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Single-atom catalysis for organic reactions

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Chinese Chemical Letters 2023年第6期34卷 121-129页

作者： Hanyu Hu Jiangbo Xi Key Laboratory of Novel Biomass-Based Environmental and Energy Materials in Petroleum and Chemical Industry Key Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemistry and Environmental EngineeringWuhan Institute of TechnologyWuhan 430205China

Metal-based catalysis,including homogeneous and heterogeneous catalysis,plays a significant role in the modern chemical *** catalysis is widely used due to the high efficiency,easy catalyst separation and ***,the metal-utilization efficiency for conventional heterogeneous catalysts needs further improvement compared to homogeneous *** tackle this,the pursing of heterogenizing homogeneous catalysts has always been attractive but *** a recently emerging class of catalytic material,single-atom catalysts(SACs)are expected to bridge homogeneous and heterogeneous catalytic process in organic reactions and have arguably become the most active new frontier in catalysis *** this review,a brief introduction and development history of single-atom catalysis and SACs involved organic reactions are *** addition,recent advances in SACs and their practical applications in organic reactions such as oxidation,reduction,addition,coupling reaction,and other organic reactions are thoroughly *** understand structure-property relationships of single-atom catalysis in organic reactions,active sites or coordination structure,metal atom-utilization efficiency(e.g.,turnover frequency,TOF calculated based on active metal)and catalytic performance(e.g.,conversion and selectivity)of SACs are comprehensively ***,the application limitations,development trends,future challenges and perspective of SAC for organic reaction are discussed.

关键词： Single-atom catalysis Active site Metal utilization Organic reaction catalytic performance

Collaborative integration of Fe-N_(x)active center into defective sulfur/selenium-doped carbon for efficient oxygen electrocatalysts in liquid and flexible Zn-air batteries

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Chinese Chemical Letters 2024年第9期35卷 421-425页

作者： Yufeng Wu Mingjun Jing Juan Li Wenhui Deng Mingguang Yi Zhanpeng Chen Meixia Yang Jinyang Wu Xinkai Xu Yanson Bai Xiaoqing Zou Tianjing Wu Xianyou Wang National Base for International Science&Technology Cooperation National Local Joint Engineering Laboratory for Key Materials of New Energy Storage BatteryKey Laboratory of Environmentally Friendly Chemistry and Application of Ministry of EducationXiangtan UniversityXiangtan 411105China

Strategic active site organization is imperative for the advancement of effective and long-lasting catalysts of oxygen reduction ***,the controllable multi-active site design is a highly intricate topic for catalyst *** pre-trapping and post-activation strategy,Fe-N bonding structure and S,Se functionalized heteroatom are integrated into a conductive porous *** this process,the nitrogen-abundant polymer 1,3,5-triformylbenzene-tris(4-aminophenyl)benzene(Tf-TAPA)adsorbs Fe^(3+)under the intrinsically metal anchoring ability of N atoms and simultaneously in-situ assembles longchain ***,the Fe^(3+)is transformed into Fe-N_(x)moieties with the conversion of the organic chain to incompletely graphitized ***,the alteration of the electronic configuration achieved through the introduction of dual-atom S and Se leads to a pronounced enhancement in catalytic *** from the Fe-N_(x)bonding structure,dense structural defects,and conductive carbon networks,the resultant Fe-S,Se/NCNs possesses a positive half-wave potential of 0.86 V and a 90%current retention rate,outstripping the Pt/C ***,the liquid and flexible ZAB driven by Fe-S,Se/NCNs achieves large power densities of 259.7 and 164.7 m W/cm^(2),*** study provides a new comprehension in developing an efficient and stable M-N-C oxygen electrocatalyst.

关键词： Atomic regulation Chalcogens co-doped catalytic performance Noble metal-free electrocatalyst Zn-air battery

Synthesis of PbS-K2La2Ti3O10 composite and its photocatalytic activity for hydrogen production

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Progress in Natural Science:Materials International 2012年第2期22卷 120-125页

作者： Dipak Rana Department of Chemical and Biological Engineering University of OttawaOttawaCanada K1N 6N5

Photocatalyst,lead sulfide(PbS)-intercalated layer perovskite-type compound(K2La2Ti3O10),was synthesized via ion-exchange reaction,butylamine pillaring and sulfuration processes under the assistance of the microwave *** structure of the photocatalysts was determined by means of powder X-ray diffraction,scanning electron microscope,ultraviolet-visible diffuse reflection spectra and photoluminescence *** the photocatalytic activity of the composite compound for hydrogen production was also *** experimental results showed that the intercalation of PbS in the layered space of K2La2Ti3O10 greatly improved the absorption edge and the photocatalytic *** production of the PbS-K2La2Ti3O10 was 127.19 mmol/(g cat)after 3 h irradiation of ultraviolet light.

