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Molecular Design Strategy for Ordered Mesoporous Stoichiometric Metal Oxide

Angewandte Chemie 2019年第44期131卷

作者： Changyao Wang Xiaoyue Wan Linlin Duan Peiyuan Zeng Liangliang Liu Dingyi Guo Yuan Xia Ahmed A. Elzatahry Yongyao Xia Wei Li Dongyuan Zhao Laboratory of Advanced Materials Department of Chemistry Shanghai Key Lab of Molecular Catalysis and Innovative Materials iChEM and State Key Laboratory of Molecular Engineering of Polymers Fudan University Shanghai 200433 China Institute of Advanced Synthesis School of Chemistry and Molecular Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials Nanjing Tech University Nanjing 211816 China Materials Science and Technology Program College of Arts and Sciences Qatar University PO Box 2713 Doha Qatar

A molecular design strategy is used to construct ordered mesoporous Ti 3+ ‐doped Li 4 Ti 5 O 12 nanocrystal frameworks (OM‐Ti 3+ ‐Li 4 Ti 5 O 12 ) by the stoichiometric cationic coordination assembly process. Ti 4+ /Li + ‐citrate chelate is designed as a new molecular precursor, in which the citrate can not only stoichiometrically coordinate Ti 4+ with Li + homogeneously at the atomic scale, but also interact strongly with the PEO segments in the Pluronic F127. These features make the co‐assembly and crystallization process more controllab.e, thus benefiting for the formation of the ordered mesostructures. The resultant OM‐Ti 3+ ‐Li 4 Ti 5 O 12 shows excellent rate (143 mAh g −1 at 30 C) and cycling performances (<0.005 % fading per cycle). This work could open a facile avenue to constructing stoichiometric ordered mesoporous oxides or minerals with highly crystalline frameworks.

关键词： Assemblierung Li4Ti5O12 Lithium-Ionen-Batterien Mesoporöse Materialien

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1T-MoS2 Enriched Hierarchical MoS2/MoO3 Produced by Phase Transformation for the Efficient Hydrogen Evolution Reaction

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Chemistry, an Asian journal 2023年第5期18卷 2023 Jan 25页

作者： Xiao Zhang Yi-Xuan Liu Yi Lu Ge Tian Xiao-Yu Yang Wuhan University of Technology International School of Materials Science and Engineering CHINA. Wuhan University of Technology School of Materials Science and Engineering CHINA. Heinrich-Heine-Universitat Dusseldorf Institut für Anorganische Chemie und Strukturchemie CHINA. Wuhan University of Technology State Key Laboratory of Advanced Technology for Materials Synthesis and Processing CHINA. Wuhan University of Technology 122 Luoshi Road 430070 Wuhan CHINA.

In recent years, transition metal sulfides have been widely studied in the context of their use as electrocatalysts. The electrocatalytic propensity of the classical semiconductor MoS2, which exists in the 1T and 2H phase structures, has attracted extensive attention. Therefore, the synthesis of highly active and stable MoS2-based catalysts has become the goal of many research efforts. We recently developed a method that can be utilized to prepare the MoS2/MoO3 heterojunction in a phase-controlled manner. 1T-MoS2 phase enriched MoS2/MoO3 heterojunction can be generated using a simple hydrothermal and acid treatment sequence and that the heterojunction has a unique three-dimensional structure, large active surface area, and therefore achieve a low overpotential and high catalytic current density, as well as the long-term stability for the hydrogen evolution reaction.

