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Author:

Yu, Linqun (Yu, Linqun.) | Wang, Qiushi (Wang, Qiushi.) | Zhuang, Chunqiang (Zhuang, Chunqiang.) | Huang, Jin-Dou (Huang, Jin-Dou.) | Zhu, Yongan (Zhu, Yongan.) | Jing, Xuedong (Jing, Xuedong.) | Guo, Yuhang (Guo, Yuhang.) | Tong, Ye-Xiang (Tong, Ye-Xiang.) | Zhang, Zhenyi (Zhang, Zhenyi.)

Indexed by:

EI Scopus SCIE

Abstract:

Lewis acids (LAs) or Lewis bases (LBs) have been recognized as crucial catalytically active sites for enhancing the adsorption and conversion of inert CO2. However, engineering of periodic frustrated Lewis pairs (PFLPs) on the surfaces of semiconductor photocatalysts presents significant challenges, and the synergistic mechanism of PFLPs in CO2 photoreduction remains unclear. In this study, we propose a strategy that utilizes periodic oxygen vacancies to engineer dual-metallic PFLPs on bimetallic oxide semiconductor surfaces. We employ SrNb2O6-x as a model photocatalyst to elucidate the synergistic effect of PFLPs on CO2 photoreduction. Within each FLP unit, the LA (Sr2+) captures an O atom from CO2 while the LB (Nb4+) engages in an interaction with the C atom and concurrently facilitates transfer of photoinduced electrons from SrNb2O6-x to adsorbed CO2. Thus, SrNb2O6-x with the PFLPs-enriched surface exhibits ultrahigh CO2 adsorption and a low energy barrier for CO desorption. Under focused sunlight irradiation, SrNb2O6-x demonstrates nearly 100% selectivity in converting CO2 to CO at a rate of 25.5 mu mol g(-1) h(-1). This study presents a method for designing metal PFLPs on inorganic photocatalyst surfaces, which could contribute to the practical implementation of CO2 photoreduction.

Keyword:

periodic frustrated Lewis pairs CO2 reduction inorganicsemiconductor CO selectivity photocatalysis

Author Community:

  • [ 1 ] [Yu, Linqun]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China
  • [ 2 ] [Wang, Qiushi]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China
  • [ 3 ] [Huang, Jin-Dou]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China
  • [ 4 ] [Zhu, Yongan]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China
  • [ 5 ] [Jing, Xuedong]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China
  • [ 6 ] [Guo, Yuhang]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China
  • [ 7 ] [Zhang, Zhenyi]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China
  • [ 8 ] [Zhuang, Chunqiang]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 9 ] [Tong, Ye-Xiang]Sun Yat Sen Univ, Sch Chem, MOE Key Lab Bioinorgan & Synthet Chem, Sch Mat Sci & Engn,Key Lab Low Carbon Chem & Energ, Guangzhou 510275, Peoples R China

Reprint Author's Address:

  • [Zhang, Zhenyi]Dalian Minzu Univ, Sch Phys & Mat Engn, Key Lab New Energy & Rare Earth Resource Utilizat, Key Lab Photosensit Mat & Devices Liaoning Prov, 18 Liaohe West Rd, Dalian 116600, Peoples R China

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Source :

ACS NANO

ISSN: 1936-0851

Year: 2025

Issue: 7

Volume: 19

Page: 7239-7252

1 7 . 1 0 0

JCR@2022

Cited Count:

WoS CC Cited Count: 1

SCOPUS Cited Count: 1

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 7

Affiliated Colleges:

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