 2020, The Authors. All rights reserved.

关键词： Electrons

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A Honeycomb‐Like Bulk Superstructure of Carbon Nanosheets for Electrocatalysis and Energy Storage

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Angewandte Chemie 2020年第44期132卷

作者： Lianli Zou Chun‐Chao Hou Qiuju Wang Yong‐Sheng Wei Zheng Liu Jun‐Sheng Qin Huan Pang Qiang Xu Research Institute of Electrochemical Energy National Institute of Advanced Industrial Science and Technology (AIST) Ikeda Osaka 563-8577 Japan Graduate School of Engineering Kobe University Nada Ku Kobe Hyogo 657-8501 Japan AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory (ChEM-OIL) National Institute of Advanced Industrial Science and Technology (AIST) Sakyo-ku Kyoto 606-8501 Japan Inorganic Functional Materials Research Institute National Institute of Advanced Industrial Science and Technology (AIST) 2266-98 Anagahora Shimoshidami Moriyamaku Nagoya Aichi 463-8560 Japan State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry International Center of Future Science Jilin University Changchun 130012 P. R. China School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225009 China

Superstructures have attracted extensive attention because of their potential applications in materials science and biology. Herein, we fabricate the first centimeter‐sized porous superstructure of carbon nanosheets (SCNS) by using metal–organic framework nanoparticles as a template and polyvinylpyrrolidone as an additional carbon source. The SCNS shows a honeycomb‐like morphology with wall‐sharing carbon cages, in each cavity of which a porous carbon sphere is encapsulated. A single piece of SCNS is directly used as the electrode for a two‐electrode symmetrical supercapacitor cell without any binders and supports, benefiting from its advantage in ultra‐large geometric size, and the Fe‐immobilized SCNS exhibits excellent catalytic performances for oxygen reduction reaction and in a Zn–air battery. This synthetic strategy presents a facile approach for preparing functional SCNS at centimetric scale with controllable morphologies and compositions favoring the fabrication of energy devices.

关键词： carbon nanosheets honeycomb-like structures metal–organic frameworks oxygen reduction reaction superstructures

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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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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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Author Correction: Real-space measurement of orbital electron populations for Li1-xCoO2

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Nature Communications 2022年第1期13卷 1页

作者： Tongtong Shang Dongdong Xiao Xiaohui Rong Ang Gao Ting Lin Zhexin Tang Xiaozhi Liu Xinyan Li Qinghua Zhang Ruijuan Xiao Xuefeng Wang Dong Su Yong-Sheng Hu Hong Li Lin Gu Fanqi Meng Ce-Wen Nan Yuren Wen Qian Yu Ze Zhang Vaclav Petricek Lijun Wu Yimei Zhu Jian-Min Zuo Jing Zhu Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 P. R. China School of Physical Sciences University of Chinese Academy of Sciences Beijing 100049 China Songshan Lake Materials Laboratory Dongguan 523808 P. R. China State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 P. R. China School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 P. R. China Department of Materials Science and Engineering Center of Electron Microscopy and State Key Laboratory of Silicon Materials Zhejiang University Hangzhou 310027 P. R. China Institute of Physics Academy of Sciences of the Czech Republic Praha 180 40 Czech Republic Condensed Matter Physics and Materials Science Division Brookhaven National Laboratory Upton New York 11973 USA Department of Materials Science and Engineering University of Illinois at Urbana Champaign 1304 W Green St Urbana 61801 USA Beijing National Center for Electron Microscopy Laboratory of Advanced Materials Department of Materials Science and Engineering Tsinghua University Beijing 100084 P. R. China

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Near-Infrared Emission Beyond 900 nm from Stable Radicals in Nonconjugated Poly(diphenylmethane)

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Angewandte Chemie 2024年第24期136卷

作者： Ziteng Zhang Zuping Xiong Dr. Jianyu Zhang Bo Chu Xiong Liu Weihao Tu Dr. Lei Wang Prof. Jing Zhi Sun Prof. Chengjian Zhang Prof. Haoke Zhang Prof. Xinghong Zhang Prof. Ben Zhong Tang Department of Polymer Science and Engineering Zhejiang University Hangzhou 310058 China State Key Laboratory of Motor Vehicle Biofuel Technology International Research Center for X Polymers Zhejiang University Hangzhou 310058 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Zhejiang University Hangzhou 310058 China Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University Hangzhou 311215 China Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Institute for Advanced Study The Hong Kong University of Science and Technology Hong Kong 999077 China Centre of Healthcare Materials Shaoxing Institute Zhejiang University Shaoxing 312000 China School of Science and Engineering Shenzhen Institute of Aggregate Science and Technology The Chinese University of Hong Kong Shenzhen Guangdong 518172 China

Organic radicals with narrow energy gaps are highly sought-after for the production of near-infrared (NIR) fluorophores. However, the current repertoire of developed organic radicals is notably limited, facing challenges related to stability and low fluorescence efficiency. This study addresses these limitations by achieving stable radicals in nonconjugated poly(diphenylmethane) (PDPM). Notably, PDPM exhibits a well-balanced structural flexibility and rigidity, resulting in a robust intra-/inter-chain through-space conjugation (TSC). The stable radicals within PDPM, coupled with strong TSC, yield a remarkable full-spectrum emission spanning from blue to NIR beyond 900 nm. This extensive tunability is achieved through careful adjustments of concentration and excitation wavelength. The findings highlight the efficacy of polymerization in stabilizing radicals and introduce a novel approach for developing nonconjugated NIR emitters based on triphenylmethane subunits.

