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Revealing the Intrinsic Peroxidase-Like Catalytic Mechanism of Heterogeneous single-atom Co-MoS2

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Nano-Micro Letters 2019年第4期11卷 778-790页

作者： Ying Wang Kun Qi Shansheng Yu Guangri Jia Zhiliang Cheng Lirong Zheng Qiong Wu Qiaoliang Bao Qingqing Wang Jingxiang Zhao Xiaoqiang Cui Weitao Zheng Key Laboratory of Automobile Materials of MOE School of Materials Science and EngineeringJilin University2699 Qianjin StreetChangchun 130012People’s Republic of China Department of Materials Science and Engineering ARC Centre of Excellence in Future Low-Energy Electronics Technologies(FLEET)Monash UniversityClaytonVIC 3800Australia Key Laboratory of Photonic and Electronic Bandgap Materials Ministry of EducationCollege of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025People’s Republic of China Department of Bioengineering University of Pennsylvania210 South 33rd Street240 Skirkanich HallPhiladelphiaPA 19104USA Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100190People’s Republic of China School of Chemistry and Chemical Engineering MOE Key Laboratory of Micro-System and Micro-Structure ManufacturingHarbin Institute of TechnologyHarbin 150001People’s Republic of China

The single-atom nanozyme is a new concept and has tremendous prospects to become a next-generation ***,few studies have been carried out to elucidate the intrinsic mechanisms for both the single atoms and the supports in single-atom ***,the heterogeneous single-atom Co-MoS2(SA Co-MoS2)is demonstrated to have excellent potential as a high-performance peroxidase *** of the well-defined structure of SA Co-MoS2,its peroxidase-like mechanism is extensively interpreted through experimental and theoretical *** to the different adsorption energies of substrates on different parts of SA Co-MoS2 in the peroxidase-like reaction,SA Co favors electron transfer mechanisms,while MoS2 relies on Fenton-like *** different catalytic pathways provide an intrinsic understanding of the remarkable performance of SA *** present study not only develops a new kind of single-atom catalyst(SAC)as an elegant platform for understanding the enzyme-like activities of heterogeneous nanomaterials but also facilitates the novel application of SACs in biocatalysis.

关键词： Biocatalysis Nanozymes Peroxidase mimic Reaction mechanisms single-atom catalysts

Ultrastable single-atom gold catalysts with strong covalent metal-support interaction （CMSI）

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Nano Research 2015年第9期8卷 2913-2924页

作者： Botao Qiao Jin-Xia Liang Aiqin Wang Cong-Qiao Xu Jun Li Tao Zhang Jingyue (Jimmy) Liu Department of Physics Arizona State University Tempe Arizona 85287 USA State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China Department of Chemistry & Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education Tsinghua University Beijing 100084 China Guizhou Provincial Key Laboratory of Computational Nano-Material Science Guizhou Normal College Guiyang 550018 China

Supported noble metal nanoparticles （including nanoclusters） are widely used in many industrial catalytic processes. While the finely dispersed nanostructures are highly active, they are usually thermodynamically unstable and tend to aggregate or sinter at elevated temperatures. This scenario is particularly true for supported nanogold catalysts because the gold nanostructures are easily sintered at high temperatures, under reaction conditions, or even during storage at ambient temperature. Here, we demonstrate that isolated Au single atoms dispersed on iron oxide nanocrystallites （Aul/FeOx） are much more sintering- resistant than Au nanostructures, and exhibit extremely high reaction stability for CO oxidation in a wide temperature range. Theoretical studies revealed that the positively charged and surface-anchored Aul atoms with high valent states formed significant covalent metal-support interactions （CMSIs）, thus providing the ultra-stability and remarkable catalytic performance. This work may provide insights and a new avenue for fabricating supported Au catalysts with ultra-high stability.

