In:
Angewandte Chemie International Edition, Wiley, Vol. 60, No. 13 ( 2021-03-22), p. 7382-7388
Abstract:
The development of efficient electrocatalysts for the CO 2 reduction reaction (CO 2 RR) remains a challenge. Demonstrated here is a NiSn atomic‐pair electrocatalyst (NiSn‐APC) on a hierarchical integrated electrode, which exhibits a synergistic effect in simultaneously promoting the activity and selectivity of the CO 2 RR to formate. The NiSn atomic pair consists of adjacent Ni and Sn, each coordinated with four nitrogen atoms (N 4 ‐Ni‐Sn‐N 4 ). The as‐prepared NiSn‐APC displays exceptional activity for the CO 2 RR to formate with a turnover frequency of 4752 h −1 , a formate productivity of 36.7 mol h −1 g Sn −1 and an utilization degree of active sites (57.9 %), which are superior to previously reported single‐atomic catalysts. Both experimental data and density‐functional theory calculations verify the electron redistribution of Sn imposed by adjacent Ni, which reduces the energy barrier of the *OCHO intermediate and makes this potential‐determining step thermodynamically spontaneous. This synergistic catalysis provides a successful paradigm for rational design and preparation of atomic‐pair electrocatalysts with enhanced performance.
Type of Medium:
Online Resource
ISSN:
1433-7851
,
1521-3773
DOI:
10.1002/anie.202014655
Language:
English
Publisher:
Wiley
Publication Date:
2021
detail.hit.zdb_id:
2011836-3
detail.hit.zdb_id:
123227-7
