Wu Ze, Liu Yujing, Wang Dongdong, Zhang Yiqiong, Gu Kaizhi, He Zejin, Liu Limin, Liu Hanwen, Fan Jincheng, Chen Chen, Wang Shuangyin
College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha, Hunan, 410114, P. R. China.
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, the National Supercomputer Centers in Changsha, Hunan University, Changsha, Hunan, 410082, P. R. China.
Adv Mater. 2024 Mar;36(11):e2309470. doi: 10.1002/adma.202309470. Epub 2023 Dec 22.
Electrocatalytic reduction of nitric oxide (NO) to ammonia (NH ) is a clean and sustainable strategy to simultaneously remove NO and synthesize NH . However, the conversion of low concentration NO to NH is still a huge challenge. In this work, the dilatation strain between Cu and Co interface over Cu@Co catalyst is built up and investigated for electroreduction of low concentration NO (volume ratio of 1%) to NH . The catalyst shows a high NH yield of 627.20 µg h cm and a Faradaic efficiency of 76.54%. Through the combination of spherical aberration-corrected transmission electron microscopy and geometric phase analyses, it shows that Co atoms occupy Cu lattice sites to form dilatation strain in the xy direction within Co region. Further density functional theory calculations and NO temperature-programmed desorption (NO-TPD) results show that the surface dilatation strain on Cu@Co is helpful to enhance the NO adsorption and reduce energy barrier of the rate-determining step (*NO to *NOH), thereby accelerating the catalytic reaction. To simultaneously realize NO exhaust gas removal, NH green synthesis, and electricity output, a Zn-NO battery with Cu@Co cathode is assembled with a power density of 3.08 mW cm and an NH yield of 273.37 µg h cm .
将一氧化氮（NO）电催化还原为氨（NH₃）是一种同时去除NO并合成NH₃的清洁且可持续的策略。然而，将低浓度NO转化为NH₃仍然是一个巨大的挑战。在这项工作中，构建并研究了Cu@Co催化剂上Cu与Co界面之间的膨胀应变，用于将低浓度NO（体积比为1%）电还原为NH₃。该催化剂显示出627.20 μg h⁻¹ cm⁻²的高NH₃产率和76.54%的法拉第效率。通过结合球差校正透射电子显微镜和几何相位分析表明，Co原子占据Cu晶格位点，在Co区域内的xy方向形成膨胀应变。进一步的密度泛函理论计算和NO程序升温脱附（NO-TPD）结果表明，Cu@Co上的表面膨胀应变有助于增强NO吸附并降低速率决定步骤（NO到NOH）的能垒，从而加速催化反应。为了同时实现NO废气去除、NH₃绿色合成和电力输出，组装了具有Cu@Co阴极的Zn-NO电池，其功率密度为3.08 mW cm⁻²，NH₃产率为273.37 μg h⁻¹ cm⁻²。
