Yao Chai, Leyi Zhao, Zirui Pang, Liang Wan, Heng Jiang, Chi Chung Tsoi, Yu Du, Huaping Jia, Yujiao Zhu, Detao Liu, Mingjie Li, Fengjia Xie, Guangya Zhou, Xuming Zhang
{"title":"CdS纳米羽毛通过直接电子-质子耦合实现了辅酶NAD(P)H的高效无电子介质光催化再生","authors":"Yao Chai, Leyi Zhao, Zirui Pang, Liang Wan, Heng Jiang, Chi Chung Tsoi, Yu Du, Huaping Jia, Yujiao Zhu, Detao Liu, Mingjie Li, Fengjia Xie, Guangya Zhou, Xuming Zhang","doi":"10.1039/d5ta03036f","DOIUrl":null,"url":null,"abstract":"Photocatalytic regeneration of coenzyme NAD(P)H is essential for energy metabolism and reductive biosynthesis. Traditional systems depend on indirect electron-coupled proton transfer with precious metal-based electron mediators, adding complexity and cost. Here, we demonstrate that CdS nanofeather photocatalysts can achieve visible-light photocatalytic coenzyme NAD(P)H regeneration without electron mediators. Under visible-light irradiation, the NAD+ conversion of the CdS nanofeather photocatalyst reached 66.0% (1h), showing 70.5% selectivity for the physiologically active product 1,4-NADH. When electron mediators are used, the NAD+ conversion is 72.7% (1h). Furthermore, the expansion of substrate types indicates that another coenzyme, NADPH, also can be effectively regenerated without the assistance of an electron mediator. The unique morphology facilitates efficient charge separation and rapid migration, satisfying the electron concentration demands for NAD(P)H regeneration. Mechanistic studies show that the process involves stepwise electron-proton-electron transfer characterized by direct electron-coupled proton transfer. NADH is produced via the pathway NAD+ → NAD• → enol-NADH•+ → enol-NADH → 1,4-NADH, fundamentally differing from the indirect electron transfer mechanism that relies on electron mediators. This work introduces visible-light photocatalytic coenzyme NAD(P)H regeneration without electron mediators, achieving competitive conversion.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"12 1","pages":""},"PeriodicalIF":10.7000,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"CdS nanofeathers enable efficient electron-mediator-free photocatalytic regeneration of coenzyme NAD(P)H via direct electron-proton coupling\",\"authors\":\"Yao Chai, Leyi Zhao, Zirui Pang, Liang Wan, Heng Jiang, Chi Chung Tsoi, Yu Du, Huaping Jia, Yujiao Zhu, Detao Liu, Mingjie Li, Fengjia Xie, Guangya Zhou, Xuming Zhang\",\"doi\":\"10.1039/d5ta03036f\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Photocatalytic regeneration of coenzyme NAD(P)H is essential for energy metabolism and reductive biosynthesis. Traditional systems depend on indirect electron-coupled proton transfer with precious metal-based electron mediators, adding complexity and cost. Here, we demonstrate that CdS nanofeather photocatalysts can achieve visible-light photocatalytic coenzyme NAD(P)H regeneration without electron mediators. Under visible-light irradiation, the NAD+ conversion of the CdS nanofeather photocatalyst reached 66.0% (1h), showing 70.5% selectivity for the physiologically active product 1,4-NADH. When electron mediators are used, the NAD+ conversion is 72.7% (1h). Furthermore, the expansion of substrate types indicates that another coenzyme, NADPH, also can be effectively regenerated without the assistance of an electron mediator. The unique morphology facilitates efficient charge separation and rapid migration, satisfying the electron concentration demands for NAD(P)H regeneration. Mechanistic studies show that the process involves stepwise electron-proton-electron transfer characterized by direct electron-coupled proton transfer. NADH is produced via the pathway NAD+ → NAD• → enol-NADH•+ → enol-NADH → 1,4-NADH, fundamentally differing from the indirect electron transfer mechanism that relies on electron mediators. This work introduces visible-light photocatalytic coenzyme NAD(P)H regeneration without electron mediators, achieving competitive conversion.\",\"PeriodicalId\":82,\"journal\":{\"name\":\"Journal of Materials Chemistry A\",\"volume\":\"12 1\",\"pages\":\"\"},\"PeriodicalIF\":10.7000,\"publicationDate\":\"2025-07-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Materials Chemistry A\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d5ta03036f\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d5ta03036f","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
CdS nanofeathers enable efficient electron-mediator-free photocatalytic regeneration of coenzyme NAD(P)H via direct electron-proton coupling
Photocatalytic regeneration of coenzyme NAD(P)H is essential for energy metabolism and reductive biosynthesis. Traditional systems depend on indirect electron-coupled proton transfer with precious metal-based electron mediators, adding complexity and cost. Here, we demonstrate that CdS nanofeather photocatalysts can achieve visible-light photocatalytic coenzyme NAD(P)H regeneration without electron mediators. Under visible-light irradiation, the NAD+ conversion of the CdS nanofeather photocatalyst reached 66.0% (1h), showing 70.5% selectivity for the physiologically active product 1,4-NADH. When electron mediators are used, the NAD+ conversion is 72.7% (1h). Furthermore, the expansion of substrate types indicates that another coenzyme, NADPH, also can be effectively regenerated without the assistance of an electron mediator. The unique morphology facilitates efficient charge separation and rapid migration, satisfying the electron concentration demands for NAD(P)H regeneration. Mechanistic studies show that the process involves stepwise electron-proton-electron transfer characterized by direct electron-coupled proton transfer. NADH is produced via the pathway NAD+ → NAD• → enol-NADH•+ → enol-NADH → 1,4-NADH, fundamentally differing from the indirect electron transfer mechanism that relies on electron mediators. This work introduces visible-light photocatalytic coenzyme NAD(P)H regeneration without electron mediators, achieving competitive conversion.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.