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Exfoliated 2D Layered and Nonlayered Metal Phosphorous Trichalcogenides Nanosheets as Promising Electrocatalysts for CO2 Reduction
Authors:Honglei Wang  Dr Yunfei Jiao  Bing Wu  Dr Dong Wang  Yueqi Hu  Prof?Dr Fei Liang  Dr Chen Shen  Dr Andrea Knauer  Prof?Dr Dan Ren  Dr Hongguang Wang  Prof?Dr Peter A van Aken  Prof?Dr Hongbin Zhang  Prof?Dr Zdenek Sofer  Prof?Dr Michael Grätzel  Prof?Dr Peter Schaaf
Institution:1. Chair Materials for Electrical Engineering and Electronics, Institute of Materials Science and Engineering and Institute of Micro and Nanotechnologies MacroNano, TU Ilmenau, Gustav-Kirchhoff-Str. 5, 98693 Ilmenau, Germany;2. Laboratory of Photonics and Interfaces, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland;3. Department of Inorganic Chemistry, University of Chemistry and Technology Prague, Technická 5, 166 28 Prague 6, Czech Republic;4. Institut für Materialwissenschaft, Technische Universität Darmstadt, 64289 Darmstadt, Germany;5. Institute of Micro- and Nanotechnologies MacroNano®, TU Ilmenau, Gustav-Kirchhoff- Str.7, 98693 Ilmenau, Germany;6. Max Planck Institute for Solid State Research, Heisenbergstr. 1, 70569 Stuttgart, Germany
Abstract:Two-dimensional (2D) materials catalysts provide an atomic-scale view on a fascinating arena for understanding the mechanism of electrocatalytic carbon dioxide reduction (CO2 ECR). Here, we successfully exfoliated both layered and nonlayered ultra-thin metal phosphorous trichalcogenides (MPCh3) nanosheets via wet grinding exfoliation (WGE), and systematically investigated the mechanism of MPCh3 as catalysts for CO2 ECR. Unlike the layered CoPS3 and NiPS3 nanosheets, the active Sn atoms tend to be exposed on the surfaces of nonlayered SnPS3 nanosheets. Correspondingly, the nonlayered SnPS3 nanosheets exhibit clearly improved catalytic activity, showing formic acid selectivity up to 31.6 % with ?7.51 mA cm?2 at ?0.65 V vs. RHE. The enhanced catalytic performance can be attributed to the formation of HCOO* via the first proton-electron pair addition on the SnPS3 surface. These results provide a new avenue to understand the novel CO2 ECR mechanism of Sn-based and MPCh3-based catalysts.
Keywords:2D Materials  CO2 ECR  Exfoliation  MPCh3 Nanosheets  Nonlayered
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