当前位置: X-MOL 学术Phys. Chem. Chem. Phys. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Theoretical investigation of single-atom catalysts anchored on pure carbon substrate for electroreduction of NO to NH3
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-11-16 , DOI: 10.1039/d2cp03704a
Yanle Li 1, 2 , Guokui Zheng 2, 3 , Lei Li 4 , Xingwang Zhang 3 , Ziqi Tian 2 , Liang Chen 2
Affiliation  

NO electrochemical reduction (NOER) can convert harmful NO pollutants into useful NH3 under ambient conditions, and thus is attracting increasing interest. With density functional theory calculations, we investigated a series of single transition metal (TM) atoms (Sc to Au) located on a pure carbon substrate C558 (TM@C558), as a potential electrocatalyst for NOER. The C558 substrate could stabilize the TM atom with delocalized π electrons, and activate TM atoms via charge transfer. Cu, Ag and Au doped systems are picked out with low limiting potentials for NOER and the inhibition of side reactions. The outstanding activities of Cu-, Ag- and Au@C558 systems are related to their appropriate d band centers and the moderate adsorption intensities of intermediates. Based on the simulations, a volcano relationship between NO binding energy and predicted activity is reported. After simulating the stability of these three single-atom catalysts, Au@C558 is finally regarded as the most promising NOER electrocatalyst with high stability. This work is expected to help with the discovery of novel NOER electrocatalysts in future experiments.

中文翻译:

固定在纯碳基底上的单原子催化剂用于将 NO 电还原为 NH3 的理论研究

NO 电化学还原 (NOER) 可以在环境条件下将有害的 NO 污染物转化为有用的 NH 3,因此受到越来越多的关注。通过密度泛函理论计算,我们研究了位于纯碳基底 C 558 (TM@C 558 ) 上的一系列单一过渡金属 (TM) 原子(Sc 到 Au),作为 NOER 的潜在电催化剂。C 558衬底可以用离域的π电子稳定TM原子,并通过电荷转移激活TM原子。Cu、Ag 和 Au 掺杂系统被挑选出来,具有低的 NOER 极限电位和副反应的抑制作用。Cu-、Ag- 和 Au@C 558的突出活性系统与其适当的 d 带中心和中间体的适度吸附强度有关。基于模拟,报告了 NO 结合能与预测活性之间的火山关系。在对这三种单原子催化剂的稳定性进行模拟后,Au@C 558最终被认为是最有前途的高稳定性 NOER 电催化剂。这项工作有望有助于在未来的实验中发现新型 NOER 电催化剂。
更新日期:2022-11-16
down
wechat
bug