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Regulating the Mechanical and Optical Properties of Polymer-based Nanocomposites by Sub-Nanowires

Angewandte Chemie 2022年第5期135卷

作者： Feng Yuan Dr. Chen Ouyang Minzheng Yang Prof. Wenxiong Shi Dr. Weibin Ren Prof. Yang Shen Prof. Yan Wei Prof. Xuliang Deng Prof. Xun Wang Institute of Medical Technology Peking University Health Science Center Beijing 100191 China Beijing Laboratory of Biomedical Materials Department of Geriatric Dentistry Peking University School and Hospital of Stomatology Beijing 100081 China Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University Beijing 100084 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (supporting) Formal analysis (supporting) State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China Contribution: Software (supporting) Contribution: Formal analysis (supporting) Contribution: Formal analysis (supporting) Supervision (supporting) Contribution: Conceptualization (equal) Formal analysis (lead) Supervision (lead) Contribution: Conceptualization (lead) Supervision (lead) Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Methodology (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Sub-nanowires (SNWs) exhibit great potential applications in nanocomposites owing to their high specific surface area, high flexibility, and similarity to polymer chains in dimension, which are a good entry point to bridge inorganic materials and polymer materials. Herein, we synthesized hydroxyapatite sub-nanowires (HAP SNWs) and engineered hydroxyapatite sub-nanowires/polyimide (HSP) gels and films by simple mixing of HAP SNWs and polyimide (PI). Benefiting from the interactions between HAP SNWs and PI, these nanocomposites were a continuous hybrid network. As the increase of HAP SNWs contents, the viscosity and modulus of HSP gels were greatly improved by one or two orders of magnitude compared with PI gel. HSP films not only maintained high transparency but also gained high haze, as well as exhibited enhanced Young's modulus. Thus, both HSP gels and films developed in this work are promising for various applications in coatings and high-performance films.

关键词： Gels Nanocomposites Nanowires Thin Films

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Unsupervised Learning-Guided Accelerated Discovery of Alkaline Anion Exchange Membranes for Fuel Cells

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Angewandte Chemie 2023年第19期135卷

作者： Dr. Xiuyang Zou Guodong Xu Pengda Fang Dr. Weizheng Li Zhiyu Jin Dr. Siyu Guo Yin Hu Prof. Meisheng Li Ji Pan Prof. Zhe Sun Prof. Feng Yan Jiangsu Engineering Laboratory of Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Negative Carbon Technologies College of Chemistry Suzhou Key Laboratory of Soft Material and New Energy College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Contribution: Data curation (supporting) Contribution: Formal analysis (equal) Contribution: Formal analysis (supporting) Contribution: Validation (equal) Contribution: Methodology (supporting) School of Chemistry and Chemical Engineering Jiangsu Key Laboratory for Chemistry of Low-Dimensional Materials Huaiyin Normal University Huaian 223300 China Contribution: Software (equal) Contribution: Software (supporting) Contribution: Conceptualization (equal) Contribution: Conceptualization (lead)

Without insight into the correlation between the structure and properties, anion exchange membranes (AEMs) for fuel cells are developed usually using the empirical trial and error method or simulation methods. Here, a virtual module compound enumeration screening (V-MCES) approach, which does not require the establishment of expensive training databases and can search the chemical space containing more than 4.2×10 5 candidates was proposed. The accuracy of the V-MCES model was considerably improved when the model was combined with supervised learning for the feature selection of molecular descriptors. Techniques from V-MCES, correlating the molecular structures of the AEMs with the predicted chemical stability, generated a ranking list of potential high stability AEMs. Under the guidance of V-MCES, highly stable AEMs were synthesized. With understanding of AEM structure and performance by machine learning, AEM science may enter a new era of unprecedented levels of architectural design.