关键词： 1T-MoS2 MoS2/MoO3 hierarchical heterojunction phase transformation hydrogen evolution reaction

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Appending Coronene Diimide with Carbon Nanohoops Allows for Rapid Intersystem Crossing in Neat Film

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Angewandte Chemie 2024年第18期136卷

作者： Jingjing Zhao Jingwen Xu Dr. Huaxi Huang Kangwei Wang Prof. Dr. Di Wu Prof. Dr. Ramesh Jasti Prof. Dr. Jianlong Xia State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center of Smart Materials and Devices Wuhan University of Technology 430070 Wuhan China These authors contributed equally International School of Materials Science and Engineering Wuhan University of Technology 430070 Wuhan China School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology 430070 Wuhan China Department of Chemistry and Biochemistry Materials Science Institute University of Oregon 97403 Eugene Oregon USA

The development of innovative triplet materials plays a significant role in various applications. Although effective tuning of triplet formation by intersystem crossing (ISC) has been well established in solution, the modulation of ISC processes in the solid state remains a challenge due to the presence of other exciton decay channels through intermolecular interactions. The cyclic structure of cycloparaphenylenes (CPPs) offers a unique platform to tune the intermolecular packing, which leads to controllab.e exciton dynamics in the solid state. Herein, by integrating an electron deficient coronene diimide (CDI) unit into the CPP framework, a donor-acceptor type of conjugated macrocycle ( CDI-CPP ) featuring intramolecular charge-transfer (CT) interaction was designed and synthesized. Effective intermolecular CT interaction resulting from a slipped herringbone packing was confirmed by X-ray crystallography. Transient spectroscopy studies showed that CDI-CPP undergoes ISC in both solution and the film state, with triplet generation time constants of 4.5 ns and 238 ps, respectively. The rapid triplet formation through ISC in the film state can be ascribed to the cooperation between intra- and intermolecular charge-transfer interactions. Our results highlight that intermolecular CT interaction has a pronounced effect on the ISC process in the solid state, and shed light on the use of the characteristic structure of CPPs to manipulate intermolecular CT interactions.

关键词： cycloparaphenylenes rylene diimides triplet materials intersystem crossing

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Correction: Ensemble-machine-learning-based correlation analysis of internal and band characteristics of thermoelectric materials

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Journal of materials Chemistry C 2020年第37期8卷 13091-13091页

作者： Lihao Chen Ben Xu Jia Chen Ke Bi Changjiao Li Shengyu Lu Guosheng Hu Yuanhua Lin State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 P. R. China School of Science Beijing University of Posts and Telecommunications P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center for Smart Materials and Device Integration International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 P. R. China Software School Xiamen University Xiamen 361005 P. R. China

Correction for ‘Ensemble-machine-learning-based correlation analysis of internal and band characteristics of thermoelectric materials’ by Lihao Chen et al., J. Mater. Chem. C, 2020, DOI: 10.1039/d0tc02855j.

Correction for ‘Ensemble-machine-learning-based correlation analysis of internal and band characteristics of thermoelectric materials’ by Lihao Chen et al., J. Mater. Chem. C, 2020, DOI: 10.1039/d0tc02855j.

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Photokatalysatoren auf Graphenbasis für die Produktion von Solarbrennstoffen

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Angewandte Chemie 2015年第39期127卷

作者： Quanjun Xiang Bei Cheng Jiaguo Yu College of Resources and Environment Huazhong Agricultural University Wuhan 430070 (China) State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 (China) Department of Physics Faculty of Science King Abdulaziz University Jeddah 21589 (Saudi‐Arabien) http://***/rid/G‐4317‐2010

Aufgrund des zunehmenden Energiebedarfs und wachsender Umweltprobleme erfahren die Produktion von Solarbrennstoffen durch photokatalytische Wasserspaltung und die CO 2 ‐Reduktion mithilfe von Photokatalysatoren beträchtliches Interesse. In den letzten Jahren haben zahlreiche Studien gezeigt, dass die Effizienz der Photokatalysatoren für die Produktion von Solarbrennstoffen deutlich gesteigert werden kann, wenn man Graphen verwendet, das eine besondere konjugierte 2D‐Struktur und spezielle elektronischen Eigenschaften besitzt. Dieser Aufsatz gibt einen Überblick über jüngste Fortschritte bei der Anwendung von Photokatalysatoren auf Graphenbasis für die Produktion von Solarbrennstoffen einschließlich der CO 2 ‐Reduktion zu Kohlenwasserstoffen und der H 2 ‐Erzeugung mittels Wasserspaltung. Die Grundlagen der Wasserspaltung und der CO 2 ‐Reduktion werden kurz dargestellt. Die für die Verbesserung der photokatalytischen Leistung relevanten Funktionen des Graphens werden diskutiert. Mit Blick auf bestehende Herausforderungen und Möglichkeiten auf diesem vielversprechenden Gebiet werden schließlich mögliche Perspektiven erörtert.

