posted on 2023-11-02, 11:40authored byYiqun Chen, Minqi Xia, Cao Zhou, Yan Zhang, Changkai Zhou, Fengfei Xu, Biao Feng, Xizhang Wang, Lijun Yang, Zheng Hu, Qiang Wu
Renewable-driven electrochemical CO2 reduction
reaction
(CO2RR) to syngas is an encouraging alternative strategy
to traditional fossil fuel-based syngas production, and the development
of industrial-level electrocatalysts is vital. Herein, based on theoretical
optimization of metal species, hierarchical CoxNi1–x–N–C
dual single-atom catalyst (DSAC) with individual NiN4 (CO
preferential) and CoN4 (H2 preferential) moieties
was constructed by a two-step pyrolysis route. The Co0.5Ni0.5–N–C exhibits a stable CO Faradaic
efficiency of 50 ± 5% and an industrial-level current density
of 101–365 mA cm–2 in an ultrawide potential
window of −0.5 to −1.1 V. The CO/H2 ratio
of syngas can be conveniently tuned by regulating the Co/Ni ratio.
The coupled effect of NiN4 and CoN4 moieties
under a local high-pH microenvironment is responsible for the regulation
of the CO/H2 selectivity and yield for the CoxNi1–x–N–C
catalyst, which is not present in the mixed Co–N–C and
Ni–N–C catalyst. This study provides a promising DSAC
strategy for achieving industrial-level syngas production via CO2RR.