Phosphorus‐Doped Graphene Aerogel as Self‐Supported Electrocatalyst for CO2‐to‐Ethanol Conversion. Issue 25 (12th July 2022)

• Record Type: Journal Article
• Authors: Yang, Fangqi; Liang, Caihong; Yu, Haoming; Zeng, Zheling; Lam, Yeng Ming; Deng, Shuguang; Wang, Jun
• Is Part Of: Advanced science. Volume 9:Issue 25(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-07-12
• Subjects: CO2 reduction -- electrocatalysis -- ethanol -- graphene aerogel -- phosphorus; Science -- Periodicals; 505
• DOI: 10.1002/advs.202202006
• Languages: English
• ISSNs: 2198-3844

Abstract

Abstract: Electrochemical reduction of carbon dioxide (CO2 ) to ethanol is a promising strategy for global warming mitigation and resource utilization. However, due to the intricacy of C─C coupling and multiple proton–electron transfers, CO2 ‐to‐ethanol conversion remains a great challenge with low activity and selectivity. Herein, it is reported a P‐doped graphene aerogel as a self‐supporting electrocatalyst for CO2 reduction to ethanol. High ethanol Faradaic efficiency (FE) of 48.7% and long stability of 70 h are achieved at −0.8 VRHE . Meanwhile, an outstanding ethanol yield of 14.62 µmol h −1 cm −2 can be obtained, outperforming most reported electrocatalysts. In situ Raman spectra indicate the important role of adsorbed *CO intermediates in CO2 ‐to‐ethanol conversion. Furthermore, the possible active sites and optimal pathway for ethanol formation are revealed by density functional theory calculations. The graphene zigzag edges with P doping enhance the adsorption of *CO intermediate and increase the coverage of *CO on the catalyst surface, which facilitates the *CO dimerization and boosts the EtOH formation. In addition, the hierarchical pore structure of P‐doped graphene aerogels exposes abundant active sites and facilitates mass/charge transfer. This work provides inventive insight into designing metal‐free catalysts for liquid products from CO2 electroreduction. Abstract : P‐doped graphene aerogel is used as self‐supporting electrodes for favorable ethanol production from carbon dioxide (CO2 ) electroreduction with ethanol Faradaic efficiency (FE) and yield. This work can inspire the development of metal‐free electrocatalysts for C2+ production.