Enhanced Electroreduction of Carbon Dioxide to Methanol Using Zinc Dendrites Pulse‐Deposited on Silver Foam

The electrocatalytic CO2 reduction reaction (CO2RR) can dynamise the carbon cycle by lowering anthropogenic CO2 emissions and sustainably producing valuable fuels and chemical feedstocks. Methanol is arguably the most desirable C1 product of CO2RR, although it typically forms in negligible amounts....

Full description

Saved in:
Bibliographic Details
Published in:Angewandte Chemie International Edition 2019-02, Vol.58 (8), p.2256-2260
Main Authors: Low, Qi Hang, Loo, Nicholas Wei Xian, Calle‐Vallejo, Federico, Yeo, Boon Siang
Format: Article
Language:English
Subjects:
Anthropogenic factors
Carbon cycle
Carbon dioxide
Carbon dioxide emissions
Carbon monoxide
Catalysis
Catalysts
Chemical reduction
Dendrites
electrochemistry
Foams
Human influences
Methanol
Organic chemistry
Silver
silver foam
Zinc
zinc dendrites
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:The electrocatalytic CO2 reduction reaction (CO2RR) can dynamise the carbon cycle by lowering anthropogenic CO2 emissions and sustainably producing valuable fuels and chemical feedstocks. Methanol is arguably the most desirable C1 product of CO2RR, although it typically forms in negligible amounts. In our search for efficient methanol‐producing CO2RR catalysts, we have engineered Ag‐Zn catalysts by pulse‐depositing Zn dendrites onto Ag foams (PD‐Zn/Ag foam). By themselves, Zn and Ag cannot effectively reduce CO2 to CH3OH, while their alloys produce CH3OH with Faradaic efficiencies of approximately 1 %. Interestingly, with nanostructuring PD‐Zn/Ag foam reduces CO2 to CH3OH with Faradaic efficiency and current density values reaching as high as 10.5 % and −2.7 mA cm−2, respectively. Control experiments and DFT calculations pinpoint strained undercoordinated Zn atoms as the active sites for CO2RR to CH3OH in a reaction pathway mediated by adsorbed CO and formaldehyde. Surprisingly, the stability of the *CHO intermediate does not influence the activity. Full Metal Jacket: Zinc dendrites pulse‐deposited on silver foam convert CO2 to CH3OH with a Faradaic efficiency (FE)CH₃OH of 10.5 % and a jCH₃OH of −2.7 mA cm−2 in aqueous solution. Strained, undercoordinated zinc atoms were identified as the active sites in a reaction pathway mediated by adsorbed CO and formaldehyde. Surprisingly, the stability of the *CHO intermediate does not influence the activity.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201810991