关键词： Alkaline Stability Anion Exchange Membranes Degradation Prediction Machine Learning Material Genomics

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Glucose-Responsive Charge-Switchable Lipid Nanoparticles for Insulin Delivery

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Angewandte Chemie 2023年第20期135卷

作者： Yun Liu Yanfang Wang Yuejun Yao Juan Zhang Wei Liu Kangfan Ji Xinwei Wei Yuanwu Wang Prof. Xiangsheng Liu Prof. Shiming Zhang Prof. Jinqiang Wang Prof. Zhen Gu Key Laboratory of Advanced Drug Delivery Systems of Zhejiang Province College of Pharmaceutical Sciences Zhejiang University 310058 Hangzhou China Jinhua Institute of Zhejiang University 321299 Jinhua China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Software (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Data curation (supporting) Investigation (supporting) Visualization (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Writing - review & editing (supporting) Contribution: Investigation (supporting) Zhejiang Cancer Hospital Hangzhou Institute of Medicine (HIM) Chinese Academy of Sciences 310022 Hangzhou China Department of Electrical and Electronic Engineering The University of Hong Kong 999077 Hong Kong SAR China Second Affiliated Hospital Zhejiang University School of Medicine 310009 Hangzhou China Contribution: Conceptualization (lead) Data curation (equal) Formal analysis (equal) Funding acquisition (lead) Investigation (lead) Methodology (equal) Project administration (lead) Resources (lead) Software (lead) Supervision (lead) Validation (supporting) Visualization (supporting) Writing - review & editing (lead) Department of General Surgery Sir Run Run Shaw Hospital School of Medicine Zhejiang University 310009 Hangzhou China Zhejiang Laboratory of Systems & Precision Medicine Zhejiang University Medical Center 310009 Hangzhou China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University 310009 Hangzhou China Contribution: Funding acquisition (lead) Project administration (lead) Resources (lead) Softwar

Lipid nanoparticle-based drug delivery systems have a profound clinical impact on nucleic acid-based therapy and vaccination. Recombinant human insulin, a negatively-charged biomolecule like mRNA, may also be delivered by rationally-designed positively-charged lipid nanoparticles with glucose-sensing elements and be released in a glucose-responsive manner. Herein, we have designed phenylboronic acid-based quaternary amine-type cationic lipids that can self-assemble into spherical lipid nanoparticles in an aqueous solution. Upon mixing insulin and the lipid nanoparticles, a heterostructured insulin complex is formed immediately arising from the electrostatic attraction. In a hyperglycemia-relevant glucose solution, lipid nanoparticles become less positively charged over time, leading to reduced attraction and subsequent insulin release. Compared with native insulin, this lipid nanoparticle-based glucose-responsive insulin shows prolonged blood glucose regulation ability and blood glucose-triggered insulin release in a type 1 diabetic mouse model.

关键词： Diabetes Drug Delivery Glucose-Responsive Insulin Delivery Lipid Nanoparticles

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H2O2-Responsive NIR-II AIE Nanobomb for Carbon Monoxide Boosting Low-Temperature Photothermal Therapy

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Angewandte Chemie 2022年第36期134卷

作者： Gongcheng Ma Zhongke Liu Chunguang Zhu Prof. Huajie Chen Prof. Ryan T. K. Kwok Prof. Pengfei Zhang Ben Zhong Tang Prof. Lintao Cai Prof. Ping Gong Guangdong Key Laboratory of Nanomedicine Shenzhen Engineering Laboratory of Nanomedicine and Nanoformulations CAS-HK Joint Lab for Biomaterials Research Laboratory for Biomedical Optics and Molecular Imaging Shenzhen Key Laboratory for Molecular Imaging CAS Key Lab for Health Informatics Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China University of Chinese Academy of Sciences Beijing 100049 China Contribution: Data curation (lead) Validation (lead) Writing - original draft (lead) Nano Science and Technology Institute University of Science & Technology of China Suzhou 215123 China Contribution: Data curation (equal) Investigation (equal) Key Laboratory of Environmentally Friendly Chemistry and Application of the Ministry of Education College of Chemistry Xiangtan University Xiangtan 411105 China Contribution: Data curation (supporting) Methodology (supporting) Contribution: Project administration (supporting) Resources (supporting) Supervision (supporting) Writing - review & editing (equal) 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 (HKUST) Clear Water Bay Kowloon Hong Kong China Contribution: Funding acquisition (equal) Supervision (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Formal analysis (lead) Methodology (equal) Project administration (lead) Resources (equal) Supervision (equal) Writing - original draft (equal) Writing - review & editing (lead) School of Science and Engineering Shenzhen Institute of Aggregate Science and Technology The Chinese University of Hong Kong Shenzhen Guangdong 518172 China Contribution: Formal analysis (supporting) Funding acquisition (equal) Writing - review & editing (supporting) Contribution: Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - revi

