In:
Nanoscale, Royal Society of Chemistry (RSC), Vol. 14, No. 4 ( 2022), p. 1211-1218
Abstract:
The electrochemical CO 2 reduction reaction (CO 2 RR) has become a promising technology to resolve globally accelerating CO 2 emissions and produce chemical fuels. In this work, the electrocatalytic performance of transition metal (TM = Cu, Cr, Mn, Co, Ni, Mo, Pt, Rh, Ru and V) triatomic clusters embedded in a graphdiyne (GDY) monolayer (TM 3 @GDY) for CO 2 RR is investigated by density functional theory (DFT) calculations. The results indicate that Cr 3 @GDY possesses the best catalytic performance with a remarkably low rate-limiting step of 0.39 eV toward the CO 2 product, and it can also effectively suppress the hydrogen evolution reaction (HER) during the entire CO 2 RR process. Studies on the rate-limiting steps (CHO* + H + + e − → CHOH) of Cr n @GDY ( n = 1–4) structures demonstrate that the high catalytic performance is attributed to the strong synergistic reaction of three Cr atoms interacting with the C atom for the Cr 3 @GDY structure. The strong synergistic reaction gives rise to the weakest interaction between O–Cr atoms, which leads to the strongest interaction between O–H atoms and makes the hydrogenation process easier for the Cr 3 @GDY structure. Furthermore, ab initio molecular dynamics simulations (AIMD) at 500 K reveal the high thermodynamic stability of the Cr 3 @GDY structure. These studies may provide a new approach for designing highly efficient electrocatalysts for the CO 2 RR under ambient conditions.
Type of Medium:
Online Resource
ISSN:
2040-3364
,
2040-3372
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2022
detail.hit.zdb_id:
2515664-0
