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

Lawrence, Matthew J.1; Celorrio, Veronica6; Sargeant, Elizabeth1; Huang, Haoliang2; Rodriguez-Lopez, Joaquin3; Zhu, Yuanmin4,5; Gu, Meng5; Russell, Andrea E.2; Rodriguez, Paramaconi1

2022

10.1021/acsami.1c19298

ACS Applied Materials & Interfaces   影响因子和分区

1944-8244

1944-8252

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.

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

SCI ; EI

英语

其他

China Scholarship Council[201608440295] ; National Natural Science Foundation of China[21802065,12004156] ; Shenzhen Natural Science Fund[20200925154115001,"JCYJ20190809181601639"]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000741059400001

AMER CHEMICAL SOC

20220311468009

Catalyst selectivity ; Coordination reactions ; Copper oxides ; Electrochemistry ; Mass spectrometry ; Nanocatalysts ; Oxidation ; X ray absorption spectroscopy

Nanotechnology:761 ; Chemistry:801 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Atomic and Molecular Physics:931.3

Web of Science

1.Univ Birmingham, Sch Chem, Birmingham B15 2TT, W Midlands, England
2.Univ Southampton, Sch Chem, Southampton SO17 1BJ, Hants, England
3.Univ Illinois, Dept Chem, Urbana, IL 61801 USA
4.Dongguan Univ Technol, Sch Mat Sci & Engn, Dongguan 523808, Peoples R China
5.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
6.Diamond Light Source Ltd, Diamond House, Didcot OX11 0DE, Oxon, England

Lawrence, Matthew J.,Celorrio, Veronica,Sargeant, Elizabeth,et al. 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[J]. ACS Applied Materials & Interfaces,2022,14(2):2742-2753.

Lawrence, Matthew J..,Celorrio, Veronica.,Sargeant, Elizabeth.,Huang, Haoliang.,Rodriguez-Lopez, Joaquin.,...&Rodriguez, Paramaconi.(2022).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.ACS Applied Materials & Interfaces,14(2),2742-2753.

Lawrence, Matthew J.,et al."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".ACS Applied Materials & Interfaces 14.2(2022):2742-2753.