Low-temperature photothermal therapy (PTT), which circumvents the limitations of conventional PTT (e.g., thermotolerance and adverse effects), is an emerging therapeutic strategy which shows great potential for future clinical applications. The expression of heat shock proteins (HSPs) can dramatically impair the therapeutic efficacy of PTT. Thus, inhibition of HSPs repair and reducing the damage of nearby normal cells is crucial for improving the efficiency of low-temperature PTT. Herein, we developed a nanobomb based on the self-assembly of NIRII AIE polymer PBPTV and carbon monoxide (CO) carrier polymer mPEG(CO). This smart nanobomb can be exploded in a tumor microenvironment in which hydrogen peroxide is overexpressed and release CO into cancer cells to significantly inhibit the expression of HSPs and hence improve the antitumor efficiency of the low-temperature PTT.

关键词： Aggregation Induced Emission Gas Therapy Heat Shock Protein NIR-II Photothermal Therapy

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Construction of Catalytic Covalent Organic Frameworks with Redox-Active Sites for the Oxygen Reduction and the Oxygen Evolution Reaction

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Angewandte Chemie 2022年第49期134卷

作者： Minghao Liu Sijia Liu Dr. Cheng-Xing Cui Qiyang Miao Prof. Yue He Prof. Xuewen Li Prof. Qing Xu Prof. Gaofeng Zeng CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute (SARI) Chinese Academy of Sciences (CAS) Shanghai 201210 P. R. China School of Chemical Engineering University of Chinese Academy of Sciences 19A Yuquan Road Beijing 100049 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Writing - original draft (lead) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Data curation (equal) Investigation (equal) Writing - original draft (equal) School of Chemistry and Chemical Engineering Henan Institute of Science and Technology Xinxiang 453003 P. R. China Contribution: Methodology (lead) Software (lead) Writing - original draft (supporting) Contribution: Conceptualization (supporting) Software (supporting) Department of Oral and Maxillofacial-Head and Neck Oncology Shanghai Ninth People's Hospital Shanghai Jiao Tong University Shanghai 200011 P. R. China Contribution: Project administration (equal) Resources (equal) Writing - original draft (equal) Contribution: Data curation (supporting) Investigation (supporting) Methodology (supporting) Contribution: Conceptualization (lead) Project administration (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Conceptualization (equal) Funding acquisition (lead) Project administration (lead) Writing - original draft (equal) Writing - review & editing (lead)

Construction of catalytic covalent organic frameworks (COFs) for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is significant but rarely demonstrated. In this work, we have first constructed bifunctional COFs towards ORR and OER by integrating diarylamine derivatives into the Co-porphyrin based frameworks. Both of the new COFs (CoTAPP-PATA-COF and CoTAPP-BDTA-COF) have good ordered structures, high surface areas, and robust chemical stability. The diarylamine units, as a typical electron donor and redox-active cores, promote intramolecular electron transport along the frameworks and improve the electrochemically active surface areas. Thus, the COFs showed higher catalytic activities than that of the COF without redox-active units. CoTAPP-PATA-COF had a halfwave potential of 0.80 V towards ORR, and delieved an overpotential of 420 mV for OER in 0.1 M KOH. The theoretical calculation revealed introducing diarylamine unites improved the oxygen electrocatalysis.

