Ang Li, Huiying Qiu, Zhaohui Wang, Yanzhi Sun, Yang Tang, Pingyu Wan, Haomin Jiang* and Yongmei Chen*,
{"title":"在水性电解质中通过促进 -OH 生成电催化将甲烷转化为乙醇","authors":"Ang Li, Huiying Qiu, Zhaohui Wang, Yanzhi Sun, Yang Tang, Pingyu Wan, Haomin Jiang* and Yongmei Chen*, ","doi":"10.1021/acssuschemeng.4c03759","DOIUrl":null,"url":null,"abstract":"<p >Converting methane (CH<sub>4</sub>), the greenhouse gas, into high-value liquid oxygenates by an electrochemical method under mild conditions is a desired technology for establishing an energy- and environment-sustainable society. However, challenges from the competition of the oxygen evolution reaction and selectivity of the desired products still exist. Here we report the catalytic performance of Cu<sub>2</sub>O/CuO for electrochemical conversion of methane into ethanol (CH<sub>3</sub>CH<sub>2</sub>OH). Density functional theory calculations demonstrated that the Cu<sub>2</sub>O/CuO interface enables efficient CH<sub>4</sub> adsorption, which provides an effective pathway for methane utilization under mild conditions. Based on electrochemical studies and electron paramagnetic resonance (EPR) measurement results, it is confirmed that the activated CH<sub>4</sub> is converted to CH<sub>3</sub>CH<sub>2</sub>OH by reaction with active oxygen species (<sup>•</sup>OH radicals) electrogenerated <i>in situ</i> through the water oxidation reaction over Cu<sub>2</sub>O/CuO on the anode. Under the optimized conditions, a Faraday efficiency (FE) of 21.1% and a production rate of 126.7 μmol g<sub>cat</sub><sup>–1</sup> h<sup>–1</sup> at ambient pressure for CH<sub>3</sub>CH<sub>2</sub>OH production were obtained, and the FE remained ∼19.0% at 2.2 V cell voltage during 8 h of electrolysis. When the pressure in the bath was lifted to 4.0 bar, the production rate of 441.3 μmol g<sub>cat</sub><sup>–1</sup> h<sup>–1</sup> with an FE of 69.2% was obtained due to the higher solubility of CH<sub>4</sub> in aqueous solution.</p>","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":7.1000,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electrocatalytic Conversion of Methane to Ethanol via Promoted •OH Generation in Aqueous Electrolyte\",\"authors\":\"Ang Li, Huiying Qiu, Zhaohui Wang, Yanzhi Sun, Yang Tang, Pingyu Wan, Haomin Jiang* and Yongmei Chen*, \",\"doi\":\"10.1021/acssuschemeng.4c03759\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Converting methane (CH<sub>4</sub>), the greenhouse gas, into high-value liquid oxygenates by an electrochemical method under mild conditions is a desired technology for establishing an energy- and environment-sustainable society. However, challenges from the competition of the oxygen evolution reaction and selectivity of the desired products still exist. Here we report the catalytic performance of Cu<sub>2</sub>O/CuO for electrochemical conversion of methane into ethanol (CH<sub>3</sub>CH<sub>2</sub>OH). Density functional theory calculations demonstrated that the Cu<sub>2</sub>O/CuO interface enables efficient CH<sub>4</sub> adsorption, which provides an effective pathway for methane utilization under mild conditions. Based on electrochemical studies and electron paramagnetic resonance (EPR) measurement results, it is confirmed that the activated CH<sub>4</sub> is converted to CH<sub>3</sub>CH<sub>2</sub>OH by reaction with active oxygen species (<sup>•</sup>OH radicals) electrogenerated <i>in situ</i> through the water oxidation reaction over Cu<sub>2</sub>O/CuO on the anode. Under the optimized conditions, a Faraday efficiency (FE) of 21.1% and a production rate of 126.7 μmol g<sub>cat</sub><sup>–1</sup> h<sup>–1</sup> at ambient pressure for CH<sub>3</sub>CH<sub>2</sub>OH production were obtained, and the FE remained ∼19.0% at 2.2 V cell voltage during 8 h of electrolysis. When the pressure in the bath was lifted to 4.0 bar, the production rate of 441.3 μmol g<sub>cat</sub><sup>–1</sup> h<sup>–1</sup> with an FE of 69.2% was obtained due to the higher solubility of CH<sub>4</sub> in aqueous solution.</p>\",\"PeriodicalId\":25,\"journal\":{\"name\":\"ACS Sustainable Chemistry & Engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.1000,\"publicationDate\":\"2024-06-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sustainable Chemistry & Engineering\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acssuschemeng.4c03759\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sustainable Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acssuschemeng.4c03759","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Electrocatalytic Conversion of Methane to Ethanol via Promoted •OH Generation in Aqueous Electrolyte
Converting methane (CH4), the greenhouse gas, into high-value liquid oxygenates by an electrochemical method under mild conditions is a desired technology for establishing an energy- and environment-sustainable society. However, challenges from the competition of the oxygen evolution reaction and selectivity of the desired products still exist. Here we report the catalytic performance of Cu2O/CuO for electrochemical conversion of methane into ethanol (CH3CH2OH). Density functional theory calculations demonstrated that the Cu2O/CuO interface enables efficient CH4 adsorption, which provides an effective pathway for methane utilization under mild conditions. Based on electrochemical studies and electron paramagnetic resonance (EPR) measurement results, it is confirmed that the activated CH4 is converted to CH3CH2OH by reaction with active oxygen species (•OH radicals) electrogenerated in situ through the water oxidation reaction over Cu2O/CuO on the anode. Under the optimized conditions, a Faraday efficiency (FE) of 21.1% and a production rate of 126.7 μmol gcat–1 h–1 at ambient pressure for CH3CH2OH production were obtained, and the FE remained ∼19.0% at 2.2 V cell voltage during 8 h of electrolysis. When the pressure in the bath was lifted to 4.0 bar, the production rate of 441.3 μmol gcat–1 h–1 with an FE of 69.2% was obtained due to the higher solubility of CH4 in aqueous solution.
期刊介绍:
ACS Sustainable Chemistry & Engineering is a prestigious weekly peer-reviewed scientific journal published by the American Chemical Society. Dedicated to advancing the principles of green chemistry and green engineering, it covers a wide array of research topics including green chemistry, green engineering, biomass, alternative energy, and life cycle assessment.
The journal welcomes submissions in various formats, including Letters, Articles, Features, and Perspectives (Reviews), that address the challenges of sustainability in the chemical enterprise and contribute to the advancement of sustainable practices. Join us in shaping the future of sustainable chemistry and engineering.