Pre‐Adsorbed H‐Assisted N<sub>2</sub> Activation on Single‐Atom Cadmium‐O<sub>5</sub> Decorated In<sub>2</sub>O<sub>3</sub> for Efficient NH<sub>3</sub> Electrosynthesis
Zhibo Yao, Shiqiang Liu, Honghong Liu, Yukun Ruan, Song Hong, Tai‐Sing Wu, Leiduan Hao, Y. L. Soo, Pei Xiong, Molly Meng‐Jung Li, Alex W. Robertson, Qineng Xia, Liang‐Xin Ding, Zhenyu Sun
Abstract
Abstract The electrocatalytic nitrogen reduction reaction (NRR) provides a promising avenue for sustainable and decentralized green ammonia (NH 3 ) synthesis. To promote the NRR, the design and synthesis of efficient electrocatalysts with an elucidated reaction mechanism is critically important. Here, surface hydrogenation‐facilitated NRR is demonstrated to yield NH 3 at low overpotentials on oxygen‐deficient In 2 O 3 plates decorated with single atom CdO 5 that have a weak N 2 ‐binding capability. Adsorbed * H is calculated to be first produced via the Volmer reaction (H 2 O + e − → * H + OH − ) and then reacts with dissolved N 2 to generate * N 2 H 2 , which is likely the rate determining step (RDS) of the whole process. Cd atoms and oxygen vacancies in In 2 O 3 jointly enhance the activation of N 2 and accelerate the RDS, boosting the NRR. An NH 3 production rate of as high as 57.5 µg h −1 mg cat −1 is attained at a mild potential, which is retained to a large extent even after 44 h of continuous polarization.