高选择性和稳定性SnO_2纳米催_省略_CO_2电化学还原为甲酸_英文_付奕舒.docVIP

available at 催journal homepage: /locate/chnjc Article (Special Issue on Electrocatalysis Transformation) Electrochemical CO2 reduction to formic acid on crystalline SnO2 nanosphere catalyst with high selectivity and stability Yishu Fu a, Yanan Li a, Xia Zhang a, Yuyu liu b,c,#, Xiaodong Zhou d, Jinli Qiao a,* ab College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China c Graduate School of Environmental Studies, Tohoku University, Sendai 980-8579, Japan d Department of Chemical Engineering, University of South Carolina, Columbia, SC 29208, USA Article history: Received 18 December 2015 Accepted 27 January 2016 Keywords: Carbon dioxide reduction Tin dioxide Formate Faradaic efficiency 1. Introduction A novel catalyst for CO2 electroreduction based on nanostructured SnO2 was synthesized using a facile hydrothermal self-assembly method. The electrochemical activity showed that the catalyst gave outstanding catalytic activity and selectivity in CO2 electroreduction. The catalytic activity and formate selectivity depended strongly on the electrolyte conditions. A high faradaic efficiency, i.e., 56%, was achieved for formate formation in KHCO3 (0.5 mol/L). This is attributed to control of formate production by mass and charge transfer processes. Electrolysis experiments using SnO2-50/GDE (an SnO2-based gas-diffusion electrode, where 50 indicates the 50% ethanol content of the electrolyte) as the catalyst, showed that the electrolyte pH also affected CO2 reduction. The optimum electrolyte pH for obtaining a high faradaic efficiency for formate production was 8.3. This is mainly because a neutral or mildly alkaline environment maintains the oxide stability. The fara-daic efficiency for formate production declined with time. X-ray photoelectron spectroscopy showed that this is the result of deposition of trace amounts of fluo