Sirlon F. Blaskievicz, Ivo F. Teixeira, Lucia H. Mascaro, Mariolino Carta, Neil B. McKeown, Yuanzhu Zhao, Frank Marken
{"title":"镍修饰聚七嗪酰亚胺氢介导的光电催化","authors":"Sirlon F. Blaskievicz, Ivo F. Teixeira, Lucia H. Mascaro, Mariolino Carta, Neil B. McKeown, Yuanzhu Zhao, Frank Marken","doi":"10.1007/s12678-023-00852-9","DOIUrl":null,"url":null,"abstract":"Abstract Polymeric carbon nitrides (C 3 N 4 ) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":null,"pages":null},"PeriodicalIF":2.7000,"publicationDate":"2023-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)\",\"authors\":\"Sirlon F. Blaskievicz, Ivo F. Teixeira, Lucia H. Mascaro, Mariolino Carta, Neil B. McKeown, Yuanzhu Zhao, Frank Marken\",\"doi\":\"10.1007/s12678-023-00852-9\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Abstract Polymeric carbon nitrides (C 3 N 4 ) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract\",\"PeriodicalId\":535,\"journal\":{\"name\":\"Electrocatalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.7000,\"publicationDate\":\"2023-11-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Electrocatalysis\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1007/s12678-023-00852-9\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Electrocatalysis","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1007/s12678-023-00852-9","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Hydrogen-Mediated Photoelectrocatalysis with Nickel-Modified Poly(Heptazine Imides)
Abstract Polymeric carbon nitrides (C 3 N 4 ) are photochemically active organic semiconductors that can be produced in a wide range of structural types. Here, a poly-(heptazine imide) containing nickel single atoms (Ni-PHI) is employed for photochemical hydrogen production and is compared to the non-nickel-doped semiconductor. Film deposits are formed on a platinum disk electrode (to detect hydrogen) and a coating of the molecularly rigid polymer of intrinsic microporosity PIM-1 is applied to (i) mechanically stabilize the photo-catalyst film without impeding photocatalysis and (ii) assist in the interfacial hydrogen capture/oxygen suppression process. In the presence of hole quenchers such as methanol or ethanol, anodic photocurrents linked to hydrogen production/oxidation are observed. A comparison with an experiment on glassy carbon confirms the formation of interfacial hydrogen as a mediator. The effects of hole quencher concentration are evaluated. The system Pt/Ni-PHI/PIM-1 is employed in a single-compartment photo-fuel cell. Graphical Abstract
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