Rationally designed nitrogen-doped carbon macroporous fibers with uneven loading of single cobalt sites for efficient aqueous Zn-CO₂ batteries

• Main Authors: Zhao, Yafei, Pei, Zhihao, Lu, Xue Feng, Luan, Deyan, Wang, Xin, Lou, David Xiong Wen
• Other Authors: School of Chemical and Biomedical Engineering
• Format: Article
• Language: English
• Published: 2023
• Subjects: Science::Chemistry; Classification Description; CO2 Electroreduction
• Online Access: https://hdl.handle.net/10356/166114
• Institution: Nanyang Technological University

Atomically dispersed metal catalysts supported on the rigidly hollow matrix are promising materials for developing carbon-neutral technologies. Herein, we develop an elaborate multistep templating approach to fabricate cobalt single-atom-decorated nitrogen-doped carbon macroporous fibers (Co SAs@NCMFs). During the thermal reduction, the cobalt nanoparticles derived from the sintered Co2+ ions are formed at 600°C, which can be further transformed into unevenly loaded atomically dispersed cobalt sites at 1,000°C. The Co SAs@NCMF catalyst delivers excellent CO Faradaic efficiency (98.4%) and turnover frequency (38,390 h−1) at −1.0 V versus reversible hydrogen electrode for CO2 electroreduction. Furthermore, benefiting from the multiple advantageous features, including rigidly hollow structure, high specific surface area, and accessible active sites, the Co SAs@NCMF electrode shows outstanding rechargeability and stable cycle life in aqueous Zn-CO2 batteries.