关键词： Bifunctional Catalysts Covalent Organic Frameworks Oxygen Evolution Reaction Oxygen Reduction Reaction Redox-Active Sites

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Entropy-Mediated Polymer–Cluster Interactions Enable Dramatic Thermal Stiffening Hydrogels for Mechanoadaptive Smart Fabrics

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Angewandte Chemie 2022年第34期134卷

作者： Jia Wu Baohu Wu Prof. Jiaqing Xiong Shengtong Sun Prof. Peiyi Wu State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Chemistry Chemical Engineering and Biotechnology & Center for Advanced Low-dimension Materials Donghua University Shanghai 201620 China Contribution: Data curation (lead) Investigation (lead) Jülich Centre for Neutron Science (JCNS) at Heinz Maier-Leibnitz Zentrum (MLZ) Forschungszentrum Jülich Lichtenbergstr. 1 85748 Garching Germany Contribution: Investigation (supporting) Software (lead) Innovation Center for Textile Science and Technology Donghua University Shanghai 201620 China Contribution: Methodology (equal) Contribution: Conceptualization (equal) Funding acquisition (equal) Supervision (equal) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (equal) Project administration (lead) Supervision (equal) Writing - original draft (supporting) Writing - review & editing (lead)

Thermal stiffening materials that are naturally soft but adaptively self-strengthen upon heat are intriguing for load-bearing and self-protection applications at elevated temperatures. However, to simultaneously achieve high modulus change amplitude and high mechanical strength at the stiffened state remains challenging. Herein, entropy-mediated polymer–mineral cluster interactions are exploited to afford thermal stiffening hydrogels with a record-high storage modulus enhancement of 13 000 times covering a super wide regime from 1.3 kPa to 17 MPa. Such a dramatic thermal stiffening effect is ascribed to the transition from liquid-liquid to solid–liquid phase separations, and at the molecular level, driven by enhanced polymer–cluster interactions. The hydrogel is further processed into sheath–core fibers and smart fabrics, which demonstrate self-strengthening and self-powered sensing properties by co-weaving another liquid metal fiber as both the joule heater and triboelectric layer.

关键词： Adaptive Materials Hydrogels Sensing Smart Fabrics Thermal Stiffening

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Tailored Fluorosurfactants through Controlled/Living Radical Polymerization for Highly Stable Microfluidic Droplet Generation

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Angewandte Chemie 2023年第3期136卷

作者： Xiangke Li Shi-Yang Tang Yang Zhang Jiayuan Zhu Helen Forgham Chun-Xia Zhao Cheng Zhang Thomas P. Davis Ruirui Qiao Australian Institute of Bioengineering and Nanotechnology The University of Queensland Brisbane Queensland 4072 Australia Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) School of Electronics and Computer Science University of Southampton Southampton SO17 1BJ UK School of Engineering Faculty of Science and Engineering Macquarie University Sydney NSW 2109 Australia School of Chemical Engineering and Advanced Materials The University of Adelaide Adelaide SA 5005 Australia Contribution: Formal analysis (equal) Investigation (equal) Supervision (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Funding acquisition (lead) Methodology (lead) Supervision (lead) Writing - original draft (equal) Writing - review & editing (lead)

Droplet-based microfluidics represents a disruptive technology in the field of chemistry and biology through the generation and manipulation of sub-microlitre droplets. To avoid droplet coalescence, fluoropolymer-based surfactants are commonly used to reduce the interfacial tension between two immiscible phases to stabilize droplet interfaces. However, the conventional preparation of fluorosurfactants involves multiple steps of conjugation reactions between fluorinated and hydrophilic segments to form multiple-block copolymers. In addition, synthesis of customized surfactants with tailored properties is challenging due to the complex synthesis process. Here, we report a highly efficient synthetic method that utilizes living radical polymerization (LRP) to produce fluorosurfactants with tailored functionalities. Compared to the commercialized surfactant, our surfactants outperform in thermal cycling for polymerase chain reaction (PCR) testing, and exhibit exceptional biocompatibility for cell and yeast culturing in a double-emulsion system. This breakthrough synthetic approach has the potential to revolutionize the field of droplet-based microfluidics by enabling the development of novel designs that generate droplets with superior stability and functionality for a wide range of applications.

