期刊
NANOSCALE
卷 10, 期 32, 页码 15262-15272出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8nr04961k
关键词
-
类别
资金
- National Natural Science Foundation of China [21673137]
- Science and Technology Commission of Shanghai Municipality [16ZR1413900, 18030501100]
- Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory [DE-SC0012704]
Single-atom catalysts (SACs) have emerged as an excellent platform for enhancing catalytic performance. Inspired by the recent experimental synthesis of nitrogenated holey 2D graphene (C2N-h2D) (Mahmood et aL, Nat. Commun., 2015, 6, 6486-6493), we report density functional theory calculations combined with computational hydrogen electrode model to show that C2N-h2D supported metal single atoms (M@C2N) are promising electrocatalysts for CO2 reduction reaction (CO2 RR). M confined at pyridinic N6 cavity promotes activation of inert O=C=O bonds and subsequent protonation steps, with *COOH -> *CO -> CHO predicted to be the primary pathway for producing methanol and methane. It is found that *CO + H+ + e -> *CHO is most likely to be the potential determining step; breaking the scaling relation of *CO and *CHO binding on M@C2N SACs may simply be a rare event that is sensitively controlled by the detailed geometry of the adsorbate. Among twelve metals screened, M@C2N SACs where M = Ti, Mn, Fe, Co, Ni, Ru were identified to be effective in catalyzing CO2 RR with lowered overpotentials (0.58 V-0.80 V).
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据