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Spatial conﬁnement of zeolitic imidazolate framework deposits by porous carbon nanospheres for dual-atom catalyst towards high-performance oxygen reduction reaction

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Nano Research 2023年第8期16卷 11464-11472页

作者： Jiayi Zhao Ping Li Kaicai Fan Wenjie Wei Fenghong Lu Huimin Zhao Bin Li Lingbo Zong Lei Wang Key Laboratory of Eco-chemical Engineering College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China

dual atom catalysts(DACs),are promising electrocatalysts for oxygen reduction reaction(ORR)on account of the potential dual-atom active sites for the optimized adsorption of catalytic intermediates and the lower reaction energy ***,spatial conﬁnement strategy to fabricate DACs with well-defined Fe,Co dual-atom active site is proposed by implanting zeolitic imidazolate frameworks inside the pores of highly porous carbon nanospheres(Fe/Co-SAs-Nx-PCNSs).The atomically dispersed dual-atom active sites facilitate the adsorption/desorption of ***,the spatial conﬁnement effect protects metal atoms *** from the rich accessible dual-atom active sites and boosted mass transport,we achieve remarkable ORR performance with half-wave potential up to 0.91 and 0.8 V(*** hydrogen electrode(RHE)),and long-term stability up to 10 h in both alkaline and acidic *** remarkably enhanced ORR catalytic property of our as-developed DACs is in the rank of excellence for 1%.The as-developed rechargeable Zn-air battery(ZAB)with Fe/Co-SAs-Nx-PCNSs air cathode delivers ultrahigh power density of 216 mW·cm^(−2),outstanding specific capacity of 813 mAh·g^(−1),and promising cycling operation durability over 160 *** flexible Zn-air battery also exhibits excellent specific capacity,cycling stability,and flexibility *** work opens up a new pathway for the multiscale design of efficient electrocatalysts with atomically dispersed multiple active sites.

关键词： spatial confinement zeolitic imidazolate framework porous carbon nanospheres(PCNSs) dual-atom catalyst oxygen reduction reaction(ORR)

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Predication of Selective Ring-opening Hydrogenolysis for Furfuryl Alcohol to Produce Pentanediol over dual-atom catalysts

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Chemical Research in Chinese Universities 2024年第1期40卷 55-63页

作者： WANG Tingting WANG Jia XI Yongjie HU Bin LI Fuwei State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000P.R.China University of Chinese Academy of Sciences Beijing 100049P.R.China

Selective activation of C-O bond is of fundamental importance in the precise conversion of oxygenates into value-added compounds in an atom-economic and sustainable manner, and meanwhile, the structurally well-defined dual-atoms catalysts (DACs) have been scarcely investigated in this field. In this study, a series of transition metal DACs anchored on nitrogen-doped graphene (TM2/NC, TM=Pt, Ir, Rh, Pd, Ru, Co, Ni and Cu) was constructed to make a comprehensive investigation of their selectivity in the hydrogenative transformation of furfuryl alcohol (FAL), an important biomass platform molecule, to 1,2-pentanediol (1,2-PeD) via selective cleavage of furanic C5-O bond, by density functional theory (DFT) calculations and microkinetic modeling. We found that Ir2/NC demonstrated a high selectivity for the cleavage of furanic C5-O bond to produce 1,2-PeD, while the production of THFAL or 1,5-pentanediol (1,5-PeD) on other TM2/NC catalysts are more favorable. Furthermore, we found that the selective C-O bond cleavage of FAL furan ring is affected by the orbital overlap between the d-orbitals of the anchored metal atoms and the p-orbitals of the adsorbed C atom in FAL, suggesting that the selectivity of the C-O bond cleavage is inextricably related with the electronic property of the anchored metals.

关键词： Furfuryl alcohol Hydrogenation dual-atom catalyst Density functional theory(DFT)calculation

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Oxygen Reduction Reaction Activity of Fe-based dual-atom catalysts with Different Local Configurations via Graph Neural Representation

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Chinese Journal of Chemical Physics 2024年第5期37卷 599-604,I0038-I0040,I0099页

作者： Xueqian Xia Zengying Ma Yucheng Huang College of Chemistry and Material Science Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Key Laboratory of Molecule-Based MaterialsAnhui Carbon Neutrality Engineering CenterAnhui Normal UniversityWuhu 241000China

