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Unlocking single-atom catalysts via amorphous substrates

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Nano Research 2024年第5期17卷 3533-3546页

作者： Bohua Sun Mingyuan Xu Xiaoxia Li Baohong Zhang Rui Hao Xiaoyu Fan Binbin Jia Dingshun She School of Engineering and Technology China University of Geosciences(Beijing)Beijing 100083China Zhengzhou Institute China University of Geosciences(Beijing)Zhengzhou 451283China College of Materials and Chemical Engineering Key Laboratory of Inorganic Nonmetallic Crystalline and Energy Conversion MaterialsChina Three Gorges UniversityYichang 443002China School of Chemistry Beihang UniversityBeijing 100191China Chinese Academy of Sciences(CAS)Key Laboratory of Nanosystem and Hierarchy Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China National Engineering Research Center of Nonferrous Metals Materials and Products for New EnergyChina GRINM Group Co.Ltd.Beijing 100088China

Single-atom catalysts(SACs)reveal great potential for application in catalysis due to their fully exposed active sites.In general,single atoms(SAs)and the coordination substrates need to have strong interactions or charge transfer to ensure the atomic dispersion,which requires the selection of a suitable substrate to stabilize the target atoms.Recent studies have demonstrated that amorphous materials with abundant defects and coordinatively unsaturated sites can be used as substrates for more efficient capturing SAs,further enhancing the catalytic performance.In this review,we discuss recent research progress of SAs loaded on amorphous substrates for enhanced catalytic activity.Firstly,we summarize the commonly used amorphous substrates for stabilizing SAs.Subsequently,we present several advanced applications of amorphous SACs in the field of catalysis,including electrocatalysis and photocatalysis.And then,we also clarify the synergistic mechanism between SAs and amorphous substrate on catalytic process.Finally,we summarize the challenges with our personal views and provide a critical outlook on how amorphous SACs continue to evolve.

关键词： single-atoms amorphous substrate synthetic strategy catalysis

Advances in the construction of diverse SuFEx linkers

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National Science Review 2023年第6期10卷 226-244页

作者： Daming Zeng Wei-Ping Deng Xuefeng Jiang Shanghai Frontiers Science Center of Optogenetic Techniques for Cell Metabolism School of Pharmacy East China University of Science and Technology Shanghai Key Laboratory of Green Chemistry and Chemical Process School of Chemistry and Molecular Engineering East China Normal University

Sulfur fluoride exchange(SuFEx),a new generation of click chemistry,was first presented by Sharpless,Dong and co-workers in 2014.Owing to the high stability and yet efficient reactivity of the SⅥ-F bond,SuFEx has found widespread applications in organic synthesis,materials science,chemical biology and drug discovery.A diverse collection of SuFEx linkers has emerged,involving gaseous SO2F2and SOF4hubs;SOF4-derived iminosulfur oxydifluorides;O-,N-and C-attached sulfonyl fluorides and sulfonimidoyl fluorides;and novel sulfondiimidoyl fluorides.This review summarizes the progress of these SuFEx connectors,with an emphasis on analysing the advantages and disadvantages of synthetic strategies of these connectors based on the SuFEx concept,and it is expected to be beneficial to researchers to rapidly and correctly understand this field,thus inspiring further development in SuFEx chemistry.

关键词： SuFEx SuFEx linker SVI–F bond synthetic strategy

Advances on Axial Coordination Design of Single‑Atom Catalysts for Energy Electrocatalysis:A Review

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纳微快报:英文版 2023年第12期15卷 188-230页

作者： Linjie Zhang Na Jin Yibing Yang Xiao‑Yong Miao Hua Wang Jun Luo Lili Han State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117People’s Republic of China State Key Laboratory of ASIC and System Shanghai Institute of Intelligent Electronics and SystemsSchool of MicroelectronicsFudan UniversityShanghai 200433People’s Republic of China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110People’s Republic of China

Single-atom catalysts(SACs)have garnered increasingly growing attention in renewable energy scenarios,especially in electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability.The intensive efforts towards the rational design and synthesis of SACs with versatile local configurations have significantly accelerated the development of efficient and sustainable electrocatalysts for a wide range of electrochemical applications.As an emergent coordination avenue,intentionally breaking the planar symmetry of SACs by adding ligands in the axial direction of metal single atoms offers a novel approach for the tuning of both geometric and electronic structures,thereby enhancing electrocatalytic performance at active sites.In this review,we briefly outline the burgeoning research topic of axially coordinated SACs and provide a comprehensive summary of the recent advances in their synthetic strategies and electrocatalytic applications.Besides,the challenges and outlooks in this research field have also been emphasized.The present review provides an in-depth and comprehensive understanding of the axial coordination design of SACs,which could bring new perspectives and solutions for fine regulation of the electronic structures of SACs catering to high-performing energy electrocatalysis.

