Modulating the Hydrogenation Mechanism of Electrochemical CO₂ Reduction Using Ruthenium Atomic Species on Bismuth

Liu, Xiao1,2; Zhen, Cheng3; Wu, Junxiu4; You, Xiao5; Wu, Yudong2; Hao, Qi2; Yu, Gang6; Gu, M. Danny7; Liu, Kai2; Lu, Jun4

2024-06-01

10.1002/adfm.202405835

ADVANCED FUNCTIONAL MATERIALS   影响因子和分区

1616-301X

1616-3028

The conversion of CO2 into formate through electrochemical methods is emerging as an elegant approach for industrial-scale CO2 utilization in the near future. Although Bismuth (Bi)-based materials have shown promise thank to their excellent selectivity, their limited reactivity remains a challenge. Herein, this study demonstrates a significant enhancement in the CO2-to-formate efficiency of Bi by incorporating ruthenium (Ru) atomic species. Ru single atom doped Bi exhibited a nearly twofold higher partial current density compared with pure Bi and Ru clusters doped Bi, while over 95% Faradaic efficiency (FE) is maintained. Through comprehensive investigations using a combined approach of electrochemical techniques, operando spectroscopy, and theoretical calculations, this study elucidates that the presence of Ru single atom promotes H2O dissociation and H* migration to Bi sites for CO2-to-formate conversion by significantly reducing the energy barrier via a H* spillover path. Besides, it is constructed Ru-Bi bridge sites for efficient CO2 hydrogenation via a non-spillover path, which served as the major mechanism for CO2-to-formate conversion in Ru single atom doped Bi.

atomic species CO2 reduction hydrogen spillover in situ FT-IR regulating water dissociation

SCI ; EI

英语

其他

Westlake University-Muyuan Joint Research Institute[206006022007] ; National Key Research and Development Project[2022YFA1503900] ; Shenzhen fundamental research funding["JCYJ20210324115809026","JCYJ20200109141216566","JCYJ20220818100212027"] ; Guangdong scientific program[2019QN01L057] ; National Foundation of China[512104-N12403ZJ] ; China Postdoctoral Foundation[2023M733021] ; null[103506022001]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001241445900001

WILEY-V C H VERLAG GMBH

MATERIALS SCIENCE

Web of Science

1.Zhejiang Univ, Coll Environm & Resource Sci, Hangzhou 310058, Zhejiang, Peoples R China
2.Westlake Univ, Sch Engn, Key Lab Coastal Environm & Resources Zhejiang Prov, Hangzhou 310030, Zhejiang, Peoples R China
3.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
4.Zhejiang Univ, Coll Chem & Biol Engn, Hangzhou 310027, Zhejiang, Peoples R China
5.Westlake Univ, Ctr Synthet Biol & Integrated Bioengn, Sch Engn, Hangzhou 310030, Zhejiang, Peoples R China
6.Beijing Normal Univ, Adv Interdisciplinary Inst Environm & Ecol, Guangdong Prov Key Lab Wastewater Informat Anal &, Zhuhai 519087, Peoples R China
7.Eastern Inst Technol, Eastern Inst Adv Study, Ningbo 315200, Zhejiang, Peoples R China

Liu, Xiao,Zhen, Cheng,Wu, Junxiu,et al. Modulating the Hydrogenation Mechanism of Electrochemical CO₂ Reduction Using Ruthenium Atomic Species on Bismuth[J]. ADVANCED FUNCTIONAL MATERIALS,2024.

Liu, Xiao.,Zhen, Cheng.,Wu, Junxiu.,You, Xiao.,Wu, Yudong.,...&Lu, Jun.(2024).Modulating the Hydrogenation Mechanism of Electrochemical CO₂ Reduction Using Ruthenium Atomic Species on Bismuth.ADVANCED FUNCTIONAL MATERIALS.

Liu, Xiao,et al."Modulating the Hydrogenation Mechanism of Electrochemical CO₂ Reduction Using Ruthenium Atomic Species on Bismuth".ADVANCED FUNCTIONAL MATERIALS (2024).