{"title":"碳负载耐杂质锰配合物催化自来水电解液选择性还原CO2","authors":"Teppei Nishi*, Naonari Sakamoto, Keita Sekizawa, Satoru Kosaka, Takeshi Morikawa and Shunsuke Sato, ","doi":"10.1021/acsaem.5c01422","DOIUrl":null,"url":null,"abstract":"<p >Electrocatalysts have been developed for reducing CO<sub>2</sub> to value-added chemicals. Although numerous metal catalysts have been reported, trace amounts of impurities such as Fe in the electrolytes deactivate the metal catalysts by deposition of metallic impurities onto their surface, generating the active sites for hydrogen evolution. To address this issue, numerous researchers have developed strategies to sustain catalytic performance. The present work demonstrates that a Mn-complex supported on multiwalled carbon nanotubes can selectively reduce CO<sub>2</sub> in the presence of impurities when a tap water-based electrolyte is used. Even when ionic metals and 15 vol % O<sub>2</sub> are present, our catalyst can selectively reduce CO<sub>2</sub> to CO with a Faraday efficiency of 87% for 12 h. Whereas a Ag electrode was deactivated by metallic impurities in the electrolyte, the Mn-complex exhibited stable performance, presumably because its selective coordination with CO<sub>2</sub> prevented interference from metal ionic impurities. Operando surface enhanced Raman spectroscopy revealed the importance of the coordination properties of a metal complex for selective CO<sub>2</sub> reduction in the presence of ionic impurities.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 15","pages":"11297–11302"},"PeriodicalIF":5.5000,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective CO2 Reduction in Tap-Water Electrolyte Catalyzed by Impurity-Resistant Mn-Complex Supported on Carbon\",\"authors\":\"Teppei Nishi*, Naonari Sakamoto, Keita Sekizawa, Satoru Kosaka, Takeshi Morikawa and Shunsuke Sato, \",\"doi\":\"10.1021/acsaem.5c01422\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Electrocatalysts have been developed for reducing CO<sub>2</sub> to value-added chemicals. Although numerous metal catalysts have been reported, trace amounts of impurities such as Fe in the electrolytes deactivate the metal catalysts by deposition of metallic impurities onto their surface, generating the active sites for hydrogen evolution. To address this issue, numerous researchers have developed strategies to sustain catalytic performance. The present work demonstrates that a Mn-complex supported on multiwalled carbon nanotubes can selectively reduce CO<sub>2</sub> in the presence of impurities when a tap water-based electrolyte is used. Even when ionic metals and 15 vol % O<sub>2</sub> are present, our catalyst can selectively reduce CO<sub>2</sub> to CO with a Faraday efficiency of 87% for 12 h. Whereas a Ag electrode was deactivated by metallic impurities in the electrolyte, the Mn-complex exhibited stable performance, presumably because its selective coordination with CO<sub>2</sub> prevented interference from metal ionic impurities. Operando surface enhanced Raman spectroscopy revealed the importance of the coordination properties of a metal complex for selective CO<sub>2</sub> reduction in the presence of ionic impurities.</p>\",\"PeriodicalId\":4,\"journal\":{\"name\":\"ACS Applied Energy Materials\",\"volume\":\"8 15\",\"pages\":\"11297–11302\"},\"PeriodicalIF\":5.5000,\"publicationDate\":\"2025-07-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsaem.5c01422\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsaem.5c01422","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Selective CO2 Reduction in Tap-Water Electrolyte Catalyzed by Impurity-Resistant Mn-Complex Supported on Carbon
Electrocatalysts have been developed for reducing CO2 to value-added chemicals. Although numerous metal catalysts have been reported, trace amounts of impurities such as Fe in the electrolytes deactivate the metal catalysts by deposition of metallic impurities onto their surface, generating the active sites for hydrogen evolution. To address this issue, numerous researchers have developed strategies to sustain catalytic performance. The present work demonstrates that a Mn-complex supported on multiwalled carbon nanotubes can selectively reduce CO2 in the presence of impurities when a tap water-based electrolyte is used. Even when ionic metals and 15 vol % O2 are present, our catalyst can selectively reduce CO2 to CO with a Faraday efficiency of 87% for 12 h. Whereas a Ag electrode was deactivated by metallic impurities in the electrolyte, the Mn-complex exhibited stable performance, presumably because its selective coordination with CO2 prevented interference from metal ionic impurities. Operando surface enhanced Raman spectroscopy revealed the importance of the coordination properties of a metal complex for selective CO2 reduction in the presence of ionic impurities.
期刊介绍:
ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.