State Key Laboratory of Chemo/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, P. R. China.
Department of Materials Science and Engineering, University of Toronto, Toronto, ON M5S 3E4, Canada.
J Am Chem Soc. 2023 Mar 29;145(12):6899-6904. doi: 10.1021/jacs.3c00276. Epub 2023 Mar 14.
Electrocatalytic nitric oxide (NO) reduction not only provides an extremely promising strategy for ambient NH generation but also alleviates the artificially disrupted N-cycle balance. However, exploring efficient electrocatalysts to enhance the NO electroreduction performance remains a significant challenge. Herein, a hexagonal-close-packed Co nanosheet (hcp-Co) is prepared and exhibits a high NH yield of 439.50 μmol cm h and a Faraday efficiency of 72.58%, outperforming the face-centered cubic phase of the Co nanosheet (fcc-Co) and most reported electrocatalysts. Through the combination of density functional theory calculations and NO temperature-programmed desorption experiments, the superior catalytic NO reduction reaction (NORR) activity on the hcp-Co can be attributed to the unique electron structures and proton shuttle effect. A proof-of-concept device of Zn-NO batteries using the hcp-Co as the cathode is assembled and shows a power density of 4.66 mW cm, which is superior to the reported performance in the literature so far.
电催化一氧化氮 (NO) 还原不仅为环境 NH3 的生成提供了极具前景的策略，还缓解了人为破坏的 N 循环平衡。然而，探索高效的电催化剂来增强 NO 电还原性能仍然是一个重大挑战。在此，制备了六方密排 Co 纳米片 (hcp-Co)，表现出 439.50 μmol cm h 的高 NH3 产率和 72.58%的法拉第效率，优于面心立方相的 Co 纳米片 (fcc-Co) 和大多数报道的电催化剂。通过密度泛函理论计算和 NO 程序升温脱附实验的结合，hcp-Co 上独特的电子结构和质子穿梭效应可以归因于其优越的催化 NO 还原反应 (NORR) 活性。组装了以 hcp-Co 为阴极的 Zn-NO 电池的概念验证装置，其功率密度为 4.66 mW cm，优于迄今为止文献中报道的性能。
