期刊
ADVANCED ENERGY MATERIALS
卷 10, 期 45, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202002499
关键词
CO(2)reduction; dual sites; porous architectures; sp hybridization; sulfur modification
类别
资金
- National Natural Science Foundation of China [21972015, 51672034]
- Young top talents project of Liaoning Province [XLYC1907147]
- Joint Research Fund Liaoning-Shenyang National Laboratory for Materials Science [2019JH3/30100003]
- Fundamental Research Funds for the Central Universities [DUT20TD06]
- Swedish Research Council
- K&A Wallenberg Foundation
Electrochemical CO(2)reduction is regarded as a promising strategy for the sustainable conversion of greenhouse gas. However, it still remains a significant challenge to manipulate the selectivity and activity. Herein, amorphous and porous Cd modified by sulfur (P-Cd|S) is synthesized by a p-block sulfur dopant. In comparison with unmodified Cd metal, the P-Cd|S architecture exhibits superior activity for selective CO generation, indicating that the sulfur dopant enables a selectivity shift from formic acid to CO. The high selectivity of P-Cd|S is partially ascribed to the local alkalization and suppression of hydrogen evolution as indicated by the finite element analysis. In-depth mechanistic investigations by operando Raman, Infrared, and X-ray photoelectron spectroscopy in combination with theory calculations indicate that the covalently hybridized sp band system with dual collaborative sites (Cd(delta)(+)and S-delta(-)) gives rise to a strong interplay with CO(2)molecules and carbonaceous species, leading to the natural elimination of linear correlation among intermediates binding for d-band metals and the convenient modulation of selectivity toward CO versus HCOOH.
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