English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT
  Revealing the CO Coverage Driven C-C Coupling Mechanism for Electrochemical CO2 Reduction on Cu2O Nanocubes via Operando Raman Spectroscopy

Zhan, C., Dattila, F., Rettenmaier, C., Bergmann, A., Kühl, S., García-Muelas, R., et al. (2021). Revealing the CO Coverage Driven C-C Coupling Mechanism for Electrochemical CO2 Reduction on Cu2O Nanocubes via Operando Raman Spectroscopy. ACS Catalysis, 11(13), 7694-7701. doi:10.1021/acscatal.1c01478.

Item is

Basic

show hide
Genre: Journal Article

Files

show Files
hide Files
:
acscatal.1c01478.pdf (Publisher version), 4MB
Name:
acscatal.1c01478.pdf
Description:
-
Visibility:
Public
MIME-Type / Checksum:
application/pdf / [MD5]
Technical Metadata:
Copyright Date:
2021
Copyright Info:
The Author(s)

Locators

show

Creators

show
hide
 Creators:
Zhan, Chao1, Author              
Dattila, Federico2, Author
Rettenmaier, Clara1, Author              
Bergmann, Arno1, Author              
Kühl, Stefanie1, Author              
García-Muelas, Rodrigo2, Author
Lopez, Nuria2, Author
Roldan Cuenya, Beatriz1, Author              
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
2Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST), 43007 Tarragona, Spain, ou_persistent22              

Content

show
hide
Free keywords: -
 Abstract: Electrochemical reduction of carbon dioxide (CO2RR) is an attractive route to close the carbon cycle and potentially turn CO2 into valuable chemicals and fuels. However, the highly selective generation of multicarbon products remains a challenge, suffering from poor mechanistic understanding. Herein, we used operando Raman spectroscopy to track the potential-dependent reduction of Cu2O nanocubes and the surface coverage of reaction intermediates. In particular, we discovered that the potential-dependent intensity ratio of the Cu–CO stretching band to the CO rotation band follows a volcano trend similar to the CO2RR Faradaic efficiency for multicarbon products. By combining operando spectroscopic insights with Density Functional Theory, we proved that this ratio is determined by the CO coverage and that a direct correlation exists between the potential-dependent CO coverage, the preferred C–C coupling configuration, and the selectivity to C2+ products. Thus, operando Raman spectroscopy can serve as an effective method to quantify the coverage of surface intermediates during an electrocatalytic reaction.

Details

show
hide
Language(s): eng - English
 Dates: 2021-03-312021-05-192021-07-02
 Publication Status: Published online
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.1c01478
 Degree: -

Event

show

Legal Case

show

Project information

show hide
Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

Source 1

show
hide
Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: Washington, DC : ACS
Pages: 8 Volume / Issue: 11 (13) Sequence Number: - Start / End Page: 7694 - 7701 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435