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Possible structural origin of superconductivity in Sr-doped Bi2Se3

Physical Review materials 2018年第1期2卷 014201-014201页

作者： Zhuojun Li Meng Wang Dejiong Zhang Nan Feng Wenxiang Jiang Chaoqun Han Weijiong Chen Mao Ye Chunlei Gao Jinfeng Jia Jixue Li Shan Qiao Dong Qian Ben Xu He Tian Bo Gao CAS Center for Excellence in Superconducting Electronics (CENSE) Shanghai 200050 China State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences 865 Changning Road Shanghai 200050 China University of Chinese Academy of Sciences Beijing 100049 China Center of Electron Microscopy and State Key Laboratory of Silicon Materials School of Materials Science and Engineering Zhejiang University Hangzhou 310027 China State Key Laboratory of New Ceramics and Fine Processing Department of Materials Science and Engineering Tsinghua University Beijing 100084 People's Republic of China Key Laboratory of Artificial Structures and Quantum Control (Ministry of Education) School of Physics and Astronomy Shanghai Jiao Tong University Shanghai 200240 China State Key Laboratory of Surface Physics and Department of Physics Fudan University Shanghai 200433 China Collaborative Innovation Center of Advanced Microstructures Nanjing 210093 China

Doping bismuth selenide (Bi2Se3) with elements such as copper and strontium (Sr) can induce superconductivity, making the doped materials interesting candidates to explore potential topological superconducting behaviors. It was thought that the superconductivity of doped Bi2Se3 was induced by dopant atoms intercalated in van der Waals gaps. However, several experiments have shown that the intercalation of dopant atoms may not necessarily make doped Bi2Se3 superconducting. Thus, the structural origin of superconductivity in doped Bi2Se3 remains an open question. Herein, we combined material synthesis and characterization, high-resolution transmission electron microscopy, and first-principles calculations to study the doping structure of Sr-doped Bi2Se3. We found that the emergence of superconductivity is strongly related with n-type dopant atoms. Atomic-level energy-dispersive x-ray mapping revealed various n-type Sr dopants that occupy intercalated and interstitial positions. First-principles calculations showed that the formation energy of a specific interstitial Sr doping position depends strongly on the Sr doping level. This site changes from a metastable position at low Sr doping level to a stable position at high Sr doping level. The calculation results explain why quenching is necessary to obtain superconducting samples when the Sr doping level is low and also why slow furnace cooling can yield superconducting samples when the Sr doping level is high. Our findings suggest that Sr atoms doped at interstitial locations, instead of those intercalated in van der Waals gaps, are most likely to be responsible for the emergence of superconductivity in Sr-doped Bi2Se3.

关键词： Dopants Impurities in superconductors

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Solution-Grown Chloride Perovskite Crystal of Red Afterglow

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Angewandte Chemie 2021年第46期133卷

作者： Wei Zheng Xiuling Li Nianqiao Liu Shao Yan Xiaojia Wang Xiangzhou Zhang Yeqi Liu Yanjie Liang Yuhai Zhang Hong Liu Collaborative Innovation Center of Technology and Equipment for Biological Diagnosis and Therapy in Universities of Shandong Institute for Advanced Interdisciplinary Research (iAIR) University of Jinan Jinan 250022 Shandong China School of Physics and Technology University of Jinan Jinan 250022 Shandong China Key Laboratory for Liquid-Solid Structure Evolution and Processing of Materials Ministry of Education Shandong University Jinan 250061 P. R. China State Key Laboratory of Crystal Materials Shandong University 27 Shandanan Road Jinan Shandong 250100 China

We report the growth of a halide-based double perovskite, Cs 2 Na x Ag 1− x InCl 6 : y %Mn, via a facile hydrothermal reaction at 180 °C. Through a co-doping strategy of both Na + and Mn 2+ , the as-prepared crystals exhibited a red afterglow featuring a high color purity (ca. 100 %) and a long duration time (>5400 s), three orders of magnitude longer than those solution-processed organic afterglow crystals. The energy transfer (ET) process between self-trapped excitons (STE) and activators was investigated through time-resolved spectroscopy, which suggested an ET efficiency up to 41 %. Importantly, the nominal concentration of dopants, especially in the case of Na + , was found a useful tool to control both energy level and number distribution of traps. Cryogenic afterglow measurements suggested that the afterglow phenomenon was likely governed by thermal-activated exciton diffusion and electron tunneling process.

