In-Induced Electronic Structure Modulations of Bi―O Active Sites for Selective Carbon Dioxide Electroreduction to Liquid Fuel in Strong Acid

作者：Chen, Wei; Chen, Rongzhen; Jiang, Yuhang; Wang, Yating; Zhu, Yihua; Li, Yuhang^*; Li, Chunzhong^*

来源：Small, 2024, 20(11): 2306795.

DOI：10.1002/smll.202306795

• acidic environment
• bismuth subcarbonate
• co(2) electroreduction
• formic acid

The formation of carbonate in neutral/alkaline solutions leads to carbonate crossover, severely reducing carbon dioxide (CO2) single pass conversion efficiency (SPCE). Thus, CO2 electrolysis is a prospective route to achieve high CO2 utilization under acidic environment. Bimetallic Bi-based catalysts obtained utilizing metal doping strategies exhibit enhanced CO2-to-formic acid (HCOOH) selectivity in alkaline/neutral media. However, achieving high HCOOH selectivity remains challenging in acidic media. To this end, Indium (In) doped Bi2O2CO3 via hydrothermal method is prepared for in-situ electroreduction to In-Bi/BiOx nanosheets for acidic CO2 reduction reaction (CO2RR). In doping strategy regulates the electronic structure of Bi, promoting the fast derivatization of Bi2O2CO3 into Bi-O active sites to enhance CO2RR catalytic activity. The optimized Bi2O2CO3-derived catalyst achieves the maximum HCOOH faradaic efficiency (FE) of 96% at 200 mA cm(-2). The SPCE for HCOOH production in acid is up to 36.6%, 2.2-fold higher than the best reported catalysts in alkaline environment. Furthermore, in situ Raman and X-ray photoelectron spectroscopy demonstrate that In-induced electronic structure modulation promotes a rapid structural evolution from nanobulks to Bi/BiOx nanosheets with more active species under acidic CO2RR, which is a major factor in performance improvement.

• 单位
  华东理工大学