Rational Design of Sulfur-Doped Copper Catalysts for the Selective Electroreduction of Carbon Dioxide to Formate
| Autor: | Albertus D. Handoko, Boon Siang Yeo, Yun Huang, Gregory K. L. Goh, Yilin Deng |
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| Rok vydání: | 2017 |
| Předmět: |
Formates
Formic acid General Chemical Engineering Inorganic chemistry chemistry.chemical_element 02 engineering and technology 010402 general chemistry Photochemistry Electrocatalyst 01 natural sciences Catalysis chemistry.chemical_compound Environmental Chemistry General Materials Science Formate Electrodes Polysulfide Electrochemical reduction of carbon dioxide Electrochemical Techniques Carbon Dioxide 021001 nanoscience & nanotechnology Sulfur Copper 0104 chemical sciences General Energy chemistry Microscopy Electron Scanning 0210 nano-technology Oxidation-Reduction |
| Zdroj: | ChemSusChem. 11:320-326 |
| ISSN: | 1864-5631 |
| DOI: | 10.1002/cssc.201701314 |
| Popis: | The selective electroreduction of CO2 to formate (or formic acid) is currently of great interest in the field of renewable energy utilization. In this work, we designed a sulfur-doped Cu2O-derived Cu catalyst, and showed that the presence of sulfur could significantly tune the selectivity of Cu from producing a myriad of CO2 reduction products to almost exclusively formate. Sulfur is doped into the Cu catalysts by dipping the Cu substrates into ammonium polysulfide solutions. Catalyst films with the highest sulfur content of 2.7 atom% showed the largest formate current density (jHCOO-) of -13.9 mA/cm2 at -0.9 V vs. RHE, which is ~46 times larger than that previously reported on Cu(110) surfaces. At -0.8 V vs. RHE, the Faradaic efficiency of formate was maintained at ~75% for 12 h of continuous electrolysis. By analyzing how the jHCOO- and jH2 of the catalysts evolved with different sulfur content, we show that sulfur doping efficaciously increases formate production, while suppressing the hydrogen evolution reaction. Ag-S and Cu-Se catalysts did not exhibit any significant enhancement towards the reduction of CO2 to formate. This demonstrates clearly that sulfur and copper acted synergistically to promote the selective formation of formate. A hypothesis of the role of sulfur is proposed and discussed. |
| Databáze: | OpenAIRE |
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