关键词： doped chloride perovskite double perovskites hydrothermal synthesis red afterglow crystals self-trapped excitons

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Design of Ligand-Nonbridging Sites in Metal–Organic Frameworks for Boosting Lithium Storage Capacity

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Angewandte Chemie 2024年第6期137卷

作者： Lanju Sun Chongzhi Zhu Lukun Li Rumeng Zheng Jian Yuan Zhiliang Li Jikai Sun Guan Sheng Hao Wu Qingdao Engineering Research Center of Agricultural Recycling Economy Materials College of Chemistry and Pharmaceutical Sciences Qingdao Agricultural University 266109 Qingdao China Institute of Frontier Chemistry School of Chemistry and Chemical Engineering Shandong University 266237 Qingdao China Center for Electron Microscopy Institute for Frontier and Interdisciplinary Sciences State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology College of Materials Science and Engineering and College of Chemical Engineering Zhejiang University of Technology 310014 Hangzhou China School of Materials Science and Engineering State Key Laboratory of Heavy Oil Processing China University of Petroleum (East China) 266580 Qingdao China

Metal–organic frameworks (MOFs) are lagging in the use of lithium-ion batteries (LIBs), ascribing to full coordination between metal nodes and organic ligands, to a large extent. By integrating a modulator into a ligand with missing bridging functionality, this study elucidates the role of non-bridging defect sites in MOFs in tailoring lithium storage performance. A fully bridged pristine MOF (p-MOF) utilizing the meso-tetra(4-carboxylphenyl) porphyrin ligand is compared with a modified MOF containing non-bridging defects (d-MOF) introduced by a homologous ligand, tris(4-carboxyphenyl) porphyrin. Spectroscopic and cryogenic low-dose electron microscopy techniques verify the presence of non-bridging defect sites in the d-MOF and reveal their explicit local structure. Density functional theory calculations show significantly enhanced Li + adsorption energies and reduced Li + migration barriers at the non-bridging sites in the d-MOF compared to the fully bridging sites in the p-MOF. As a result, the d-MOF exhibits exceptional lithium storage performance, achieving a high capacity of 761 mAh g −1 at 0.05 A g −1 and superior rate performance of 203 mAh g −1 at 5 A g −1 , which substantially outperform the p-MOF. This study highlights the potential of modulating MOFs with non-bridging defects to develop high-performance LIBs.

关键词： Lithium storage Ligand engineering Defects Metal–organic frameworks Adsorption energy

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Boosting Electrocatalytic Activity of 3d-Block Metal (Hydro)oxides by Ligand-Induced Conversion

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Angewandte Chemie 2021年第19期133卷

作者： Dr. Wenxian Liu Dong Zheng Dr. Tianqi Deng Dr. Qiaoli Chen Chongzhi Zhu Chengjie Pei Dr. Hai Li Dr. Fangfang Wu Dr. Wenhui Shi Dr. Shuo-Wang Yang Prof. Yihan Zhu Prof. Xiehong Cao College of Materials Science and Engineering State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology Center for Electron Microscopy Center for Membrane Separation and Water Science & Technology College of Chemical Engineering Zhejiang University of Technology 18 Chaowang Road Hangzhou Zhejiang 310014 P. R. China Institute of High Performance Computing Agency for Science Technology and Research 1 Fusionopolis Way #16-16 Connexis Singapore 138632 Singapore Key Laboratory of Flexible Electronics and Institute of Advanced Materials Jiangsu National Synergetic Innovation Center for Advanced Materials Nanjing Tech University 30 South Puzhu Road Nanjing Jiangsu 211816 P. R. China

The 3d-transition-metal (hydro)oxides belong to a group of highly efficient, scalable and inexpensive electrocatalysts for widespread energy-related applications that feature easily tailorable crystal and electronic structures. We propose a general strategy to further boost their electrocatalytic activities by introducing organic ligands into the framework, considering that most 3d-metal (hydro)oxides usually exhibit quite strong binding with reaction intermediates and thus compromised activity due to the scaling relations. Involving weakly bonded ligands downshifts the d-band center, which narrows the band gap, and optimizes the adsorption of these intermediates. For example, the activity of the oxygen evolution reaction (OER) can be greatly promoted by ≈5.7 times over a NiCo layered double hydroxide (LDH) after a terephthalic acid (TPA)-induced conversion process, arising from the reduced energy barrier of the deprotonation of OH* to O*. Impressively, the proposed ligand-induced conversion strategy is applicable to a series of 3d-block metal (hydro)oxides, including NiFe 2 O 4 , NiCo 2 O 4 , and NiZn LDH, providing a general structural upgrading scheme for existing high-performance electrocatalytic systems.

