Selectivity control of photocatalytic CO2 reduction over ZnS-based nanocrystals: A comparison study on the role of ionic cocatalysts

doi:10.1016/j.jechem.2023.07.031

Journal of Energy Chemistry ›› 2023, Vol. 86 ›› Issue (11): 391-398.DOI: 10.1016/j.jechem.2023.07.031

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Selectivity control of photocatalytic CO₂ reduction over ZnS-based nanocrystals: A comparison study on the role of ionic cocatalysts

Hong Pang^b,1, Fumihiko Ichihara^c,1, Xianguang Meng^a, Lijuan Li^a, Yuqi Xiao^a, Wei Zhou^d,*, Jinhua Ye^b,e,*

^aHebei Provincial Laboratory of Inorganic Nonmetallic Materials, College of Materials Science and Engineering, North China University of Science and Technology, Tangshan 063210, Hebei, China;
^bInternational Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), Tsukuba 305-0044, Japan;
^cCenter for Green Research on Energy and Environmental Materials (GREEN), National Institute for Materials Science (NIMS), Tsukuba 305-0044, Japan;
^dDepartment of Applied Physics, School of Science, Tianjin University, Tianjin 300072, China;
^eGraduate School of Chemical Sciences and Engineering, Hokkaido University, Sapporo 060-0814, Japan

Received:2023-06-03 Revised:2023-07-21 Accepted:2023-07-25 Online:2023-11-15 Published:2023-11-07
Contact: *E-mail addresses: mengxg_materchem@163.com (X. Meng), weizhou@tju.edu.cn (W. Zhou), jinhua.YE@nims.go.jp (J. Ye).
About author:¹These authors contributed equally to this work.

Abstract

Abstract: Taking copper doped ZnS (ZnS:Cu) nanocrystals as the main body of photocatalyst, the influence of different base transition metal ions (M²⁺ = Ni²⁺, Co²⁺, Fe²⁺ and Cd²⁺) on photocatalytic CO₂ reduction in inorganic reaction system is investigated. Confined single-atom Ni²⁺, Co²⁺, and Cd²⁺ sites were created via cation-exchange process and enhanced CO₂ reduction, while Fe²⁺ suppressed the photocatalytic activity for both water and CO₂ reduction. The modified ZnS:Cu photocatalysts (M/ZnS:Cu) demonstrated tunable product selectivity, with Ni²⁺ and Co²⁺ showing high selectivity for syngas production and Cd²⁺ displaying remarkable formate selectivity. DFT calculations indicated favorable H adsorption free energy on Ni²⁺ and Co²⁺ sites, promoting the hydrogen evolution reaction. The selectivity of CO₂ reduction products was found to be sensitive to the initial intermediate adsorption states. *COOH formed on Ni²⁺ and Co²⁺ while *OCHO formed on Cd²⁺, favoring the production of CO and HCOOH as the main products, respectively. This work provides valuable insights for developing efficient solar-to-fuel platforms with controlled CO₂ reduction selectivity.

Key words: CO₂ reduction, Photocatalysis, ZnS, Ionic cocatalyst, Formate, Syngas, DFT calculations

Hong Pang, Fumihiko Ichihara, Xianguang Meng, Lijuan Li, Yuqi Xiao, Wei Zhou, Jinhua Ye. Selectivity control of photocatalytic CO₂ reduction over ZnS-based nanocrystals: A comparison study on the role of ionic cocatalysts[J]. Journal of Energy Chemistry, 2023, 86(11): 391-398.

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Selectivity control of photocatalytic CO₂ reduction over ZnS-based nanocrystals: A comparison study on the role of ionic cocatalysts

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