In:
Angewandte Chemie International Edition, Wiley, Vol. 61, No. 28 ( 2022-07-11)
Abstract:
Single‐atom alloys hold great promise for electrocatalytic nitrogen reduction reaction (NRR), while the comprehensive experimental/theoretical investigations of SAAs for the NRR are still missing. Herein, PdFe 1 single‐atom alloy metallene, in which the Fe single atoms are confined on a Pd metallene support, is first developed as an effective and robust NRR electrocatalyst, delivering exceptional NRR performance with an NH 3 yield of 111.9 μg h −1 mg −1 , a Faradaic efficiency of 37.8 % at −0.2 V (RHE), as well as a long‐term stability for 100 h electrolysis. In‐depth mechanistic investigations by theoretical computations and operando X‐ray absorption/Raman spectroscopy indentify Pd‐coordinated Fe single atoms as active centers to enable efficient N 2 activation via N 2 ‐to‐Fe σ‐donation, reduced protonation energy barriers, suppressed hydrogen evolution and excellent thermodynamic stability, thus accounting for the high activity, selectivity and stability of PdFe 1 for the NRR.
Type of Medium:
Online Resource
ISSN:
1433-7851
,
1521-3773
DOI:
10.1002/anie.202205923
Language:
English
Publisher:
Wiley
Publication Date:
2022
detail.hit.zdb_id:
2011836-3
detail.hit.zdb_id:
123227-7
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