关键词： single-atom catalysis,goId catalyst,CO oxidation,covalent metal-supportinteraction

Design of high performance nanozymes: a single-atom strategy

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Science China(Life Sciences) 2019年第5期62卷 710-712页

作者： Shichao Lin Hui Wei Department of Biomedical Engineering College of Engineering and Applied Sciences Nanjing National Laboratory of MicrostructuresJiangsu Key Laboratory of Artificial Functional Materials Nanjing University State Key Laboratory of Analytical Chemistry for Life Science and State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University

Nanozymes, nanomaterials with enzyme-like characteristics,are emerging as novel artificial enzymes (Gao et al., 2007;Manea et al., 2004;Yan, 2018). They are superior to natural enzymes in many ways, such as higher sta... 详细信息

关键词： a single-atom strategy Design of high performance nanozymes NC Zn

Silver based single atom catalyst with heteroatom coordination environment as high performance oxygen reduction reaction catalyst

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Nano Research 2022年第9期15卷 7968-7975页

作者： Rui Sui Xuejiang Zhang Xingdong Wang Xinyu Wang Jiajing Pei Yufeng Zhang Xuerui Liu Wenxing Chen Wei Zhu Zhongbin Zhuang State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical TechnologyBeijing 100029China International Clean Energy Research Office China Three Gorges CorporationBeijing 100038China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory of Energy Environmental Catalysis Beijing University of Chemical TechnologyBeijing 100029China

Ag is a potential low-cost oxygen reduction reaction(ORR)catalyst in alkaline condition,which is important for the zinc-air ***,we report that an Ag based single atom catalyst with heteroatom ***1-h-NPClSC,has been synthesized and shown much improved performance towards ORR by manipulating the coordination environment of the Ag *** shows a high half wave potential(0.896 V)and a high turnover frequency(TOF)(5.9 s^(−1))at 0.85 V,which are higher than the previously reported Ag based catalysts and commercial Pt/C.A zinc-air battery with high peak power density of 270 mW·cm^(−2)is fabricated by using the Ag1-h-NPClSC as air *** high performance is attributed to(1)the hollow structure providing good mass transfer;(2)the single atom metal center structure providing high utility of the Ag;(3)heteroatom coordination environment providing the adjusted binding to the ORR *** functional theory(DFT)calculations show that the energy barrier for the formation of OOH*,which is considered as the rate determine step for ORR on Ag nanoparticles,is lowered on Ag1-h-NPClSC,thus improving the ORR *** work demonstrates that the well manipulated Ag based single atom catalysts are promising in electrocatalysis.

关键词： Ag single-atom heteroatom coordination oxygen reduction zinc-air battery

Design of hierarchical, three-dimensional free-standing single-atom electrode for H2O2 production in acidic media

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Carbon Energy 2020年第2期2卷 276-282页

作者： Jincheng Zhang Hongbin Yang Jiajian Gao Shibo Xi Weizheng Cai Junming Zhang Ping Cui Bin Liu School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingaporeSingapore Institute of Chemical and Engineering Sciences Agency for ScienceTechnology and ResearchSingaporeSingapore

Electrochemical reduction of molecular O2 to hydrogen peroxide(H2O2)offers a promising solution for water purification and environmental ***,we design a hierarchical free-standing single-Co-atom(with Co-N4 coordination)electrode for oxygen reduction reaction(ORR)via a two-electron pathway to make H2O2 in acidic *** current density of the single-Co-atom electrode reached 51 mA/cm2 at 0.1 V vs reversible hydrogen electrode,lasting for more than 10 hours of continuous operation with H2O2 selectivity greater than 80%.Toward practical application,the single-Co-atom electrode was directly used to assemble an electrochemical cell to produce H2O2 at a rate of 676 mol/kgcat/h with a cell voltage of about 1.6 V.

关键词： CoN4 free-standing H2O2 oxygen reduction reaction single-atom

single-atom catalyst of transition metals(Mo,Nb,W,Ta/Co) composite with nitrogen-doped carbon for dye-sensitized solar cells

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Single-atom catalyst of transition metals(Mo,Nb,W,Ta/Co) com...

