Cargando…

The simplest construction of single-site catalysts by the synergism of micropore trapping and nitrogen anchoring

Single-site catalysts feature high catalytic activity but their facile construction and durable utilization are highly challenging. Herein, we report a simple impregnation-adsorption method to construct platinum single-site catalysts by synergic micropore trapping and nitrogen anchoring on hierarchi...

Descripción completa

Detalles Bibliográficos
Autores principales: Zhang, Zhiqi, Chen, Yugang, Zhou, Liqi, Chen, Chi, Han, Zhen, Zhang, Bingsen, Wu, Qiang, Yang, Lijun, Du, Lingyu, Bu, Yongfeng, Wang, Peng, Wang, Xizhang, Yang, Hui, Hu, Zheng
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6458126/
https://www.ncbi.nlm.nih.gov/pubmed/30971769
http://dx.doi.org/10.1038/s41467-019-09596-x
Descripción
Sumario:Single-site catalysts feature high catalytic activity but their facile construction and durable utilization are highly challenging. Herein, we report a simple impregnation-adsorption method to construct platinum single-site catalysts by synergic micropore trapping and nitrogen anchoring on hierarchical nitrogen-doped carbon nanocages. The optimal catalyst exhibits a record-high electrocatalytic hydrogen evolution performance with low overpotential, high mass activity and long stability, much superior to the platinum-based catalysts to date. Theoretical simulations and experiments reveal that the micropores with edge-nitrogen-dopants favor the formation of isolated platinum atoms by the micropore trapping and nitrogen anchoring of [PtCl(6)](2-), followed by the spontaneous dechlorination. The platinum-nitrogen bonds are more stable than the platinum-carbon ones in the presence of adsorbed hydrogen atoms, leading to the superior hydrogen evolution stability of platinum single-atoms on nitrogen-doped carbon. This method has been successfully applied to construct the single-site catalysts of other precious metals such as palladium, gold and iridium.