关键词： CO2‐Reduktion Graphen Photokatalyse Solarbrennstoffe Wasserstofferzeugung

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Symmetry-Broken Ru Nanoparticles with Parasitic Ru-Co Dual-Single Atoms Overcome the Volmer Step of Alkaline Hydrogen Oxidation

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Angewandte Chemie 2024年第12期136卷

作者： Xueqin Q. Mu Prof. Suli L. Liu Mengyang Y. Zhang Zechao C. Zhuang Ding Chen Yuru R. Liao Hongyu Y. Zhao Prof. Shichun C. Mu Dingsheng S. Wang Prof. Zhihui H. Dai School of Chemistry and Molecular Engineering Nanjing Tech University Nanjing 211816 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 P. R. China Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University Beijing 100084 P. R. China

Efficient dual-single-atom catalysts are crucial for enhancing atomic efficiency and promoting the commercialization of fuel cells, but addressing the sluggish kinetics of hydrogen oxidation reaction (HOR) in alkaline media and the facile dual-single-atom site generation remains formidable challenges. Here, we break the local symmetry of ultra-small ruthenium (Ru) nanoparticles by embedding cobalt (Co) single atoms, which results in the release of Ru single atoms from Ru nanoparticles on reduced graphene oxide (Co 1 Ru 1,n /rGO). In situ operando spectroscopy and theoretical calculations reveal that the oxygen-affine Co atom disrupts the symmetry of ultra-small Ru nanoparticles, resulting in parasitic Ru and Co dual-single-atom within Ru nanoparticles. The interaction between Ru single atoms and nanoparticles forms effective active centers. The parasitism of Co atoms modulates the adsorption of OH intermediates on Ru active sites, accelerating HOR kinetics through faster formation of *H 2 O. As anticipated, Co 1 Ru 1,n /rGO exhibits ultrahigh mass activity (7.68 A mg Ru −1 ) at 50 mV and exchange current density (0.68 mA cm −2 ), which are 6 and 7 times higher than those of Ru/rGO, respectively. Notably, it also displays exceptional durability surpassing that of commercial Pt catalysts. This investigation provides valuable insights into hybrid multi-single-atom and metal nanoparticle catalysis.

关键词： dual-single-atom catalysts hydrogen oxidation reaction symmetry-breaking parasitic Ru nanoparticles

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Long-term Durability of Seawater Electrolysis for Hydrogen: From Catalysts to Systems

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Angewandte Chemie 2024年第47期136卷

作者： Yu Liu Yong Wang Prof. Paolo Fornasiero Prof. Ge Tian Prof. Peter Strasser Prof. Xiao-Yu Yang State Key Laboratory of Silicate Materials for Architectures & State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & School of Chemistry Chemical Engineering and Life Sciences & Foshan Xianhu Laboratory & Laoshan Laboratory & School of Materials Science and Engineering & International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China Department of Chemical and Pharmaceutical Sciences University of Trieste and ICCOM-CNR and INSTM Trieste Research Units 34127 Trieste Italy Technical University Berlin Department of Chemistry 10623 Berlin Germany

Direct electrochemical seawater splitting is a renewable, scalab.e, and potentially economic approach for green hydrogen production in environments where ultra-pure water is not readily availab.e. However, issues related to low durability caused by complex ions in seawater pose great challenges for its industrialization. In this review, a mechanistic analysis of durability issues of electrolytic seawater splitting is discussed. We critically analyze the development of seawater electrolysis and identify the durability challenges at both the anode and cathode. Particular emphasis is given to elucidating rational strategies for designing electrocatalysts/electrodes/interfaces with long lifetimes in realistic seawater including inducing passivating anion layers, preferential OH − adsorption, employing anti-corrosion materials, fabricating protective layers, immobilizing Cl − on the surface of electrocatalysts, tailoring Cl − adsorption sites, inhibition of OH − binding to Mg 2+ and Ca 2+ , inhibition of Mg and Ca hydroxide precipitation adherence, and co-electrosynthesis of nano-sized Mg hydroxides. synthesis methods of electrocatalysts/electrodes and innovations in electrolyzer are also discussed. Furthermore, the prospects for developing seawater splitting technologies for clean hydrogen generation are summarized. We found that researchers have rethought the role of Cl − ions, as well as more attention to cathodic reaction and electrolyzers, which is conducive to accelerate the commercialization of seawater electrolysis.