Nickel-iron in the second coordination shell boost single-atomicsite iridium catalysts for high-performance urea electrooxidation

第五届新型太阳能电池学术研讨会

作者：张婷婷云斯宁西安建筑科技大学材料与矿资学院功能材料研究所

Typical dye-sensitized solar cells(DSSCs) are composed of a fluorine-doped tin oxide(FTO) glass,a dyed coated TiO anode,an electrolyte,and a counter electrode(CE).The CE in DSSC systems played the roles of reducing Iand collecting *** CE material platinum(Pt) electrode is expensive and can be decomposed to PtI or H Pt I by I/Iredox couple in the electrolyte,thus limited its large-scale commercial application in DSSCs due to the critical issues on the cell performance and long-term ***,it is urgent to explore Pt-free CEs to facilitate the industrial development of ***-cost carbon materials and transition metals compound are widely utilized as CEs in *** transition metals with carbon materials(e.g.,nitrogen-doped carbon) is expected to have both the advantage of the two ***-atom dispersed metal and nitrogen bi-modified carbon material(Co-N-C) catalyst is already proved to be a promising candidate for substituting Pt in *** present work is to synthesis single-atom dispersed transition metals(e.g.,Mo,Nb,W,Ta/Co) into nitrogen-doped carbon to instead of costly Pt electrode.

关键词： dye-sensitized solar cells transition metal single-atom counter electrode carbon materials

来源： cnki会议评论

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Nano Research 2024年第5期17卷 3919-3926页

作者： Xiaoyu Chen Jiawei Wan Jing Chai Liang Zhang Fang Zhang Qinghua Zhang Lin Gu Lirong Zheng Ranbo Yu Department of Physical Chemistry School of Metallurgical and Ecological EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Key Laboratory of Biochemical Engineering Key Laboratory of Biopharmaceutical Preparation and DeliveryChinese Academy of SciencesInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center for Combustion Energy School of Vehicle and MobilityState Key Laboratory of Intelligent Green Vehicle and MobilityTsinghua UniversityBeijing 100084China Analysis and Testing Center Beijing Institute of TechnologyBeijing 100081China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials Department of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China

single-atom catalysts(SACs)with high catalytic activity as well as great stability are demonstrating great promotion in electrocatalytic energy conversion,which is also a big challenge to ***,we proposed a facile synthetic strategy to construct nickel-iron bimetallic hydroxide nanoribbon stabilized single-atom iridium catalysts(Ir-NiFe-OH),where the nickel-iron hydroxide nanoribbon not only can serve as good electronic conductor,but also can well stabilize and fully expose single-atom *** as catalyst for urea oxidation reaction(UOR),it exhibited excellent UOR performance that it only needed a low operated potential of 1.38 V to achieve the current density of 100 mA·cm^(-2).In-situ Fourier transform infrared spectroscopy,X-ray absorption spectrum,and density functional theory calculations proved that Ir species are active centers and the existence of both Ni and Fe in the local structure of Ir atom can optimize the d-band center of Ir species,promoting the adsorption of intermediates and desorption of products for *** hydrogen evolution reaction(HER)/UOR electrocatalytic cell demanded voltages of 1.46 and 1.50 V to achieve 50 and 100 mA·cm^(-2),respectively,which demonstrated a higher activity and better stability than those of conventional *** work opens a new avenue to develop catalysts for UORs with boosted activity and stability.