关键词： Droplet Microfluidics Fluorosurfactant Perfluoropolyether Living Radical Polymerization

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Pore “Softening” and Emergence of Breathability Effects of New Keplerate Nano-Containers

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Angewandte Chemie 2023年第20期135卷

作者： Alexander Elliott James McAllister De-Liang Long Yu-Fei Song Haralampos N. Miras School of Chemistry The University of Glasgow Glasgow G12 8QQ UK Contribution: Formal analysis (lead) Investigation (supporting) Validation (lead) Contribution: Resources (supporting) Contribution: Data curation (equal) Formal analysis (equal) Writing - review & editing (equal) State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Centre for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 China Contribution: Conceptualization (supporting) Investigation (supporting) Resources (supporting) Validation (supporting) Writing - review & editing (equal) Contribution: Conceptualization (lead) Formal analysis (equal) Funding acquisition (lead) Investigation (lead) Methodology (equal) Project administration (lead) Supervision (lead) Writing - original draft (equal) Writing - review & editing (lead)

The self-assembly of porous molecular nanocapsules offer unique opportunities to investigate a range of interesting phenomena and applications. However, to design nanocapsules with pre-defined properties, thorough understanding of their structure-property relation is required. Here, we report the self-assembly of two elusive members of the Keplerate family, [Mo 132 Se 60 O 312 (H 2 O) 72 (AcO) 30 ] 42− {Mo 132 Se 60 } 1 and [W 72 Mo 60 Se 60 O 312 (H 2 O) 72 (AcO) 30 ] 42− {W 72 Mo 60 Se 60 } 2 , that have been synthesised using pentagonal and dimeric ([Mo 2 O 2 Se 2 ] 2+ ) building blocks and their structures have been confirmed via single crystal X-ray diffractions. Our comparative study involving the uptake of organic ions and the related ligand exchange of various ligand sizes by the {Mo 132 Se 60 } and previously reported Keplerates {Mo 132 O 60 }, {Mo 132 S 60 } based on the ligand exchange rates, revealed the emergence of increased “breathability” that dominates over the pore size as we transition from the {Mo 132 S 60 } to the “softer” {Mo 132 Se 60 } molecular nano-container.

关键词： Host-Guest Systems Keplerate Polyoxometalates Selenium Self-Assembly

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In Situ Polymerized 1,3-Dioxolane Electrolyte for Integrated Solid-State Lithium Batteries

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Angewandte Chemie 2023年第12期135卷

作者： Ye Qian Mi Wei Deng Chaohui He Prof. Dr. Osman Eksik Yi Ping Zheng De Kun Yao Dr. Xian Bin Liu Yan Hong Yin Ye Sheng Li Prof. Dr. Bao Yu Xia Prof. Dr. Zi Ping Wu Ganzhou Key Laboratory of Advanced Metals and Functional Materials Faculty of Materials Metallurgy and Chemistry Jiangxi University of Science and Technology Ganzhou 341000 China Contribution: Data curation (lead) Contribution: Formal analysis (lead) Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service Failure Wuhan National Laboratory for Optoelectronics School of Chemistry and Chemical Engineering Huazhong University of Science and Technology Wuhan 430074 China Institute of Nanotechnology Gebze Technical University Gebze 41400 Turkey Contribution: Investigation (equal) Contribution: Methodology (lead) Contribution: Supervision (equal) Writing - original draft (lead) Contribution: Resources (lead) Contribution: Conceptualization (lead) Supervision (lead) Visualization (lead) Writing - review & editing (equal) Contribution: Project administration (lead) Supervision (lead) Validation (lead) Writing - original draft (lead)