关键词： Single-atom catalyst Axial coordination synthetic strategy Electrocatalytic application

The synthetic strategy and Magnetic Properties of Novel Heterometallic Metal-azido Complex

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The Synthetic Strategy and Magnetic Properties of Novel Hete...

Rational design and synthesis of cerium dioxide-based nanocomposites

第六届全国物理无机化学会议

作者： Cui Zhao~1,Yongkun Jiao~1,Fuchen Liu~(1,*) 1 School of Chemistry and Chemical Engineering,Tianjin University of Technology,Tianjin,300384

＜正＞The synthesis of heterometallic complexes is of current focus,which is justified not only by the fascinating structural diversity of such complexes but also by their potential applications as functional materials in magnetism, molecular adsorption,light conversion devices,and bimetallic catalysis.Metal-azido complexes have attracted

关键词： Metal-azido Heterometallic synthetic strategy Hydrothermal reaction Magnetic Properties

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Nano Research 2023年第3期16卷 3622-3640页

作者： Haiyan An Liangliang Liu Nan Song Hongmei Zhu Yu Tang State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China School of Pharmacy Lanzhou UniversityLanzhou 730000China

Cerium dioxide(CeO_(2))-based nanocomposites,as a branch of nanocomposites,are always constructed from CeO_(2)combining with other constituents,which exhibit enhanced performance and excellent stability due to their inherent synergistic systems.The modulation of morphology,size,and types of doping of active metals can be achieved by designing the structures,which providing the opportunity to construct diverse CeO_(2)-based nanocomposites.The optimization of the structure enables the design of new multifunctional CeO_(2)-based nanocomposites for various applications such as the field of catalysis.In this minireview,we describe the recent development of the nanocomposites based on noble metal-,transition metal-,and metal-organic framework(MOF)-CeO_(2),which are synthesized through various scientific and rational methods.Meanwhile,the design,synthesis,and basic working principles for CeO_(2)-based nanocomposites are also elucidated.In addition,some examples of their catalytic applications such as electrocatalysis,photocatalysis,and thermocatalysis are also discussed.Finally,the structure-activity relationship in guiding the design and synthesis of CeO_(2)-based nanocomposites is summarized and prospected.

关键词： CeO_(2) nanocomposites synthetic strategy catalysis

Recent advances in metal-free CDs/g-C_(3)N_(4) photocatalysts:synthetic strategies,mechanism insight,and applications

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Journal of Materials Science & Technology 2023年第19期150卷 11-26页

作者： Xingxing Yang Lina Sheng Yongli Ye Jiadi Sun Zaijun Li Xiao Ning Jin Cao Xiulan Sun State Key Laboratory of Food Science and Technology School of Food Science and TechnologyCollaborative Innovation Center of Food Safety and Quality ControlJiangnan UniversityWuxi 214122China Yixing Institute of Food and Biotechnology Co. LtdYixing 214200China School of Chemical and Material Engineering Jiangnan UniversityWuxi 214122China National Institutes for Food and Drug Control Beijing 100050China

Carbon dots/graphite carbon nitride(CDs/g-C_(3)N_(4)),a novel composite photocatalyst,has shown great po-tential for applications in energy regeneration and environmental remediation owing to its following advantages:metal-free,low cost,easily tunable,and excellent photocatalytic performance.Hence,we reviewed the development of synthetic strategies,photocatalytic enhancement mechanisms,and pho-tocatalytic applications of CDs/g-C_(3)N_(4) in this study.First,the three composite strategies of CDs and g-C_(3)N_(4)-self-assembly,solvothermal,and calcination polymerization are outlined,and their advantages and disadvantages are described in detail.Moreover,the photocatalytic enhancement mechanism of the com-posite strategies was elucidated according to the variation trends of CDs/g-C_(3)N_(4) band structure,electronic properties,light absorption range,and interfacial charge transfer.Then,the applications of CDs/g-C_(3)N_(4) in hydrogen evolution,pollutant degradation,CO_(2) reduction,and bacterial disinfection in recent years are reviewed systematically.Finally,the current obstacles and future research directions of CDs/g-C_(3)N_(4) are discussed from the perspective of preparation technology and practical applications,respectively.

