气凝胶
催化作用
电合成
部分
硝酸盐
碳纤维
氨
无机化学
吸附
选择性催化还原
化学
材料科学
电化学
纳米技术
有机化学
物理化学
复合数
电极
复合材料
作者
Ran Li,Taotao Gao,Pengfei Wang,Wenxi Qiu,Kui Liu,Yuanting Liu,Zhaoyu Jin,Panpan Li
标识
DOI:10.1016/j.apcatb.2023.122677
摘要
Electrocatalytic nitrate reduction reaction (NitRR) to NH3 provides an appealing route to reform the energy-consuming ammonia industry. Considerable studies have demonstrated transition-metal-based catalysts for the NitRR, while most of them suffer from high cost, poor stability, and unsatisfactory selectivity. In this work, a group of carbon-based aerogel catalysts with regulated N species have been developed for highly efficient nitrate-to-ammonia reduction. The results show that the electrocatalytic performance is dependent on the graphitic-N moiety, where the catalyst with the highest content of graphitic-N moiety exhibits a maximum NH3 yield rate of 1.33 mgNH3 h−1 cm−2 with the faradaic efficiency of ca. 95%. The theoretical investigation further reveals the strong adsorption of nitrate on graphitic-N moiety as the reason for the enhanced NO3ˉ-to-NH3 activity. This study, thus, provides a fundamental understanding of the intrinsic mechanism of the NitRR on nitrogen-doped carbon structures, facilitating the rational design of metal-free catalysts for advanced electrosynthesis.
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