Solid-state lithium batteries are promising and safe energy storage devices for mobile electronics and electric vehicles. In this work, we report a facile in situ polymerization of 1,3-dioxolane electrolytes to fabricate integrated solid-state lithium batteries. The in situ polymerization and formation of solid-state dioxolane electrolytes on interconnected carbon nanotubes (CNTs) and active materials is the key to realizing a high-performance battery with excellent interfacial contact among CNTs, active materials and electrolytes. Therefore, the electrodes could be tightly integrated into batteries through the CNTs and electrolyte. Electrons/ions enable full access to active materials in the whole electrode. Electrodes with a low resistance of 4.5 Ω □ −1 and high lithium-ion diffusion efficiency of 2.5×10 −11 cm 2 s −1 can significantly improve the electrochemical kinetics. Subsequently, the batteries demonstrated high energy density, amazing charge/discharge rate and long cycle life.

关键词： Interface Lithium Battery Polymerization Solid-State Electrolyte

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Synthesis of Bandgap-tunable Transition Metal Sulfides through Gas-phase Cation Exchange-induced Topological Transformation

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Angewandte Chemie 2023年第18期135卷

作者： Pengfei Da Prof. Yao Zheng Yang Hu Zelong Wu Hongyu Zhao Yicheng Wei Linchuan Guo Jingjing Wang Yanping Wei Prof. Shibo Xi Prof. Chun-Hua Yan Prof. Pinxian Xi State Key Laboratory of Applied Organic Chemistry Frontiers Science Center for Rare Isotopes College of Chemistry and Chemical Engineering Lanzhou University Lanzhou 730000 China Contribution: Data curation (lead) Formal analysis (lead) Writing - original draft (lead) Writing - review & editing (lead) School of Chemical Engineering and Advanced Materials The University of Adelaide Adelaide South Australia 5005 Australia Contribution: Conceptualization (equal) Writing - original draft (supporting) Writing - review & editing (supporting) Contribution: Data curation (equal) Contribution: Investigation (equal) Contribution: Methodology (equal) Contribution: Data curation (supporting) Northwest Institute of Eco-Environment and Resources Chinese Academy of Sciences Lanzhou 730000 China Contribution: Investigation (supporting) College of Science Gansu Agricultural University Lanzhou 730070 China Institute of Chemical and Engineering Sciences A*STAR 1 Pesek Road Jurong Island 627833 Singapore Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and Applications PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry College of Chemistry and Molecular Engineering Peking University Beijing 100871 China Contribution: Conceptualization (supporting) Resources (equal) Writing - review & editing (equal) Contribution: Conceptualization (lead) Project administration (lead) Resources (equal) Supervision (lead) Writing - original draft (equal) Writing - review & editing (equal)

Oriented synthesis of transition metal sulfides (TMSs) with controlled compositions and crystal structures has long been promising for electronic devices and energy applications. Liquid-phase cation exchange (LCE) is a well-studied route by varying the compositions. However, achieving crystal structure selectivity is still a great challenge. Here, we demonstrate gas-phase cation exchange (GCE), which can induce a specific topological transformation (TT), for the synthesis of versatile TMSs with identified cubic or hexagonal crystal structures. The parallel six-sided subunit (PSS), a new descriptor, is defined to describe the substitution of cations and the transition of the anion sublattice. Under this principle, the band gap of targeted TMSs can be tailored. Using the photocatalytic hydrogen evolution as an example, the optimal hydrogen evolution rate of a zinc-cadmium sulfide (ZCS4) is determined to be 11.59 mmol h −1 g −1 , showing a 36.2-fold improvement over CdS.

关键词： Bandgap Engineering Cation Exchange Photocatalytic Hydrogen Evolution Topological Transformation Transition Metal Sulfides

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