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Engineering the axial coordination of cobalt single atom catalysts for efficient photocatalytic hydrogen evolution

Nano Research 2024年第6期17卷 5114-5121页

作者： Ning Kang Lingwen Liao Xue Zhang Zhen He Binlu Yu Jiahong Wang Yongquan Qu Paul KChu Seeram Ramakrishna Xue-Feng Yu Xin Wang Licheng Bai Materials Interfaces Center Shenzhen Institute of Advanced TechnologyChinese Academy of Sciences(CAS)Shenzhen 518055China Key Laboratory of Materials Physics Anhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsChinese Academy of SciencesHefei 230031China Department of Chemistry City University of Hong KongKowloonHong Kong 999077China Hong Kong Branch of National Precious metals Material Engineering Research Center(NPMM) City University of Hong KongKowloonHong Kong 999077China Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of Industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Department of Physics and Department of Materials Science and Engineering City University of Hong KongKowloonHong Kong 999077China National University of Singapore(NUS)Centre for Nanofibers and Nanotechnology Department of Mechanical EngineeringNational University of SingaporeSingapore 117542Singapore

Improving the catalytic activity of non-noble metal single atom catalysts(SACs)has attracted considerable attention in materials *** optimizing the local electronic structure of single atom can greatly improve their catalytic activity,it often involves in-plane modulation and requires high ***,we report a novel strategy to manipulate the local electronic structure of SACs via the modulation of axial Co-S bond anchored onto graphitic carbon nitride(C_(3)N_(4))at room temperature(RT).Each Co atom is bonded to four N atoms and one S atom(Co-(N,S)/C_(3)N_(4)).Owing to the greater electronegativity of S in the Co-S bond,the local electronic structure of the Co atoms is available to be controlled at a relatively moderate ***,when employed for the photocatalytic hydrogen evolution reaction,the adsorption energy of intermediate hydrogen(H*)on the Co atoms is remarkably *** the presence of the Co-(N,S)/C_(3)N_(4)SACs,the hydrogen evolution rates reach up to 10 mmol/(g·h),which is nearly 10 and 2.5 times greater than the rates in the presence of previously reported transition metal/C_(3)N_(4)and noble platinum nanoparticles(PtNPs)/C_(3)N_(4)catalysts,*** to the tailorable axial Co-S bond in the SAC,the local electronic structure of the Co atoms can be further optimized for other photocatalytic *** axial coordination engineering strategy is universal in catalyst designing and can be used for a variety of photocatalytic applications.

关键词： transition metal single-atom local electronic structure photocatalytic hydrogen evolution graphitic carbon nitride axial coordination environment

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