In:
Small, Wiley, Vol. 18, No. 16 ( 2022-04)
Abstract:
Exploring catalyst reconstruction under the electrochemical condition is critical to understanding the catalyst structure–activity relationship as well as to design effective electrocatalysts. Herein, a PbF 2 nanocluster is synthesized and its self‐reconstruction under the CO 2 reduction condition is investigated. F − leaching, CO 2 ‐saturated environment, and application of a cathodic potential induce self‐reconstruction of PbF 2 to Pb 3 (CO 3 ) 2 (OH) 2 , which effectively catalyze the CO 2 reduction to formate. The in situ formed Pb 3 (CO 3 ) 2 (OH) 2 discloses 〉 80% formate Faradaic efficiencies (FEs) across a broad range of potentials and achieves a maximum formate FE of ≈90.1% at −1.2 V versus reversible hydrogen electrode (RHE). Kinetic studies show that the CO 2 reduction reaction (CO 2 RR) on the Pb 3 (CO 3 ) 2 (OH) 2 is rate‐limited at the CO 2 protonation step, in which proton is supplied by bicarbonate (HCO 3 − ) in the electrolyte. To improve the CO 2 RR kinetics, the Pb 3 (CO 3 ) 2 (OH) 2 is further doped with Pd (4 wt%) to enhance its HCO 3 − adsorption, which leads to accelerated protonation of CO 2 . Therefore, the Pd‐Pb 3 (CO 3 ) 2 (OH) 2 (4 wt%) reveals higher formate FEs of 〉 90% from −0.8 to −1.2 V versus RHE and reaches a maximum formate FE of 96.5% at −1.2 V versus RHE with a current density of ≈13 mA cm −2 .
Type of Medium:
Online Resource
ISSN:
1613-6810
,
1613-6829
DOI:
10.1002/smll.202107885
Language:
English
Publisher:
Wiley
Publication Date:
2022
detail.hit.zdb_id:
2168935-0
Bookmarklink