关键词： electronic-structure engineering flexible Zn–air batteries layered double hydroxides metal–organic frameworks oxygen evolution reaction

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Corrigendum to ‘Characterization and formation mechanism of ultra-fine ferrite grains in dissimilar metal weld between austenitic stainless steel and low alloy ferritic steel’ [Mater. Charact. https://***/10.1016/***.2020.110777]

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materials Characterization 2021年 174卷

作者： Xiaogang Li Zhipeng Cai Xin Chen Shuqing Dong Wenhe Cai Xiaoming Shi Chaoyu Han Yu Zhang Kejian Li Jiluan Pan Department of Mechanical Engineering Tsinghua University Beijing 100084 China Key Laboratory for Advanced Materials Processing Technology Ministry of Education Beijing 100084 China State Key Laboratory of Tribology Tsinghua University Beijing 100084 China Collaborative Innovation Center of Advanced Nuclear Energy Technology Tsinghua University Beijing 100084 China China Datang Corporation Science and Technological Research Institute Thermal Power Technology Research Institute Beijing 100040 China Jiangsu Nantong Power Generation Co. Ltd. Nantong 226000 China

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A Highly Active Molybdenum Carbide Catalyst with Dynamic Carbon Flux for Reverse Water-Gas Shift Reaction

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Angewandte Chemie 2024年第6期137卷

作者： Mengtao Zhang Yuchen Zhu Jie Yan Junzhong Xie Tao Yu Mi Peng Jiayun Zhao Yao Xu Aowen Li ChunJiang Jia Lin He Meng Wang Wu Zhou Rongming Wang Hong Jiang Chuan Shi Jose Rodriguez Ding Ma Beijing National Laboratory for Molecular Sciences New Cornerstone Laboratory College of Chemistry and Molecular Engineering Peking University Beijing 100871 China State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing 100083 China State Key Laboratory of Fine Chemicals College of Chemical Engineering Dalian University of Technology Dalian 116024 China School of Physical Sciences and CAS Key Laboratory of Vacuum Physics University of Chinese Academy of Sciences Beijing 100049 China Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials School of Chemistry and Chemical Engineering Shandong University Jinan 250100 China State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics (LICP) Chinese Academy of Sciences Lanzhou 730000 China Chemistry Division Building 555 Brookhaven National Laboratory Post Office Box 5000 Upton NY 11973-5000 USA

Molybdenum carbide has been reported as an efficient and stable catalyst for reverse water-gas shift (RWGS) reaction. The conventional understanding of the mechanism suggests domination of the surface phenomena, with only surface or subsurface layers partaking in the catalytic cycle. In this study, we presented a highly active MoC catalyst from carburization process, which showed a mass-specific reaction rate over 260 μm with dynamic carbon flux in the bulk phase of the catalyst. Through Isotopic Temperature-Programmed Reaction (ITPR) analysis and Environmental Transmission Electron Microscopy (ETEM), we discerned dynamic carbon flow circulating between the α-MoC bulk phase and the gas phase reactants under the RWGS reaction atmosphere. This circulation, essential to maintaining the structural stability of the metastable α-MoC and its ultra-high reactivity, is accompanied by thorough carbon component exchange among the bulk, the surface and the gas-phase reactants during the reaction process.

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New Opportunities and Challenges of Smart Polymers in Post-Translational Modification Proteomics

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advanced materials (Deerfield Beach, Fla.) 2017年第20期29卷 2017 May;29(20)页

作者： Guangyan Qing Qi Lu Yuting Xiong Lei Zhang Hongxi Wang Xiuling Li Xinmiao Liang Taolei Sun State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China. Institute of Biomedical and Pharmaceutical Sciences College of Bioengineering Hubei University of Technology 28 Nanli Road Wuhan 430068 P. R. China. Key Laboratory of Separation Science for Analytical Chemistry Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 P. R. China. International School of Materials Science and Engineering Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China.

Protein post-translational modifications (PTMs), which denote covalent additions of various functional groups (e.g., phosphate, glycan, methyl, or ubiquitin) to proteins, significantly increase protein complexity and diversity. PTMs play crucial roles in the regulation of protein functions and numerous cellular processes. However, in a living organism, native PTM proteins are typically present at substoichiometric levels, considerably impeding mass-spectrometry-based analyses and identification. Over the past decade, the demand for in-depth PTM proteomics studies has spawned a variety of selective affinity materials capable of capturing trace amounts of PTM peptides from highly complex biosamples. However, novel design ideas or strategies are urgently required for fulfilling the increasingly complex and accurate requirements of PTM proteomics analysis, which can hardly be met by using conventional enrichment materials. Considering two typical types of protein PTMs, phosphorylation and glycosylation, an overview of polymeric enrichment materials is provided here, with an emphasis on the superiority of smart-polymer-based materials that can function in intelligent modes. Moreover, some smart separation materials are introduced to demonstrate the enticing prospects and the challenges of smart polymers applied in PTM proteomics.