关键词： Photocatalysis Graphite carbon nitride Carbon dots synthetic strategy Photocatalytic application

TiO_(2)-supported Single-atom Catalysts:Synthesis,Structure,and Application

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Chemical Research in Chinese Universities 2022年第5期38卷 1123-1138页

作者： LIU Zailun SUN Like ZHANG Qitao TENG Zhenyuan SUN Hongli SU Chenliang International Collaboration Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060P.R.China Department of Applied Chemistry Faculty of EngineeringKyushu Institute of TechnologyKitakyushu 804-8550Japan

In recent years,single-atom catalysts(SACs)have attracted increasing attention in catalysis.However,their stability is considerably challenging.As a result,fine-tuning the interaction of metal single atoms(SA)with different types of supports has emerged as an effective strategy for improving their thermal and chemical stabilities.Owing to its non-toxicity,cost-effectiveness,high abundance,and excellent stability,as well as presence of rich,tunable,and reliable anchor sites for metal SA,TiO_(2)has been extensively explored as a superior support for SACs.In this review,recent advances of TiO_(2)-supported SACs(M1/TiO_(2))are discussed,and synthetic strategies,structure elucidation,and catalytic applications are summarized.First,the recently developed synthetic strategies for M1/TiO_(2)arehighlighted and summarized,identifying the major challenges for the precise fabrication of M1/TiO_(2).Subsequently,key characterization techniques for the structure identification of M1/TiO_(2)are discussed.Next,catalytic applications of M1/TiO_(2)are highlighted,viz.photocatalysis,electrocatalysis,and thermocatalysis.In addition,the mechanism via geometric structures and electronic states of metal centers facilitate catalytic reactions is outlined.Finally,opportunities and challenges of M1/TiO_(2)in catalysis are discussed,which may inspire the future development of M1/TiO_(2)for multifunctional catalytic applications.

关键词： Single-atom catalyst TiO_(2)support synthetic strategy Characterization Catalytic application

Advance in 3D self-supported amorphous nanomaterials for energy storage and conversion

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Nano Research 2023年第7期16卷 10597-10616页

作者： Baohong Zhang Yanhong Li Haoze Bai Binbin Jia Di Liu Lidong Li School of Chemistry Beihang UniversityBeijing 100191China Department of Chemistry Tsinghua UniversityBeijing 100084China

The advancement of next-generation energy technologies calls for rationally designed and fabricated electrode materials that have desirable structures and satisfactory performance.Three-dimensional(3D)self-supported amorphous nanomaterials have attracted great enthusiasm as the cornerstone for building high-performance nanodevices.In particular,tremendous efforts have been devoted to the design,fabrication,and evaluation of self-supported amorphous nanomaterials as electrodes for energy storage and conversion devices in the past decade.However,the electrochemical performance of devices assembled with 3D self-supported amorphous nanomaterials still remains to be dramatically promoted to satisfy the demands for more practical applications.In this review,we aim to outline the achievements made in recent years in the development of 3D self-supported amorphous nanomaterials for a broad range of energy storage and conversion processes.We firstly summarize different synthetic strategies employed to synthesize 3D nanomaterials and to tailor their composition,morphology,and structure.Then,the performance of these 3D self-supported amorphous nanomaterials in their corresponding energy-related reactions is highlighted.Finally,we draw out our comprehensive understanding towards both challenges and prospects of this promising field,where valuable guidance and inspiration will surely facilitate further development of 3D self-supported amorphous nanomaterials,thus enabling more highly efficient energy storage and conversion devices that play a key role in embracing a sustainable energy future.

关键词： three-dimensional(3D)self-supported amorphous nanomaterials synthetic strategy energy storage energy conversion

Photodetectors based on two-dimensional MoS_(2) and its assembled heterostructures

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Chip 2022年第3期1卷 8-27页

作者： Tao Hu Rui Zhang Jin-Ping Li Jian-Yun Cao Feng Qiu National Center for International Research on Photoelectric and Energy Materials Yunnan Key Laboratory for Micro/Nano Materials&TechnologySchool of Materials and EnergyYunnan UniversityKunming 650500China

Photodetectors are finding various potential applications in sensing and detection,information communication,light-emitting diode,optical modulators,ultrafast laser,etc.Molybdenum disulfide(MoS_(2))has sparked great interest given its unique crystal phase,flexible preparation,structural stability,and regulable photoelectronic features.Therefore,the MoS_(2)-based photodetector is demonstrated to be an excellent device fabrication platform to explore underlying sen-sitive detection,broadband optical detection,high-speed response,low-power consumption,two-dimensional integrated circuit,and its synergetic mechanism,which is also proved to be an excellent candidate for next-generation optoelectronics.This review summarizes the structural,optical,and transport features of MoS_(2).Then the working mechanisms and figures of merit are explored for the MoS_(2)detector.Further,the detector modulation strategies are introduced in detail about layer-number engineering and chemical doping engineering.Afterward,the recent heterostructure assembling strategies(MoS_(2)/nD,n=0,1,2,3)of detector architectures are classified based on flexible van der Waals assembling.Finally,the future direction of MoS_(2)photodetectors is discussed,which can be delivered as a feasible guideline in two-dimensional photodetector and integrated circuit fields.

关键词： MoS_(2) synthetic strategy Figures of merit Heterostructure photodetector