Porous Host–Guest MOF‐Semiconductor Hybrid with Multisites Heterojunctions and Modulable Electronic Band for Selective Photocatalytic CO2 Conversion and H2 Evolution

Author:

Zhang Tianxi1,Meng Fanlu2,Gao Minmin2,Wei Jishi2,Lim Kane Jian Hong2,Lim Kang Hui1,Chirawatkul Prae3,Wong Andrew See Weng4,Kawi Sibudjing1,Ho Ghim Wei25ORCID

Affiliation:

1. Department of Chemical & Biomolecular Engineering National University of Singapore 4 Engineering Drive 4 Singapore 117585 Singapore

2. Department of Electrical and Computer Engineering National University of Singapore 4 Engineering Drive 3 Singapore 117583 Singapore

3. Synchrotron Light Research Institute (Public Organization) 111 University Avenue Muang Nakhon Ratchasima 30000 Thailand

4. Facility for Analysis Characterization Testing and Simulation (FACTS) Nanyang Technological University Singapore 639798 Singapore

5. Institute of Materials Research and Engineering A*STAR (Agency for Science, Technology and Research) 3 Research Link Singapore 117602 Singapore

Abstract

AbstractOptimizing catalysts for competitive photocatalytic reactions demand individually tailored band structure as well as intertwined interactions of light absorption, reaction activity, mass, and charge transport.  Here, a nanoparticulate host–guest structure is rationally designed that can exclusively fulfil and ideally control the aforestated uncompromising requisites for catalytic reactions. The all‐inclusive model catalyst consists of porous Co3O4 host and ZnxCd1‐xS guest with controllable physicochemical properties enabled by self‐assembled hybrid structure and continuously amenable band gap. The effective porous topology nanoassembly, both at the exterior and the interior pores of a porous metal–organic framework (MOF), maximizes spatially immobilized semiconductor nanoparticles toward high utilization of particulate heterojunctions for vital charge and reactant transfer. In conjunction, the zinc constituent band engineering is found to regulate the light/molecules absorption, band structure, and specific reaction intermediates energy to attain high photocatalytic CO2 reduction selectivity. The optimal catalyst exhibits a H2‐generation rate up to 6720 µmol g−1 h−1 and a CO production rate of 19.3 µmol g−1 h−1. These findings provide insight into the design of discrete host–guest MOF‐semiconductor hybrid system with readily modulated band structures and well‐constructed heterojunctions for selective solar‐to‐chemical conversion.

Publisher

Wiley

Subject

Biomaterials,Biotechnology,General Materials Science,General Chemistry

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