{"title":"喷雾干燥法制备碳负载Cu催化剂的研究","authors":"Lili Yang, Jinghao Lu, Chao Wang, Lianying Zhang, Chuanhui Zhang, Xingyun Li, Hongliang Li, Xiu Song Zhao","doi":"10.1016/j.mcat.2025.115162","DOIUrl":null,"url":null,"abstract":"<div><div>Electrocatalytic carbon dioxide (CO<sub>2</sub>) reduction is an appealing option that offers advantages of converting greenhouse gas CO<sub>2</sub> into value-added hydrocarbon products while storing green energy. Copper (Cu) is a unique catalyst that has adequate ability for adsorption and activation of CO<sub>2</sub>, as well as important intermediate species for forming multi-carbon (C<sub>2+</sub>) products. In particular, monovalent Cu(I) is deemed to be responsible for C-C coupling to form C<sub>2+</sub> products. However, oxidation state copper species are unstable under the CO<sub>2</sub> electrolysis conditions, tending to be reduced along with surface reconstruction. It is therefore important to develop a robust catalyst synthesis method to enhance the stability of Cu-based catalysts. Here, we demonstrate a spray-drying method for the synthesis of carbon-supported Cu catalysts for the electrocatalytic CO<sub>2</sub> reduction reaction. This method is scalable and cost-effective, allowing one to realize mass production of carbon-supported Cu catalysts. A catalyst sample thus synthesized exhibits a Faraday efficiency of C<sub>2</sub> products (e.g., ethylene, ethanol and acetic acid) as high as 85.8 %. <em>In-situ</em> attenuated total reflection-surface-enhanced infrared absorption spectroscopy and surface-enhanced Raman spectroscopy characterization results reveal that the porous carbon support stabilizes Cu<sub>2</sub>O/CuO nanoparticles, facilitate CO<sub>2</sub> adsorption, enrich local important intermediates for the C-C coupling reaction.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"582 ","pages":"Article 115162"},"PeriodicalIF":4.9000,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Spray drying synthesis of stable Cu catalyst supported on carbon with high C2 product selectivity in CO2 electrolysis\",\"authors\":\"Lili Yang, Jinghao Lu, Chao Wang, Lianying Zhang, Chuanhui Zhang, Xingyun Li, Hongliang Li, Xiu Song Zhao\",\"doi\":\"10.1016/j.mcat.2025.115162\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Electrocatalytic carbon dioxide (CO<sub>2</sub>) reduction is an appealing option that offers advantages of converting greenhouse gas CO<sub>2</sub> into value-added hydrocarbon products while storing green energy. Copper (Cu) is a unique catalyst that has adequate ability for adsorption and activation of CO<sub>2</sub>, as well as important intermediate species for forming multi-carbon (C<sub>2+</sub>) products. In particular, monovalent Cu(I) is deemed to be responsible for C-C coupling to form C<sub>2+</sub> products. However, oxidation state copper species are unstable under the CO<sub>2</sub> electrolysis conditions, tending to be reduced along with surface reconstruction. It is therefore important to develop a robust catalyst synthesis method to enhance the stability of Cu-based catalysts. Here, we demonstrate a spray-drying method for the synthesis of carbon-supported Cu catalysts for the electrocatalytic CO<sub>2</sub> reduction reaction. This method is scalable and cost-effective, allowing one to realize mass production of carbon-supported Cu catalysts. A catalyst sample thus synthesized exhibits a Faraday efficiency of C<sub>2</sub> products (e.g., ethylene, ethanol and acetic acid) as high as 85.8 %. <em>In-situ</em> attenuated total reflection-surface-enhanced infrared absorption spectroscopy and surface-enhanced Raman spectroscopy characterization results reveal that the porous carbon support stabilizes Cu<sub>2</sub>O/CuO nanoparticles, facilitate CO<sub>2</sub> adsorption, enrich local important intermediates for the C-C coupling reaction.</div></div>\",\"PeriodicalId\":393,\"journal\":{\"name\":\"Molecular Catalysis\",\"volume\":\"582 \",\"pages\":\"Article 115162\"},\"PeriodicalIF\":4.9000,\"publicationDate\":\"2025-05-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Molecular Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468823125003475\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823125003475","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Spray drying synthesis of stable Cu catalyst supported on carbon with high C2 product selectivity in CO2 electrolysis
Electrocatalytic carbon dioxide (CO2) reduction is an appealing option that offers advantages of converting greenhouse gas CO2 into value-added hydrocarbon products while storing green energy. Copper (Cu) is a unique catalyst that has adequate ability for adsorption and activation of CO2, as well as important intermediate species for forming multi-carbon (C2+) products. In particular, monovalent Cu(I) is deemed to be responsible for C-C coupling to form C2+ products. However, oxidation state copper species are unstable under the CO2 electrolysis conditions, tending to be reduced along with surface reconstruction. It is therefore important to develop a robust catalyst synthesis method to enhance the stability of Cu-based catalysts. Here, we demonstrate a spray-drying method for the synthesis of carbon-supported Cu catalysts for the electrocatalytic CO2 reduction reaction. This method is scalable and cost-effective, allowing one to realize mass production of carbon-supported Cu catalysts. A catalyst sample thus synthesized exhibits a Faraday efficiency of C2 products (e.g., ethylene, ethanol and acetic acid) as high as 85.8 %. In-situ attenuated total reflection-surface-enhanced infrared absorption spectroscopy and surface-enhanced Raman spectroscopy characterization results reveal that the porous carbon support stabilizes Cu2O/CuO nanoparticles, facilitate CO2 adsorption, enrich local important intermediates for the C-C coupling reaction.
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods