课题组孙瑜婕同学在Journal of Colloid and Interface Science发表硝酸盐还原催化剂设计相关论文
发布时间：2024-09-01
作者
Yujie Sun, Guoning Feng, Zhiwei Wang, Xiaojing Liu, Xin Chen, Rongjian Sa, Qiaohong Li, Xiaoqiang Li, Zuju Ma
发表日期
2024/12/15
期刊
Journal of Colloid and Interface Science
卷号
676
页码范围
1023-1031
出版商
Academic Press
简介
Nitrate contamination of water resources poses significant health and environmental risks, necessitating efficient denitrification methods that produce ammonia as a desirable product. The electrocatalytic nitrate reduction reaction (NO3RR) powered by renewable energy offers a promising solution, however, developing highly active and selective catalysts remains challenging. Single-atom catalysts (SACs) have shown impressive performance, but the crucial role of their coordination environment, especially the next-nearest neighbor dopant atoms, in modulating catalytic activity for NO3RR is underexplored. This study aims to optimize the NO3RR performance of tungsten (W) single atoms anchored on graphene by precisely engineering their coordination environment through first and next-nearest neighbor dopants. The stability, reaction paths, activity, and selectivity of 43 different nitrogen and boron doping configurations were systematically studied using density functional theory. The results reveal W@C3, with W coordinated to three carbon atoms, exhibits outstanding NO3RR activity with a low limiting potential of −0.36 V. Intriguingly, introducing next-nearest neighbor B and N dopants further enhances the performance, with W@C3-BN achieving a lower limiting potential of −0.26 V. This exceptional activity originates from optimal nitrate adsorption strengths facilitated by orbital hybridization and charge modulation effects induced by the dopants. Furthermore, high energy barriers for NO2 and NO formation on W@C3 and W@C3-BN ensure their selectivity towards NO3RR products. These findings provide crucial atomic-level insights into rational design strategies for high-performance single-atom NO3RR catalysts via coordination environment engineering.
《Journal of Colloid and Interface Science 》为2023年中科院大类一区论文，影响因子9.4