In situ unraveling of the effect of the dynamic chemical state on selective CO2 reduction upon zinc electrocatalysts

被引：26

作者：

Chen, Tai-Lung ^{[1
]}

Chen, Hsiao-Chien ^{[1
,2
]}

Huang, Yen-Po ^{[1
]}

Lin, Sheng-Chih ^{[1
]}

Hou, Cheng-Hung ^{[3
]}

Tan, Hui-Ying ^{[1
]}

Tung, Ching-Wei ^{[1
]}

Chan, Ting-Shan ^{[4
]}

Shyue, Jing-Jong ^{[3
,5
]}

Chen, Hao Ming ^{[1
,4
]}

机构：

[1] Natl Taiwan Univ, Dept Chem, Taipei 10617, Taiwan

[2] Natl Cheng Kung Univ, Dept Photon, Tainan 70101, Taiwan

[3] Acad Sinica, Res Ctr Appl Sci, Taipei 11529, Taiwan

[4] Natl Synchrotron Radiat Ctr, Hsinchu 30076, Taiwan

[5] Natl Taiwan Univ, Dept Mat Sci & Engn, Taipei 10617, Taiwan

来源：

NANOSCALE | 2020年 / 12卷 / 35期

关键词：

ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; HIGHLY EFFICIENT; METAL-ELECTRODES; FORMIC-ACID; ELECTROREDUCTION; EVOLUTION; HYDROGEN; COPPER;

D O I：

10.1039/d0nr03475d

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Unraveling the reaction mechanism behind the CO(2)reduction reaction (CO2RR) is a crucial step for advancing the development of efficient and selective electrocatalysts to yield valuable chemicals. To understand the mechanism of zinc electrocatalysts toward the CO2RR, a series of thermally oxidized zinc foils is prepared to achieve a direct correlation between the chemical state of the electrocatalyst and product selectivity. The evidence provided byin situRaman spectroscopy, X-ray absorption spectroscopy (XAS) and X-ray diffraction significantly demonstrates that the Zn(ii) and Zn(0) species on the surface are responsible for the production of carbon monoxide (CO) and formate, respectively. Specifically, the destruction of a dense oxide layer on the surface of zinc foil through a thermal oxidation process results in a 4-fold improvement of faradaic efficiency (FE) of formate toward the CO2RR. The results fromin situmeasurements reveal that the chemical state of zinc electrocatalysts could dominate the product profile for the CO2RR, which provides a promising approach for tuning the product selectivity of zinc electrocatalysts.

引用

页码：18013 / 18021

页数：9

共 43 条

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