关键词： single-atom iridium coordinate structure nanoribbon urea electrooxidation

single Pt atom decorated graphitic carbon nitride as an efficient photocatalyst for the hydrogenation of nitrobenzene into aniline

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Nano Research 2019年第8期12卷 1817-1823页

作者： Tianwei He Chunmei Zhang Lei Zhang Aijun Du School of Chemistry Physics and Mechanical EngineeringScience and Engineering FacultyQueensland University of TechnologyGardens Point CampusBrisbaneQLD 4001Australia

The hydrogenation of nitrobenzene into aniline is one of industrially important reactions, but still remains great challenge due to the lack of highly active, chemo-selective and eco-friendly catalyst. By using extensive density functional theory (DFT) calculations, herein we predict that single Pt atom decorated g-C3N4 (Pt@g-C3N4) exhibits excellent catalytic activity and selectivity for the conversion of nitrobenzene into aniline under visible light. The overall activation energy barrier for the hydrogenation of nitrobenzene on single atom Pt@g-C3N4 catalyst is even lower than that of the bare Pt(111) surface. The dissociation of N-0 bonds on single Pt atom is triggered by single hydrogen atom rather than double hydrogen atoms on the Pt(111) surface. Moreover, the Pt@g-C3N4 catalyst exhibits outstanding chemoselectivity towards the common reducible substituents, such as phenyl,-C=C,-C = C and -CHO groups during the hydrogenation. In addition, the doped single Pt atom can significantly enhance the photoconversion efficiency by broadening the light absorption of the pristine g-C3N4 to visible light region. Our results highlight an interesting and experimentally synthesized single-atom photocatalyst (Pt@g-C3N4) for efficient hydrogenation of nitrobenzene to aniline under a sustainable and green approach.

关键词： chemoselective hydrogenation single-atom catalyst photocatalyst nitrobenzene

Controlled synthesis of single cobalt atom catalysts via a facile one-pot pyrolysis for efficient oxygen reduction and hydrogen evolution reactions

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Science Bulletin 2019年第15期64卷 1095-1102页

作者： Yao Wang Linhui Chen Zhanxin Mao Lishan Peng Rui Xiang Xianyi Tang Jianghai Deng Zidong Wei Qiang Liao Chongqing Key Laboratory of Chemical Process for Clean Energy and Resource Utilization College of Chemistry and Chemical Engineering.Chongqing UniversityChongqing400044China Institute of New-Energy and Low-Carbon Technology Sichuan UniversityChengdu610065China Key Laboratory of Low-Grade Energy Utilization Technologies and Systems Chongqing UniversityChongqing400044China

Metal-nitrogen doped carbon catalysts(M-N/C) with abundantly accessible M-Nxsites, particularly single metal atom M-N/C(SAM-N/C), have been developed as a substitute for expensive Pt-based *** catalysts are used to increase the efficiency of otherwise sluggish oxygen reduction reactions(ORR) and hydrogen evolution reactions(HER). However, although the agglomerated metal nanoparticles are usually easy to form, they are very difficult to remove due to the protective surface-coating carbon layers, a factor that significantly hampers SAM-N/C fabrication. Herein, we report a one-step pyrolysis approach to successfully fabricate single cobalt atom Co-N/C(SACo-N/C) by using a Co2+-SCN-coordination compound as the metal precursor. Thanks to the decomposition of Co2+-SCN-compound at lower temperature than that of carbon layer deposition, Co-rich particles grow up to larger ones before carbon layers formation. Even though encapsulated by the carbon layers, it is difficult for the large Co-rich particle to be completely sealed. And thus, it makes the Co atoms possible to escape from incomplete carbon layer, to coordinate with nitrogen atoms, and to form SACo-N/C catalysts. This SACo-N/C exhibits excellent performances for both ORR(half-wave potential of 0.878 V) and HER(overpotential at 10 mA/cm2 of178 m V), and is thus a potential replacement for Pt-based catalysts. When SACo-N/C is integrated into a Zn-O2 battery, battery with high open-circuit voltage(1.536 V) has high peak power density(266 mW/cm2)and large gravimetric energy density(755 mA h/gZn) at current densities of 100 mA/cm2. Thus, we believe that this strategy may offer a new direction for the effective generation of SAM-N/C catalysts.

关键词： Carbon nanocomposites single-atom catalysts H2 evolution O2 reduction Zn-O2 battery