School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou 730070, China.
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China.
Nano Lett. 2023 Mar 8;23(5):1735-1742. doi: 10.1021/acs.nanolett.2c04444. Epub 2023 Feb 14.
We design single-atom W confined in MoO amorphous nanosheets (W/MoO) comprising W-O motifs as a highly active and durable NORR catalyst. Theoretical and operando spectroscopic investigations reveal the dual functions of W-O motifs to (1) facilitate the activation and protonation of NO molecules and (2) promote HO dissociation while suppressing *H dimerization to increase the proton supply, eventually resulting in a self-tandem NORR mechanism of W/MoO to greatly accelerate the protonation energetics of the NO-to-NH pathway. As a result, W/MoO exhibits the highest NH-Faradaic efficiency of 91.2% and NH yield rate of 308.6 μmol h cm, surpassing that of most previously reported NORR catalysts.
我们设计了一种单原子 W 被限制在 MoO 非晶纳米片中的（W/MoO），其中包含 W-O 基作为一种高效且耐用的 NORR 催化剂。理论和原位光谱研究揭示了 W-O 基的双重功能，即（1）促进 NO 分子的活化和质子化，（2）促进 HO 解离，同时抑制*H 二聚化以增加质子供应，最终导致 W/MoO 的自串联 NORR 机制极大地加速了 NO 到 NH 途径的质子化能学。结果，W/MoO 表现出最高的 NH 法拉第效率为 91.2%和 NH 生成速率为 308.6 μmol h cm，超过了大多数先前报道的 NORR 催化剂。
