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Rational Design of Dot‐on‐Rod Nano‐Heterostructure for Photocatalytic CO<sub>2</sub> Reduction: Pivotal Role of Hole Transfer and Utilization

Zhi‐Kun XinKey Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. ChinaYu‐Ji GaoKey Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. ChinaYuying GaoKey Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. ChinaHongwei SongBeijing National Laboratory for Molecular Sciences Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P. R. ChinaJiaqing ZhaoKey Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. ChinaFengtao FanState Key Laboratory of Catalysis Dalian National Laboratory for Clean Energy The Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM) Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. ChinaAndong XiaSchool of Science Beijing University of Posts and Communications Beijing 100876 ChinaXu‐Bing LiKey Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. ChinaChen‐Ho TungKey Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. ChinaLi‐Zhu WuKey Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China

2021en

ABI

Annotatsiya

Abstract Inspired by green plants, artificial photosynthesis has become one of the most attractive approaches toward carbon dioxide (CO 2 ) valorization. Semiconductor quantum dots (QDs) or dot‐in‐rod (DIR) nano‐heterostructures have gained substantial research interest in multielectron photoredox reactions. However, fast electron–hole recombination or sluggish hole transfer and utilization remains unsatisfactory for their potential applications. Here, the first application of a well‐designed ZnSe/CdS dot‐on‐rods (DORs) nano‐heterostructure for efficient and selective CO 2 photoreduction with H 2 O as an electron donor is presented. In‐depth spectroscopic studies reveal that surface‐anchored ZnSe QDs not only assist ultrafast (≈2 ps) electron and hole separation, but also promote interfacial hole transfer participating in oxidative half‐reactions. Surface photovoltage (SPV) spectroscopy provides a direct image of spatially separated electrons in CdS and holes in ZnSe. Therefore, ZnSe/CdS DORs photocatalyze CO 2 to CO with a rate of ≈11.3 µmol g −1 h −1 and ≥85% selectivity, much higher than that of ZnSe/CdS DIRs or pristine CdS nanorods under identical conditions. Obviously, favored energy‐level alignment and unique morphology balance the utilization of electrons and holes in this nano‐heterostructure, thus enhancing the performance of artificial photosynthetic solar‐to‐chemical conversion.

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Identifikatorlar

DOI: 10.1002/adma.202106662

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