Regulating Cu Oxidation State for Electrocatalytic CO₂ Conversion into CO with Near-Unity Selectivity via Oxygen Spillover

Jia, Yufei1; Li, Dekang2; Liu, Chang1; Song, Tao3,4; Duan, Lele3,4,5,6; Li, Fusheng1; Li, Fei1; Ji, Yongfei7; Sun, Licheng1,5,6; Fan, Ke1

2024-05-01

10.1002/smll.202402537

SMALL   影响因子和分区

1613-6810

1613-6829

Cu-based catalysts are the most intensively studied in the field of electrocatalytic CO2 reduction reaction (CO2RR), demonstrating the capacity to yield diverse C-1 and C2+ products albeit with unsatisfactory selectivity. Manipulation of the oxidation state of Cu sites during CO2RR process proves advantageous in modulating the selectivity of productions, but poses a formidable challenge. Here, an oxygen spillover strategy is proposed to enhance the oxidation state of Cu during CO2RR by incorporating the oxygen donor Sb2O4. The Cu-Sb bimetallic oxide catalyst attains a remarkable CO2-to-CO selectivity approaching unity, in stark contrast to the diverse product distribution observed with bare CuO. The exceptional Faradaic efficiency of CO can be maintained across a wide range of potential windows of approximate to 700 mV in 1 m KOH, and remains independent of the Cu/Sb ratio (ranging from 0.1:1 to 10:1). Correlative calculations and experimental results reveal that oxygen spillover from Sb2O4 to Cu sites maintains the relatively high valence state of Cu during CO2RR, which diminishes the binding strength of *CO, thereby achieving heightened selectivity in CO production. These findings propose the role of oxygen spillover in CO2RR over Cu-based catalysts, and shed light on the rational design of highly selective CO2 reduction catalysts.

CO2 reduction CuO electrocatalysis oxygen spillover Sb2O4

SCI ; EI

英语

其他

Fundamental Research Funds for the Central Universities["DUT23LAB611","DUT22LK01","DUT22QN213"] ; National Natural Science Foundation of China (NSFC)[22088102] ; null[2022YFA0911900] ; null[2022YFA0911904]

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

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

WOS:001214793500001

WILEY-V C H VERLAG GMBH

Web of Science

1.Dalian Univ Technol, Inst Energy Sci & Technol, Frontier Sci Ctr Smart Mat, State Key Lab Fine Chem, Dalian 116024, Peoples R China
2.Dalian Univ Technol, Sch Chem Engn, Inst Coal Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China
3.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
4.Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Shenzhen 518055, Peoples R China
5.Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Hangzhou 310024, Peoples R China
6.Westlake Univ, Dept Chem, Sch Sci, Hangzhou 310024, Peoples R China
7.Guangzhou Univ, Higher Educ Mega Ctr, Sch Chem & Chem Engn, 230 Wai Huan Xi Rd, Guangzhou 510006, Peoples R China

Jia, Yufei,Li, Dekang,Liu, Chang,et al. Regulating Cu Oxidation State for Electrocatalytic CO₂ Conversion into CO with Near-Unity Selectivity via Oxygen Spillover[J]. SMALL,2024.

Jia, Yufei.,Li, Dekang.,Liu, Chang.,Song, Tao.,Duan, Lele.,...&Fan, Ke.(2024).Regulating Cu Oxidation State for Electrocatalytic CO₂ Conversion into CO with Near-Unity Selectivity via Oxygen Spillover.SMALL.

Jia, Yufei,et al."Regulating Cu Oxidation State for Electrocatalytic CO₂ Conversion into CO with Near-Unity Selectivity via Oxygen Spillover".SMALL (2024).