The performance of proton exchange membrane fuel cells depends heavily on the oxygen reduction reaction(ORR)at the cathode,for which platinum-based catalysts are currently the *** high cost and limited availability of platinum have driven the search for alternative *** FeN4 single-atom catalysts have shown promising potential,their ORR activity needs to be further *** contrast,dual-atom catalysts(DACs)offer not only higher metal loading but also the ability to break the ORR scaling ***,the diverse local structures and tunable coordination environments of DACs create a vast chemical space,making large-scale computational screening *** this study,we developed a graph neural network(GNN)-based framework to predict the ORR activity of Fe-based DACs,effectively addressing the challenges posed by variations in local catalyst *** model,trained on a dataset of 180 catalysts,accurately predicted the Gibbs free energy of ORR intermediates and overpotentials,and identified 32 DACs with superior catalytic activity compared to FeN4 *** approach not only advances the design of high-performance DACs,but also offers a powerful computational tool that can significantly reduce the time and cost of catalyst development,thereby accelerating the commercialization of fuel cell technologies.

关键词： Oxygen reduction reaction dual-atom catalyst Graph neural representation Density functional theory Artificial intelligence

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Transition metal-based single-atom catalysts(TM-SACs);rising materials for electrochemical CO_(2) reduction

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Journal of Energy Chemistry 2022年第7期31卷 444-471,I0012页

作者： Bishnupad Mohanty Suddhasatwa Basu Bikash Kumar Jena Materials Chemistry Department CSIR-Institute of Minerals and Materials TechnologyBhubaneswar 751013India Academy of Scientific&Innovative Research(AcSIR) Ghaziabad 201002India

The continuous increase of global atmospheric CO_(2) concentrations brutally damages our environment. A series of methods have been developed to convert CO_(2) to valuable fuels and value-added chemicals to maintain the equilibrium of carbon cycles. The electrochemical CO_(2) reduction reaction(CO_(2)RR) is one of the promising methods to produce fuels and chemicals, and it could offer sustainable paths to decrease carbon intensity and support renewable energy. Thus, significant research efforts and highly efficient catalysts are essential for converting CO_(2) into other valuable chemicals and fuels. Transition metal-based single atoms catalysts(TM-SACs) have recently received much attention and offer outstanding electrochemical applications with high activity and selectivity opportunities. By taking advantage of both heterogeneous and homogeneous catalysts, TM-SACs are the new rising star for electrochemical conversion of CO_(2) to the value-added product with high selectivity. In recent years, enormous research effort has been made to synthesize different TM-SACs with different M–Nxsites and study the electrochemical conversion of CO_(2) to CO. This review has discussed the development and characterization of different TMSACs with various catalytic sites, fundamental understanding of the electrochemical process in CO_(2) RR,intrinsic catalytic activity, and molecular strategics of SACs responsible for CO_(2)RR. Furthermore, we extensively review previous studies on 1 st-row transition metals TM-SACs(Ni, Co, Fe, Cu, Zn, Sn) and dual-atom catalysts(DACs) utilized for electrochemical CO_(2) conversions and highlight the opportunities and challenges.

关键词： CO_(2)RR Single-atom catalyst SACs dual-atom catalyst DACs Transition metals Support catalysts

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1+1>2: Learning from the interfacial modulation on single-atom electrocatalysts to design dual-atom electrocatalysts for dinitrogen reduction

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Green Energy & Environment 2023年第6期8卷 1753-1763页

作者： Qiang Zhou Feng Gong Yunlong Xie Rui Xiao College of Materials Xiamen UniversityXiamen361005China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing211189JiangsuChina Institute for Advanced Materials Hubei Normal UniversityHuangshi435002China

Developing efficient electrocatalysts for converting dinitrogen to ammonia through electrocatalysis is of significance to the decentralized ammonia production. Here, through high-throughput density functional theory calculations, we demonstrated that the interfacial modulation of hexagonal boron nitride/graphene(hBN-graphene) could sufficiently improve the catalytic activity of the single transition metal atom catalysts for nitrogen reduction reaction(NRR). It was revealed that Re@hBN-graphene and Os@hBN-graphene possessed remarkable NRR catalytic activity with low limiting potentials of 0.29 V and 0.33 V, respectively. Furthermore, the mechanism of the enhanced catalytic activity was investigated based on various descriptors of the adsorption energies of intermediates, where the synergistic effect of hBN and graphene in the hybrid substrate was found to play a key role. Motivated by the synergistic effect of hybrid substrate in single-atom catalysts, a novel strategy was proposed to efficiently design dual-atom catalysts by integrating the merits of both metal components. The as-designed dual-atom catalyst Fe-Mo@hBN exhibited more excellent NRR catalytic performance with a limiting potential of 0.17 V, manifesting the solidity of the design strategy. Our findings open new avenues for the search of heterostructure substrates for single-atom catalysts and the efficient design of dualatom catalysts for NRR.