关键词： K2La2Ti3O10 Microwave irradiation PbS Intercalation Hydrogen production catalytic performance

Synthesis of IM-5 Zeolite by Template Pre-Reaction

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China Petroleum Processing & Petrochemical Technology 2021年第2期23卷 77-83页

作者： Sun Min State Key Laboratory of catalytic Materials and Reaction Engineering Research Institute of Petroleum ProcessingSINOPECBeijing 100083

IM-5 zeolite was synthesized by hydrothermal crystallization method with 1,5-bis(N-methylpyrrolidinium)pentane bromide using the precursors N-methylpyrrolidine and 1,5-dibromopentane as raw materials of template after pre-reaction,and then aluminum,alkali,water and silicon sources were added into the reaction *** effects of the proportion of precursors and other materials and the reaction conditions on the crystallinity,crystal morphology and pore structure of the synthesized zeolites were systematically investigated,which provided the basic data for industrial *** physical properties of the synthesized samples were analyzed by XRD,SEM,and N2 adsorptiondesorption techniques,and the catalytic performance of the samples was *** results show that IM-5 zeolite can be synthesized effectively by using the template pre-reaction method,and its physical properties and catalytic activity in catalytic alkylation of benzene and methanol are comparable to those of industrial samples synthesized by traditional method.

关键词： IM-5 zeolite template pre-reaction catalytic performance

Recent Advances of Metal-Organic Frameworks-based Nanozymes for Bio-applications

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Chemical Research in Chinese Universities 2022年第6期38卷 1324-1343页

作者： WANG Yuda ZULPYA Mahmut ZHANG Xinyao XU Shihan SUN Jiao DONG Biao Department of Cell Biology Norman Bethune College of Medicine Jilin UniversityChangchun 130021P.R.China State Key Laboratory on Integrated Optoelectronics College of Electronic Science and EngineeringJilin UniversityChangchun 130012P.R.China Department of Bioengineering University of WashingtonSeattleWAUnited States

Artificial nanoenzymes with enzyme-like catalytic activity have gradually become an alternative to natural enzymes due to their low production cost,high stability,and good *** recent years,various enzyme mimics have emerged with the rapid development of ***-organic frameworks(MOFs)are a novel class of porous inorganic-organic hybrid materials made from metal ions/clusters and organic ligands,and MOFs-based nanozymes show great prospect in biosensing,biocatalysis,biomedical imaging,and therapeutic applications,due to unique properties,such as high specific surface area,high porosity,tunable morphology,and excellent biocatalytic *** this paper,the recent progresses concerning MOFs-based nanozymes are systematically summarized,including the synthesis,design strategies and related applications,which are divided into two major categories,namely,MOFs structured nanoenzymes and MOFs composite structured ***,the applications of various classifications of MOFs research are *** the end,current challenges and future perspectives of MOFs-based nanozymes are also *** is highly expected that this review on this important area can provide a meaningful guidance for tumor therapy,biosensing and other aspects.

关键词： Metal-organic framework Biocatalytic Nanoenzyme catalytic performance Biosensing

A fundamental comprehension and recent progress in advanced Pt‐based ORR nanocatalysts

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SmartMat 2021年第1期2卷 56-75页

作者： Yao Wang Dingsheng Wang Yadong Li Department of Chemistry Tsinghua UniversityBeijingChina

Today,Pt/C catalysts are widely used in proton exchange membrane fuel cells(PEMFCs).The practical applications of PEMFCs still face many limitations in the preparation of advanced Pt‐based catalysts,including high cost,limited life‐time,and insufficient power density.A kinetically sluggish oxygen reduction reaction(ORR)is primarily responsible for these *** development of advanced Pt‐based catalysts is crucial for solving these pro-blems when the large‐scale application of PEMFCs is to be ***,we demonstrate the design principle of advanced Pt‐based catalysts with an emphasis on theoretical understandings to practical ***,three main strategies(including strain effect,electronic effect,and ensemble effect)that governing the initial activity of Pt‐based electrocatalysts are ela-borated in detail in this *** advanced Pt‐based ORR catalysts are summarized and we present representative achievements to further reveal the relationship of excellent ORR performance based on theoretical *** we focus on the preparation standards of membrane electrode assembles and testing protocols in ***,we predict the remaining challenges and present our perspectives with regards to design strategies for improving ORR performance of Pt‐based catalysts in the future.

