Thomas Freese, Jelmer T. Meijer, Maria B. Brands, Georgios Alachouzos, Marc C. A. Stuart, Rafael Tarozo, Dominic Gerlach, Joost Smits, Petra Rudolf, Joost N. H. Reek and Ben L. Feringa
{"title":"氧化铁促进光化学氧还原成过氧化氢(H2O2)","authors":"Thomas Freese, Jelmer T. Meijer, Maria B. Brands, Georgios Alachouzos, Marc C. A. Stuart, Rafael Tarozo, Dominic Gerlach, Joost Smits, Petra Rudolf, Joost N. H. Reek and Ben L. Feringa","doi":"10.1039/D3EY00256J","DOIUrl":null,"url":null,"abstract":"<p >Hydrogen peroxide (H<small><sub>2</sub></small>O<small><sub>2</sub></small>) is a valuable green oxidant with a wide range of applications. Furthermore, it is recognized as a possible future energy carrier achieving safe operation, storage and transportation. The photochemical production of H<small><sub>2</sub></small>O<small><sub>2</sub></small> serves as a promising alternative to the waste- and energy-intensive anthraquinone process. Following the 12 principles of Green Chemistry, we demonstrate a facile and general approach to sustainable catalyst development utilizing earth-abundant iron and biobased sources only. We developed several iron oxide (FeO<small><sub><em>x</em></sub></small>) nanoparticles (NPs) for successful photochemical oxygen reduction to H<small><sub>2</sub></small>O<small><sub>2</sub></small> under visible light illumination (445 nm). Achieving a selectivity for H<small><sub>2</sub></small>O<small><sub>2</sub></small> of >99%, the catalyst material could be recycled for up to four consecutive rounds. An apparent quantum yield (AQY) of 0.11% was achieved for the photochemical oxygen reduction to H<small><sub>2</sub></small>O<small><sub>2</sub></small> with visible light (445 nm) at ambient temperatures and pressures (9.4–14.8 mmol g<small><sup>−1</sup></small> L<small><sup>−1</sup></small>). Reaching productivities of H<small><sub>2</sub></small>O<small><sub>2</sub></small> of at least 1.7 ± 0.3 mmol g<small><sup>−1</sup></small> L<small><sup>−1</sup></small> h<small><sup>−1</sup></small>, production of H<small><sub>2</sub></small>O<small><sub>2</sub></small> was further possible <em>via</em> sunlight irradiation and in seawater. Finally, a detailed mechanism has been proposed on the basis of experimental investigation of the catalyst's properties and computational results.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2023-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00256j?page=search","citationCount":"0","resultStr":"{\"title\":\"Iron oxide-promoted photochemical oxygen reduction to hydrogen peroxide (H2O2)†\",\"authors\":\"Thomas Freese, Jelmer T. Meijer, Maria B. Brands, Georgios Alachouzos, Marc C. A. Stuart, Rafael Tarozo, Dominic Gerlach, Joost Smits, Petra Rudolf, Joost N. H. Reek and Ben L. Feringa\",\"doi\":\"10.1039/D3EY00256J\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Hydrogen peroxide (H<small><sub>2</sub></small>O<small><sub>2</sub></small>) is a valuable green oxidant with a wide range of applications. Furthermore, it is recognized as a possible future energy carrier achieving safe operation, storage and transportation. The photochemical production of H<small><sub>2</sub></small>O<small><sub>2</sub></small> serves as a promising alternative to the waste- and energy-intensive anthraquinone process. Following the 12 principles of Green Chemistry, we demonstrate a facile and general approach to sustainable catalyst development utilizing earth-abundant iron and biobased sources only. We developed several iron oxide (FeO<small><sub><em>x</em></sub></small>) nanoparticles (NPs) for successful photochemical oxygen reduction to H<small><sub>2</sub></small>O<small><sub>2</sub></small> under visible light illumination (445 nm). Achieving a selectivity for H<small><sub>2</sub></small>O<small><sub>2</sub></small> of >99%, the catalyst material could be recycled for up to four consecutive rounds. An apparent quantum yield (AQY) of 0.11% was achieved for the photochemical oxygen reduction to H<small><sub>2</sub></small>O<small><sub>2</sub></small> with visible light (445 nm) at ambient temperatures and pressures (9.4–14.8 mmol g<small><sup>−1</sup></small> L<small><sup>−1</sup></small>). Reaching productivities of H<small><sub>2</sub></small>O<small><sub>2</sub></small> of at least 1.7 ± 0.3 mmol g<small><sup>−1</sup></small> L<small><sup>−1</sup></small> h<small><sup>−1</sup></small>, production of H<small><sub>2</sub></small>O<small><sub>2</sub></small> was further possible <em>via</em> sunlight irradiation and in seawater. Finally, a detailed mechanism has been proposed on the basis of experimental investigation of the catalyst's properties and computational results.</p>\",\"PeriodicalId\":72877,\"journal\":{\"name\":\"EES catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2023-11-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00256j?page=search\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"EES catalysis\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/ey/d3ey00256j\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"EES catalysis","FirstCategoryId":"1085","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/ey/d3ey00256j","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Iron oxide-promoted photochemical oxygen reduction to hydrogen peroxide (H2O2)†
Hydrogen peroxide (H2O2) is a valuable green oxidant with a wide range of applications. Furthermore, it is recognized as a possible future energy carrier achieving safe operation, storage and transportation. The photochemical production of H2O2 serves as a promising alternative to the waste- and energy-intensive anthraquinone process. Following the 12 principles of Green Chemistry, we demonstrate a facile and general approach to sustainable catalyst development utilizing earth-abundant iron and biobased sources only. We developed several iron oxide (FeOx) nanoparticles (NPs) for successful photochemical oxygen reduction to H2O2 under visible light illumination (445 nm). Achieving a selectivity for H2O2 of >99%, the catalyst material could be recycled for up to four consecutive rounds. An apparent quantum yield (AQY) of 0.11% was achieved for the photochemical oxygen reduction to H2O2 with visible light (445 nm) at ambient temperatures and pressures (9.4–14.8 mmol g−1 L−1). Reaching productivities of H2O2 of at least 1.7 ± 0.3 mmol g−1 L−1 h−1, production of H2O2 was further possible via sunlight irradiation and in seawater. Finally, a detailed mechanism has been proposed on the basis of experimental investigation of the catalyst's properties and computational results.