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Insight into the activity and selectivity of nanostructured copper titanates during electrochemical conversion of CO2 at neutral pH via in situ X-ray Absorption Spectroscopy

DOI: 10.1021/acsami.1c19298 DOI Help

Authors: Matthew J. Lawrence (University of Birmingham) , Veronica Celorrio (University of Bristol) , Elizabeth Sargeant (University of Birmingham) , Haoliang Huang (University of Southampton) , Joaquín Rodríguez-López (University of Illinois Urbana−Champaign) , Yuanmin Zhu (Dongguan University of Technology; Southern University of Science and Technology) , Meng Gu (Southern University of Science and Technology) , Andrea E. Russell (University of Southampton) , Paramaconi Rodriguez (University of Birmingham)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Applied Materials & Interfaces

State: Published (Approved)
Published: January 2022
Diamond Proposal Number(s): 21533

Open Access Open Access

Abstract: The electrochemical conversion of carbon dioxide (CO2) to useful chemical fuels is a promising route toward the achievement of carbon neutral and carbon negative energy technologies. Copper (Cu)- and Cu oxide-derived surfaces are known to electrochemically convert CO2 to high-value and energy-dense products. However, the nature and stability of oxidized Cu species under reaction conditions are the subject of much debate in the literature. Herein, we present the synthesis and characterization of copper-titanate nanocatalysts, with discrete Cu–O coordination environments, for the electrochemical CO2 reduction reaction (CO2RR). We employ real-time in situ X-ray absorption spectroscopy (XAS) to monitor Cu species under neutral-pH CO2RR conditions. Combination of voltammetry and on-line electrochemical mass spectrometry with XAS results demonstrates that the titanate motif promotes the retention of oxidized Cu species under reducing conditions for extended periods, without itself possessing any CO2RR activity. Additionally, we demonstrate that the specific nature of the Cu–O environment and the size of the catalyst dictate the long-term stability of the oxidized Cu species and, subsequently, the product selectivity.

Journal Keywords: CO2 reduction reaction (CO2RR); metal intercalation; layered structures; electrochemistry; copper catalyst; in situ XAS

Diamond Keywords: Carbon Capture and Storage (CCS)

Subject Areas: Chemistry, Materials, Environment

Instruments: B18-Core EXAFS

Added On: 05/01/2022 15:17


Discipline Tags:

Earth Sciences & Environment Climate Change Physical Chemistry Catalysis Chemistry Materials Science Nanoscience/Nanotechnology

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)