关键词： catalytic performance membrane electrode assembles oxygen reduction reaction proton exchange membrane fuel cells Pt‐based catalysts

Enhanced methanol-to-olefins(MTO) performance over SAPO-34 molecular sieves synthesized using novel sources of silicon and aluminium

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Clean Energy 2022年第3期6卷 528-533页

作者： Lei Guo Aihua Xing Weiping Zhu Fei Li Zhihui Guo National Institute of Clean and Low Carbon Energy Beijing 102211China

As the core technology of methanol-to-olefins(MTO),the development of a high-efficiency and low-cost molecular sieve catalyst has always been the most important ***,SAPO-34 molecular sieves were synthesized by using three different compositions of amorphous aluminium silicate as both Si and Al source under the same *** structure and composition of synthesized SAPO-34s were investigated using X-ray diffraction and X-ray fluorescence,while the morphology and physical properties were characterized using scanning electron microscopy,N2 adsorption-desorption and ammonia temperature-programmed desorption *** to the silica sol as the Si source,the SAPO-34s prepared with amorphous aluminium silicate show the higher solid yields and crystallinity,larger surface area and lower numbers of acid *** the effect of Si,the effect of the Al source on the textural structure and catalytic performance of SAPO-34s in MTO reactions was investigated in *** results confirmed that the SAPO-34s prepared using amorphous aluminium silicate have low Si content and hierarchical structure,which results in a longer catalytic lifetime and higher selectivity for light *** sample S2 exhibited the longest lifetime of 214 min and the highest selectivity for light olefins of 85.37%.This also provides a potential for the approach to obtain a high-efficiency catalyst with enhanced catalytic performance and low cost.

关键词： methanol-to-olefins SAPO-34 amorphous aluminium silicate catalytic performance

Recent progress in metal–organic frameworks(MOFs)for electrocatalysis

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Industrial Chemistry & Materials

Industrial Chemistry & Materials 2023年第1期1卷 9-38页

作者： Cha Li Hao Zhang Ming Liu Fei-Fan Lang Jiandong Pang Xian-He Bu School of Materials Science and Engineering Smart Sensing Interdisciplinary Science CentreNational Institute for Advanced MaterialsTKL of Metal and Molecule-Based Material ChemistryNankai UniversityTianjin 300350P.R.China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192P.R.China State Key Laboratory of Elemento-Organic Chemistry College of ChemistryNankai UniversityTianjin 300071P.R.China

Electrocatalytic technology opens a new path to solve the existing problems in fossil fuel consumption and environmental pollution as well as efficient energy ***–organic frameworks(MOFs),a class of crystalline porous materials with high specific surface area,high porosity and customizable structures,have emerged as promising ***,their inherently low electrical conductivity and stability greatly hinder their further ***,strategies such as synthesizing two-dimensional conductive MOFs,designing unsaturated metal sites,and building MOF nanoarrays have been developed to enhance the conductivity and catalytic reaction transfer rates of MOFs,accompanied by the rational designs of MOFs for improving their *** this review,the applications of MOF-based electrocatalysts in the hydrogen evolution reaction(HER),hydrogen oxidation reaction(HOR),oxygen evolution reaction(OER),oxygen reduction reaction(ORR)and nitrogen reduction reaction(NRR)are presented in detail with the classification of monometallic MOFs,bimetallic MOFs,MOF-based composites and MOFs as *** addition,the relationship between the structure and performance is discussed through DFT calculations used in related ***,future challenges and application prospects of MOFs in electrocatalysis are highlighted.

关键词： Metal-organic frameworks Electrocatalyst catalytic performance Catalysis Energy conversion

Atomically thin transition metal dichalcogenides for the hydrogen evolution reaction

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ChemPhysMater 2022年第2期1卷 102-111页

作者： Jianqi Zhu Rong Yang Guangyu Zhang Laboratory of Micro-Nano Optics School of Physics and Electronic EngineeringSichuan Normal UniversityChengdu 610101China Institute of Physics Chinese Academy of SciencesBeijing 100190China Songshan Lake Materials Laboratory Dongguan 523808China

Hydrogen is a sustainable and environmentally friendly fuel produced by electrolytic water *** re-quires efficient and easily accessible electrocatalysts to minimize energy ***,as a substitute to the conventional noble-metal-based catalysts,two-dimensional transition metal dichalcogenides(TMDs)have demonstrated their potential as inexpensive catalysts for the hydrogen evolution reaction(HER).In this review,we offer an overview of recent progresses in the development of layered TMDs for the *** improvements in TMD catalytic activity in terms of nanostructuring,defect and boundary engineering,heteroatom doping,and interaction with the supporting material are *** summarize with a perspective on the challenges for the future development of highly effective TMD catalysts for the HER.

关键词： Transition metal dichalcogenides Hydrogen evolution reaction Electrocatalysts catalytic performance Two-dimensional materials Nanostructures