关键词： enrichment interfaces post-translational modification proteomics smart polymers

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Isolation and Crystallographic Characterization of the Labile Isomer of Y@C82Cocrystallized with Ni(OEP): Unprecedented Dimerization of Pristine Metallofullerenes

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Angewandte Chemie 2016年第32期128卷

作者： Lipiao Bao Changwang Pan Zdenek Slanina Filip Uhlik Takeshi Akasaka Xing Lu State Key Laboratory of Materials Processing and Die & Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology 1037 Luoyu Road Wuhan 430074 P.R. China Life Science Center of Tsukuba Advanced Research Alliance University of Tsukuba Tsukuba Ibaraki 305-8577 Japan Department of Physical and Macromolecular Chemistry Charles University in Prague 12843 Prague 2 Czech Republic

Although the major isomers of M@C 82 (namely M@ C 2 v (9)‐C 82 , where M is a trivalent rare‐earth metal) have been intensively investigated, the lability of the minor isomers has meant that they have been little studied. Herein, the first isolation and crystallographic characterization of the minor Y@C 82 isomer, unambiguously assigned as Y@ C s (6)‐C 82 by cocrystallization with Ni(octaethylporphyrin), is reported. Unexpectedly, a regioselective dimerization is observed in the crystalline state of Y@ C s (6)‐C 82 . In sharp contrast, no dimerization occurs for the major isomer Y@ C 2 v (9)‐C 82 under the same conditions, indicating a cage‐symmetry‐induced dimerization process. Further experimental and theoretical results disclose that the regioselective dimer formation is a consequence of the localization of high spin density on a special cage‐carbon atom of Y@ C s (6)‐C 82 which is caused by the steady displacement of the Y atom inside the C s (6)‐C 82 cage.

关键词： Dichtefunktionalrechnungen Dimerisierungen Metallofullerene Strukturaufklärung Yttrium

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CdTe [email protected] composite-based recyclable ratiometric fluorescent sensor for rapid and sensitive detection of chlortetracycline

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Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 2022年 270卷

作者： Weikang Yang Xinyu Zheng Feng Gao Huihui Li Bo Fu Dong-Yu Guo Fuxiang Wang Qinhe Pan Key Laboratory of Advanced Materials of Tropical Island Resources of Ministry of Education School of Science Hainan University Haikou 570228 PR China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 PR China Department of Clinical Laboratory Xiamen Huli Guoyu Clinic Co. Ltd. Xiamen 361000 PR China School of Chemical Engineering and Technology Hainan University Haikou 570228 PR China

The residue problem in animal food products caused by the abuse of chlortetracycline (CTC) is one of the food safety issues that have attracted much attention. Herein, a composite was generated by embedding CdTe quantum dots (QDs) into ZIF-8 for ratiometric fluorescent analysis of CTC. With adding CTC, the green luminescence of CTC appeared under the sensitization effect of Zn 2+ in ZIF-8, but the red luminescence of CdTe QDs was reduced by the inner filtration effect of CTC. On this basis, CTC was detected by the composite with a short response time of 1 min, and the limit of detection was calculated to be 37 nM that was 17 times lower than the maximum residue limit of CTC in animal food products (626 nM). Excellent recyclability of the composite was also observed, and CTC was consecutively measured at least six times. The composite was used to determine CTC in basa fish and pure milk with satisfactory recoveries (91.0–110.0%). Portable test strips were further manufactured and the visual determination of CTC was obtained. These results convictively demonstrate that CdTe [email protected] composite as a recyclable ratiometric fluorescent sensor achieves the rapid and sensitive measurement of CTC residue in animal food products.

关键词： Chlortetracycline Ratiometric fluorescence ZIF-8 CdTe quantum dots

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Macromol. Chem. Phys. 11/2018

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Macromolecular Chemistry and Physics 2018年第11期219卷

作者： Shijing Yan Zhenxin Zhong Xiang‐Dan Li Pushan Wen Haining Zhang Lizhong Li Rui He Aiqing Zhang Myong‐Hoon Lee Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission and Ministry of Education South‐Central University for Nationalities Wuhan Hubei 430074 P. R. China Guangdong Key Laboratory of Industrial Surfactant Guangdong Research Institute of Petrochemical and Fine Chemical Engineering Guangzhou 510665 P. R. China FEI Company 5350 NE Dawson Creek Drive Hillsboro OR 97124 USA Department of Chemistry and Chemical Engineering Zunyi Normal College Zunyi Guizhou 563006 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Graduate School of Flexible and Printable Electronics Center for Polymer Fusion Technology Chonbuk National University Jeonju Chonbuk 561756 South Korea

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