{"title":"提高NiS-Zn3In2S6/Bi2S3的载流子密度和空间解耦效率,促进胺的光催化无受体脱氢","authors":"Yuanqiao Wei , Ruifang Zhang , Wei Gao , Ningzhao Shang , Xiang Cheng , Yongjun Gao , Xin Zhou , Chun Wang , Shutao Gao","doi":"10.1016/j.apsusc.2025.163325","DOIUrl":null,"url":null,"abstract":"<div><div>Photocatalytic Acceptorless Dehydrogenation (PAD) of amines to hydrogen (H<sub>2</sub>) and imines is a promising approach to produce clean energy and high-value added chemicals. However, the poor charge carrier separation performance of photocatalyst and uncontrolled side reaction, including the imines hydrogenated and C<img>C coupling, significantly hindered its development. Herein, we developed a heterojunction photocatalyst NiS-Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub>/Bi<sub>2</sub>S<sub>3</sub> (Ni-ZIS/Bi) for boosting the PAD reaction of benzylamine. Due to the enhanced density and spatial decoupling effectiveness of photogenerated charge carriers, Ni<sub>0.5%</sub>-ZIS/Bi<sub>1.2%</sub> exhibits 12.4-fold and 5.9-fold increase in production rate of H<sub>2</sub> and N-benzylidenebenzylamine (NBBA), respectively, compared with Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub>. Notably, the selectivity of NBBA increased from 28.5 % of Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub> to 98 % of NiS<sub>0.5%</sub>-ZIS/Bi<sub>1.2%</sub>. This study offers novel insight into the cooperative coupling of H<sub>2</sub> production with organic transformation processes.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"702 ","pages":"Article 163325"},"PeriodicalIF":6.3000,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing charge carrier density and spatial decoupling effectiveness of NiS-Zn3In2S6/Bi2S3 for boosting photocatalytic acceptorlessdehydrogenation of amines\",\"authors\":\"Yuanqiao Wei , Ruifang Zhang , Wei Gao , Ningzhao Shang , Xiang Cheng , Yongjun Gao , Xin Zhou , Chun Wang , Shutao Gao\",\"doi\":\"10.1016/j.apsusc.2025.163325\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Photocatalytic Acceptorless Dehydrogenation (PAD) of amines to hydrogen (H<sub>2</sub>) and imines is a promising approach to produce clean energy and high-value added chemicals. However, the poor charge carrier separation performance of photocatalyst and uncontrolled side reaction, including the imines hydrogenated and C<img>C coupling, significantly hindered its development. Herein, we developed a heterojunction photocatalyst NiS-Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub>/Bi<sub>2</sub>S<sub>3</sub> (Ni-ZIS/Bi) for boosting the PAD reaction of benzylamine. Due to the enhanced density and spatial decoupling effectiveness of photogenerated charge carriers, Ni<sub>0.5%</sub>-ZIS/Bi<sub>1.2%</sub> exhibits 12.4-fold and 5.9-fold increase in production rate of H<sub>2</sub> and N-benzylidenebenzylamine (NBBA), respectively, compared with Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub>. Notably, the selectivity of NBBA increased from 28.5 % of Zn<sub>3</sub>In<sub>2</sub>S<sub>6</sub> to 98 % of NiS<sub>0.5%</sub>-ZIS/Bi<sub>1.2%</sub>. This study offers novel insight into the cooperative coupling of H<sub>2</sub> production with organic transformation processes.</div></div>\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":\"702 \",\"pages\":\"Article 163325\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2025-04-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0169433225010396\",\"RegionNum\":2,\"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":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0169433225010396","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Enhancing charge carrier density and spatial decoupling effectiveness of NiS-Zn3In2S6/Bi2S3 for boosting photocatalytic acceptorlessdehydrogenation of amines
Photocatalytic Acceptorless Dehydrogenation (PAD) of amines to hydrogen (H2) and imines is a promising approach to produce clean energy and high-value added chemicals. However, the poor charge carrier separation performance of photocatalyst and uncontrolled side reaction, including the imines hydrogenated and CC coupling, significantly hindered its development. Herein, we developed a heterojunction photocatalyst NiS-Zn3In2S6/Bi2S3 (Ni-ZIS/Bi) for boosting the PAD reaction of benzylamine. Due to the enhanced density and spatial decoupling effectiveness of photogenerated charge carriers, Ni0.5%-ZIS/Bi1.2% exhibits 12.4-fold and 5.9-fold increase in production rate of H2 and N-benzylidenebenzylamine (NBBA), respectively, compared with Zn3In2S6. Notably, the selectivity of NBBA increased from 28.5 % of Zn3In2S6 to 98 % of NiS0.5%-ZIS/Bi1.2%. This study offers novel insight into the cooperative coupling of H2 production with organic transformation processes.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.