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Pre-Adsorbed H-Assisted N2 Activation on Single-Atom Cadmium-O5 Decorated In2O3 for Efficient NH3 Electrosynthesis
期刊文章

Pre-Adsorbed H-Assisted N2 Activation on Single-Atom Cadmium-O5 Decorated In2O3 for Efficient NH3 Electrosynthesis

Zhibo Yao, Shiqiang Liu, Honghong Liu, Yukun Ruan, Song Hong, Tai-Sing Wu, Leiduan Hao, Yun-Liang Soo, Pei Xiong, Molly Meng-Jung Li, …
Advanced Functional Materials
2022

摘要

electrocatalyses N 2 reduction NH 3 reaction mechanisms single-atom catalysts Chemistry (all) Materials Science (all) Condensed Matter Physics
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.

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