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atomically dispersed catalysts:Precise Synthesis,Structural Regulation,and Structure-Activity Relationship

CCS Chemistry 2024年第4期6卷 833-855页

作者： Yun Gao Dingsheng Wang Engineering Research Center of Advanced Rare Earth Materials Department of ChemistryTsinghua UniversityBeijing 100084

atomically dispersed catalysts(ADCs)have been diffusely researched for the development of advanced catalytic processes owing to their welldefined structure,high atomic utilization,and outstanding *** decoding the intrinsic structures and coordination microenvironments of ADCs still confronts significant *** these challenges is important for profound understanding of the structure-activity relationships and directing the future design of ***,this minireview summarizes recent progress and advanced characterization techniques for the engineering of ADCs,including single-atom catalysts,dualatom catalysts,and atomic cluster catalysts with regard to precise synthesis,structural regulation,and the structure-performance *** catalytic merits and regulation strategies of recent breakthroughs in energy conversion,enzyme mimicry,and organic synthesis are thoroughly discussed to disclose the catalytic mechanism-guided ADCs ***,a comprehensive summary of the future challenges and potential prospects is presented to stimulate more design and application possibilities for *** believe that this comprehensive minireview will open up novel pathways for the widespread utilization of ADCs in diverse catalytic processes.

关键词： atomically dispersed catalysts precise synthesis structural regulation structure-activity relationship and catalytic application

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Enhancing sintering resistance of atomically dispersed catalysts in reducing environments with organic monolayers

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Green Energy & Environment 2022年第6期7卷 1263-1269页

作者： Jing Zhang Chithra Asokan Gregory Zakem Phillip Christopher J.Will Medlin Department of Chemical and Biological Engineering University of ColoradoBoulderCOUSA Department of Chemical Engineering University of CaliforniaSanta BarbaraSanta BarbaraCAUSA

atomically dispersed precious metal catalysts maximize atom efficiency and exhibit unique ***,they are susceptible to *** reactions occurring in reducing environments tend to result in atomically dispersed metals sintering at lower temperatures than in oxidative or inert atmospheres due to the formation of mobile metal-H or metal-CO ***,we develop a new approach to mitigate sintering of oxide supported atomically dispersed metals in a reducing atmosphere using organophosphonate self-assembled monolayers(SAMs).We demonstrate this for the case of atomically dispersed Rh on Al_(2)O_(3) and TiO_(2) using a combination of CO probe molecule FTIR,temperature programmed desorption,and alkene hydrogenation rate *** suggests that SAM functionalization of the oxide provides physical diffusion barriers for the metal and weakens the interactions between the reducing gas and metal,thereby discouraging the adsorbate-promoted diffusion of metal atoms on oxide *** results show that support functionalization by organic species can provide improved resistance to sintering of atomically dispersed metals with maintained catalytic reactivity.

关键词： atomically dispersed catalysts Organic monolayers Rh Single atom catalysis Sintering

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Strong synergy between physical and chemical properties:Insight into optimization of atomically dispersed oxygen reduction catalysts

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Journal of Energy Chemistry 2024年第4期91卷 36-49页

作者： Yifan Zhang Linsheng Liu Yuxuan Li Xueqin Mu Shichun Mu Suli Liu Zhihui Dai School of Chemistry and Molecular Engineering Nanjing Tech UniversityNanjing 211816JiangsuChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology InstitutionWuhan 430070HubeiChina School of Chemistry and Materials Science Nanjing Normal UniversityNanjing 210023JiangsuChina

atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic ***,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains ***,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom *** the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed ***,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.

关键词： atomically dispersed catalysts Coordination environment Electronic orbitals Inter-site distance effect Oxygen reduction reaction

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The reformation of catalyst:From a trial-and-error synthesis to rational design

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Nano Research 2024年第4期17卷 3261-3301页

作者： Ligang Wang Jiabin Wu Shunwu Wang Huan Liu Yao Wang Dingsheng Wang Department of Chemistry Tsinghua UniversityBeijing 100084China

The appropriate catalysts can accelerate the reaction rate and effectively boost the efficient conversion of various molecules,which is of great importance in the study of chemistry,chemical industry,energy,materials and environmental ***,efficient,environmentally friendly,and easy to operate synthesis methods have been used to prepare various types of *** previous studies have reported the synthesis and characterization of the aforementioned catalysts,more still remain in trial and error methods,without in-depth consideration and improvement of traditional synthesis ***,we comprehensively summarize and compare the preparation methods of the trial-and-error synthesis strategy,structure–activity relationships and density functional theory(DFT)guided catalysts rational design for nanomaterials and atomically dispersed *** also discuss in detail the utilization of the nanomaterials and single atom catalysts for converting small molecules(H_(2)O,O_(2),CO_(2),N_(2),etc.)into value-added products driven by electrocatalysis,photocatalysis,and ***,the challenges and outlooks of mass preparation and production of efficient and green catalysts through conventional trial and error synthesis and DFT theory are featured in accordance with its current development.

关键词： trial-and-error synthesis structure–activity relationships density functional theory(DFT)guidance nanomaterials atomically dispersed catalysts

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