关键词： Nitrogen reduction reaction Boron nitride Graphene High throughput Descriptor Density functional theory Single-atom catalyst dual-atom catalyst

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Coordination-environment regulation of atomic Co-Mn dual-sites for efficient oxygen reduction reaction

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Nano Research 2024年第8期17卷 6841-6848页

作者： Caiting Sun Yarong Liu Zunhang Lv Rui Liu Changli Wang Liuhua Li Jinming Wang Yu Zhang Wenxiu Yang Bo Wang Key Laboratory of Cluster Science(Ministry of Education) Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsAdvanced Technology Research Institute(Jinan)Advanced Research Institute of Multidisciplinary ScienceSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Institute of Technology Library Beijing Institute of TechnologyBeijing 100081China

Precisely designing atomic metal-nitrogen-carbon(M-N-C)catalysts with asymmetric diatomic configurations and studying their structure–activity relationships for oxygen reduction reaction(ORR)are important for zinc-air batteries(ZABs).Herein,a dualatomic-site catalyst(DASC)with CoN_(3)S-MnN_(2)S_(2) configuration was prepared for the cathodes of *** with Co-N-C(Mn-free)and CoMn-N-C(S-free doping),CoMn-N/S-C exhibits excellent half-wave potential(0.883 V)and turnover frequency(1.54 e·s^(−1)·site^(−1)),surpassing most of the reported state-of-the-art Pt-free ORR *** CoMn-N/S-C-based ZABs achieve extremely high specific capacity(959 mAh·g^(−1))and good stability(350 h@5 mA·cm^(−2)).Density functional theory(DFT)calculation shows that the introduction of Mn and S can break the electron configuration symmetry of the original Co 3d orbital,lower the dband center of the Co site,and optimize the desorption behavior of*OH intermediate,thereby increasing the ORR activity.

关键词： metal organic frameworks oxygen reduction reaction dual-atom catalyst coordination-environment regulation zinc-air batteries

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Synergistic Effect of Graphdiyne-based Electrocatalysts

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Chemical Research in Chinese Universities 2021年第6期37卷 1242-1256页

作者： WONG Hon Ho SUN Mingzi HUANG Bolong Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARP.R.China

The synergistic effect can help improve the electrocatalyst performances by combining the advantages of individual *** particular,such an effect has been more important in the atomic *** this review,we have summarized the synergistic effect of N,X co-doping graphdiyne[X=B,S,F or transition metal(TM)]electrocatalysts and graphdiyne-based dual-atom catalyst(GDY-DAC).In general,the synergistic cooperation between two different dopants in co-doped GDY and adjacent active sites in GDY-DAC not only promotes their catalytic activity but also greatly enhances the thermodynamic stability of the *** the N,X co-doping GDY electrocatalysts,doping the heteroatoms like boron,sulphur,phosphorus,and fluorine with nitrogen can further tune the charge density distribution and electronic ***,the electron exchange between two doping atoms and GDY substrate has been discussed,where the TM-based GDY-DAC is a very promising catalyst for *** importantly,electronic interactions between different elements on GDY have been carefully *** the end,we have also supplied perspectives to the future developments of the GDY-based electrocatalysts.

关键词： Graphdiyne(GDY) Electrocatalyst Synergistic effect dual-atom catalyst co-Doped GDY

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Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

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Journal of Energy Chemistry 2024年第5期92卷 16-25页

作者： Baoyu Wang Jinshu Huang Hongguo Wu Ximing Yan Yuhe Liao Hu Li National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide&Agricultural BioengineeringMinistry of EducationState-Local Joint Laboratory for Comprehensive Utilization of BiomassCollege of Pharmacy&Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025GuizhouChina Guangxi Key Laboratory of Green Chemical Materials and Safety Technology Beibu Gulf UniversityQinzhou 535011GuangxiChina Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of ***,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous *** synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical ***,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer *** in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

关键词： Biomass conversion Heterogeneous catalysis Lignin dual-atom catalyst Selective C-ocleavage

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