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Main Title: Electrocatalytic CO2 Reduction on CuOx Nanocubes: Tracking the Evolution of Chemical State, Geometric Structure, and Catalytic Selectivity using Operando Spectroscopy
Author(s): Möller, Tim
Scholten, Fabian
Thanh, Trung Ngo
Sinev, Ilya
Timoshenko, Janis
Wang, Xingli
Jovanov, Zarko
Gliech, Manuel
Roldan Cuenya, Beatriz
Varela, Ana Sofia
Strasser, Peter
Type: Article
Abstract: The direct electrochemical conversion of carbon dioxide (CO2) into multi‐carbon (C2+) products still faces fundamental and technological challenges. While facet‐controlled and oxide‐derived Cu materials have been touted as promising catalysts, their stability has remained problematic and poorly understood. Herein we uncover changes in the chemical and morphological state of supported and unsupported Cu2O nanocubes during operation in low‐current H‐Cells and in high‐current gas diffusion electrodes (GDEs) using neutral pH buffer conditions. While unsupported nanocubes achieved a sustained C2+ Faradaic efficiency of around 60 % for 40 h, the dispersion on a carbon support sharply shifted the selectivity pattern towards C1 products. Operando XAS and time‐resolved electron microscopy revealed the degradation of the cubic shape and, in the presence of a carbon support, the formation of small Cu‐seeds during the surprisingly slow reduction of bulk Cu2O. The initially (100)‐rich facet structure has presumably no controlling role on the catalytic selectivity, whereas the oxide‐derived generation of under‐coordinated lattice defects, can support the high C2+ product yields.
Subject(s): CO2 reduction
operando spectroscopy
Issue Date: 13-Aug-2020
Date Available: 16-Dec-2020
Is Part Of: 10.14279/depositonce-12204
Language Code: en
DDC Class: 540 Chemie und zugeordnete Wissenschaften
Sponsor/Funder: TU Berlin, Open-Access-Mittel – 2020
DFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat"
BMBF, 033RC004E, CO2Plus - Verbundvorhaben: eEthylen - Nutzung elektrischer Energie aus erneuerbaren Quellen zur elektrochemischen Herstellung von Ethylen aus CO2, Teilvorhaben 5: Charakterisierung und Testung für Synthese-Struktur-Wirkungsbeziehungen
BMBF, 03SF0523C, Verbundvorhaben CO2EKAT: Elektrokatalysatorsystem für stoffliche Energiespeicherung durch gekoppelte Wasserelektrolyse und CO2-Umwandlung
EC/H2020/725915/EU/In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects/OPERANDOCAT
Journal Title: Angewandte Chemie International Edition
Publisher: Wiley
Volume: 59
Issue: 41
Publisher DOI: 10.1002/anie.202007136
Page Start: 17974
Page End: 17983
EISSN: 1521-3773
ISSN: 1433-7851
TU Affiliation(s): Fak. 2 Mathematik und Naturwissenschaften » Inst. Chemie » FG Technische Chemie
Appears in Collections:Technische Universität Berlin » Publications

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