Nano-CaCO3 templated porous carbons anchored with Fe single atoms enable high-efficiency N2 electroreduction to NH3. (10th September 2022)

• Record Type: Journal Article
• Authors: Ma, Xiaobo; Gao, Lijun; Zhang, Qiyu; Hua, Weibo; Zhang, Yating; Li, Xinyang; Yang, Juan; Ding, Shujiang; Hu, Chao
• Is Part Of: Electrochimica acta. Volume 426(2022)
• Publication Date: 2022-09-10
• Subjects: Electrocatalysis -- N2-fixation -- Hard template -- Single-atom catalysis -- Hierarchical porous carbon; Electrochemistry -- Periodicals; Electrochemistry, Industrial -- Periodicals; 541.37
• DOI: 10.1016/j.electacta.2022.140805
• Languages: English
• ISSNs: 0013-4686

Abstract

Abstract: The traditional Haber-Bosch N2 fixation process suffers from rigorous reaction conditions and massive CO2 emission. By contrast, N2 electroreduction by water to the direct production of NH3 can be conducted at room temperature and atmospheric pressure, and thus has been attracting increasingly attention. Herein, we develop a nano-CaCO3 template route for the synthesis of Fe, N co-doped porous carbon materials from zeolitic imidazolate framework-8 (ZIF-8). The Fe atoms are atomically dispersed in the skeleton of carbon and bonded with four nitrogen atoms. Interestingly, the morphology and pore structure of these carbons have notable effects on their performance for the electrocatalytic reduction of N2 . With an optimized morphology and pore structure tuned by the addition of nano-CaCO3 template, the ZIF-8 derived Fe, N co-doped carbon catalyst shows a Faradaic efficiency of 13.14% and a NH3 yield as high as 13.01 µg h −1 mgcat −1 (−0.2 vs . reversible hydrogen electrode) for N2 reduction reaction in 0.1 M KOH aqueous electrolyte. Morphology engineering strategy may open a new path to designing and synthesizing high-performance carbon-based catalysts for the electroreduction of N2 to NH3 .