关键词： direct electrochemical seawater splitting hydrogen production durability electrocatalysts/electrodes/interfaces design electrolyzer innovation

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Integrating triple intracellular metabolic pathways in living yeast cells for dual-functionalized cell beacons

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Nanomedicine: Nanotechnology, Biology and Medicine 2018年第5期14卷 1874-1874页

作者： Ran Cui Ming-Xi Zhang Zhi-Ling Zhang Dai-Wen Pang Key Laboratory of Analytical Chemistry for Biology and Medicine (Ministry of Education) College of Chemistry and Molecular Sciences Research Center for Nanobiology and Nanomedicine (MOE 985 Innovative Platform) State Key Laboratory of Virology and Wuhan Institute of Biotechnology Wuhan University Wuhan 430072 PR China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan P. R. China

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Designing a 0D/2D S‐Scheme Heterojunction over Polymeric Carbon Nitride for Visible‐Light Photocatalytic Inactivation of Bacteria

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Angewandte Chemie 2020年第13期132卷

作者： Pengfei Xia Shaowen Cao Bicheng Zhu Mingjin Liu Miusi Shi Jiaguo Yu Yufeng Zhang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China State Key Laboratory Breeding Base of Basic Science of Stomatology (Hubei-MOST) & Key Laboratory of Oral Biomedicine Ministry of Education School and Hospital of Stomatology Wuhan University Wuhan Hubei 430079 P. R. China

Constructing heterojunctions between two semiconductors with matched band structure is an effective strategy to acquire high‐efficiency photocatalysts. The S‐scheme heterojunction system has shown great potential in facilitating separation and transfer of photogenerated carriers, as well as acquiring strong photoredox ability. Herein, a 0D/2D S‐Scheme heterojunction material involving CeO 2 quantum dots and polymeric carbon nitride (CeO 2 /PCN) is designed and constructed by in situ wet chemistry with subsequent heat treatment. This S‐scheme heterojunction material shows high‐efficiency photocatalytic sterilization rate (88.1 %) towards Staphylococcus aureus (S. aureus) under visible‐light irradiation ( λ ≥420 nm), which is 2.7 and 8.2 times that of pure CeO 2 (32.2 %) and PCN (10.7 %), respectively. Strong evidence of S‐scheme charge transfer path is verified by theoretical calculations, in situ irradiated X‐ray photoelectron spectroscopy, and electron paramagnetic resonance.

关键词： Antibakterielle Materialien Photokatalyse Polymeres Kohlenstoffnitrid S-Schema-Heterokontakte

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Layered Nanosheets: Superhierarchical Inorganic/Organic Nanocomposites Exhibiting Simultaneous Ultrahigh Dielectric Energy Density and High Efficiency (Adv. Funct. Mater. 8/2021)

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advanced Functional materials 2021年第8期31卷

作者： Bingcheng Luo Zhonghui Shen Ziming Cai Enke Tian Yuan Yao Baiwen Li Ahmed Kursumovic Judith L. MacManus-Driscoll Longtu Li Long-Qing Chen Xiaohui Wang State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Center of Smart Materials and Devices Wuhan University of Technology Wuhan 430070 China School of Science China University of Geosciences Beijing 100083 China Institute of Applied Physics and Computational Mathematics Beijing 100094 China Department of Materials Science and Metallurgy University of Cambridge Cambridge CB3 0FS UK Department of Materials Science and Engineering The Pennsylvania State University University Park PA 16802 USA

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