关键词： Through-space conjugation Near-infrared emission Radicals Nonconjugated polymers

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NIR Clusteroluminescence of Non-conjugated Phenolic Resins Enabled by Through-Space Interactions

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Angewandte Chemie 2023年第30期135卷

作者： Ziteng Zhang Dr. Jianyu Zhang Zuping Xiong Bo Chu Prof. Chengjian Zhang Prof. Jing Zhi Sun Prof. Haoke Zhang Prof. Xing-Hong Zhang Prof. Ben Zhong Tang Department of Polymer Science and Engineering Zhejiang University 310058 Hangzhou China State Key Laboratory of Motor Vehicle Biofuel Technology International Research Center for X Polymers Zhejiang University 310058 Hangzhou China Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University 311215 Hangzhou China Department of Chemistry Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction and Institute for Advanced Study The Hong Kong University of Science and Technology 999077 Hong Kong China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Zhejiang University 310058 Hangzhou China Centre of Healthcare Materials Shaoxing Institute Zhejiang University 312000 Shaoxing China School of Science and Engineering Shenzhen Institute of Aggregate Science and Technology The Chinese University of Hong Kong 518172 Shenzhen Guangdong China

Clusteroluminescence (CL) and through-space interactions (TSIs) of non-conjugated molecules have drawn more attention due to their unique photophysical behaviors that are different from largely conjugated luminogens. However, achieving red and even near-infrared (NIR) emission from such systems is still challenging due to the intrinsic drawbacks of non-conjugated molecules and the lack of theories for structure–property relationships. In this work, six phenolic resins are designed and synthesized based on two molecule-engineering strategies: increasing the number of TSIs units and introducing electron-donating/-withdrawing groups. All phenolic resins are verified as luminogens with CL property (CLgens), and the first example of CLgens with NIR emission (maximum emission wavelength ≥680 nm) and high absolute quantum yield (47 %) is reported. Experiments and theoretical analysis reveal that two TSIs types, through-space locally excited state and through-space charge transfer state, play essential roles in achieving CL from these non-conjugated polymers, which could be manipulated via changing structural conformation and electron density or altering electron transition behaviors. This work not only provides an approach to manipulate TSIs and CL of non-conjugated polymers but also endows commercially available phenolic resins with high practical value as luminescence materials.

关键词： Clusteroluminescence Near-Infrared Luminescence Phenolic Resin Through-Space Interactions

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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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Regio-Regular Polymer Acceptors Enabled by Determined Fluorination on End Groups for All-Polymer Solar Cells with 15.2 % Efficiency

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Angewandte Chemie 2021年第18期133卷

作者： Han Yu Mingao Pan Rui Sun Indunil Agunawela Dr. Jianquan Zhang Yuhao Li Zhenyu Qi Han Han Xinhui Zou Wentao Zhou Dr. Shangshang Chen Dr. Joshua Yuk Lin Lai Siwei Luo Dr. Zhenghui Luo Prof. Dahui Zhao Prof. Xinhui Lu Prof. Harald Ade Prof. Fei Huang Prof. Jie Min Prof. He Yan The Institute for Advanced Studies Wuhan University Wuhan 430072 China Hong Kong University of Science and Technology–Shenzhen Research Institute No. 9 Yuexing 1st RD Hi-tech Park Nanshan Shenzhen 518057 China Department of Chemistry Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials Energy Institute and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration & Reconstruction Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China Department of Physics and Organic and Carbon Electronics Laboratories (ORaCEL) North Carolina State University Raleigh NC 27695 USA Department of Physics Chinese University of Hong Kong New Territories Hong Kong 999077 China Beijing National Laboratory for Molecular Sciences Centre for Soft Matter Science and Engineering Key Lab of Polymer Chemistry & Physics of the Ministry of Education College of Chemistry Peking University Beijing 100871 China Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and Devices South China University of Technology Guangzhou 510640 China Key Laboratory of Materials Processing and Mold Zhengzhou University Ministry of Education 450002 Zhengzhou China

Polymerization sites of small molecule acceptors (SMAs) play vital roles in determining device performance of all-polymer solar cells (all-PSCs). Different from our recent work about fluoro- and bromo- co-modified end group of IC-FBr (a mixture of IC-FBr1 and IC-FBr2), in this paper, we synthesized and purified two regiospecific fluoro- and bromo- substituted end groups (IC-FBr- o & IC-FBr- m ), which were then employed to construct two regio-regular polymer acceptors named PYF-T- o and PYF-T- m , respectively . In comparison with its isomeric counterparts named PYF-T- m with different conjugated coupling sites, PYF-T- o exhibits stronger and bathochromic absorption to achieve better photon harvesting. Meanwhile, PYF-T- o adopts more ordered inter-chain packing and suitable phase separation after blending with the donor polymer PM6, which resulted in suppressed charge recombination and efficient charge transport. Strikingly, we observed a dramatic performance difference between the two isomeric polymer acceptors PYF-T- o and PYF-T- m . While devices based on PM6:PYF-T- o can yield power conversion efficiency (PCE) of 15.2 %, devices based on PM6:PYF-T- m only show poor efficiencies of 1.4 %. This work demonstrates the success of configuration-unique fluorinated end groups in designing high-performance regular polymer acceptors, which provides guidelines towards developing all-PSCs with better efficiencies.

关键词： all-polymer solar cells fluorinated end group isomeric effect organic solar cells polymer acceptors

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