{"title":"利用纳米级电化反应实现选择性氢化催化","authors":"Mengfei Qiao , Qingyuan Wu , Ying Wang , Shanshan Gao , Ruixuan Qin , Shengjie Liu , Kehong Ding , Dongyuan Zhao , Nanfeng Zheng","doi":"10.1016/j.chempr.2024.06.030","DOIUrl":null,"url":null,"abstract":"<div><div><span>By mimicking nanoscale galvanic reactions, this study focuses on optimizing catalytic hydrogenation by introducing two spatially separated sites for the activation of H</span><sub>2</sub> into proton and electron pairs and the selective reduction of –NO<sub>2</sub>. The catalyst system is designed with the co-deposition of Pt and Fe<sub>2</sub>O<sub>3</sub><span><span> nanoparticles on conductive </span>carbon nanotubes<span>, establishing an electron-transferring pathway. Protic solvents facilitate proton transport. Upon activation of H</span></span><sub>2</sub> molecules into proton and electron pairs on Pt, modified with ammonia or amines, these active species are efficiently transferred to Fe<sub>2</sub>O<sub>3</sub><span> nanoparticles for the selective reduction of –NO</span><sub>2</sub> into amines without affecting other functional groups. Compared with Pt/CNT, which easily hydrogenates both C=C and –NO<sub>2</sub> groups of 4-nitrostyrene, the Pt&Fe<sub>2</sub>O<sub>3</sub>/CNT catalyst modified by NH<sub>3</sub> exhibits higher activity and selectivity for –NO<sub>2</sub><span> hydrogenation. Electrochemically, Pt functions as the anode for the hydrogen oxidation reaction, while Fe</span><sub>2</sub>O<sub>3</sub> acts as the cathode, selectively reducing –NO<sub>2</sub>.</div></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":"10 11","pages":"Pages 3385-3395"},"PeriodicalIF":19.1000,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective hydrogenation catalysis enabled by nanoscale galvanic reactions\",\"authors\":\"Mengfei Qiao , Qingyuan Wu , Ying Wang , Shanshan Gao , Ruixuan Qin , Shengjie Liu , Kehong Ding , Dongyuan Zhao , Nanfeng Zheng\",\"doi\":\"10.1016/j.chempr.2024.06.030\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div><span>By mimicking nanoscale galvanic reactions, this study focuses on optimizing catalytic hydrogenation by introducing two spatially separated sites for the activation of H</span><sub>2</sub> into proton and electron pairs and the selective reduction of –NO<sub>2</sub>. The catalyst system is designed with the co-deposition of Pt and Fe<sub>2</sub>O<sub>3</sub><span><span> nanoparticles on conductive </span>carbon nanotubes<span>, establishing an electron-transferring pathway. Protic solvents facilitate proton transport. Upon activation of H</span></span><sub>2</sub> molecules into proton and electron pairs on Pt, modified with ammonia or amines, these active species are efficiently transferred to Fe<sub>2</sub>O<sub>3</sub><span> nanoparticles for the selective reduction of –NO</span><sub>2</sub> into amines without affecting other functional groups. Compared with Pt/CNT, which easily hydrogenates both C=C and –NO<sub>2</sub> groups of 4-nitrostyrene, the Pt&Fe<sub>2</sub>O<sub>3</sub>/CNT catalyst modified by NH<sub>3</sub> exhibits higher activity and selectivity for –NO<sub>2</sub><span> hydrogenation. Electrochemically, Pt functions as the anode for the hydrogen oxidation reaction, while Fe</span><sub>2</sub>O<sub>3</sub> acts as the cathode, selectively reducing –NO<sub>2</sub>.</div></div>\",\"PeriodicalId\":268,\"journal\":{\"name\":\"Chem\",\"volume\":\"10 11\",\"pages\":\"Pages 3385-3395\"},\"PeriodicalIF\":19.1000,\"publicationDate\":\"2024-11-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chem\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2451929424003097\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chem","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2451929424003097","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Selective hydrogenation catalysis enabled by nanoscale galvanic reactions
By mimicking nanoscale galvanic reactions, this study focuses on optimizing catalytic hydrogenation by introducing two spatially separated sites for the activation of H2 into proton and electron pairs and the selective reduction of –NO2. The catalyst system is designed with the co-deposition of Pt and Fe2O3 nanoparticles on conductive carbon nanotubes, establishing an electron-transferring pathway. Protic solvents facilitate proton transport. Upon activation of H2 molecules into proton and electron pairs on Pt, modified with ammonia or amines, these active species are efficiently transferred to Fe2O3 nanoparticles for the selective reduction of –NO2 into amines without affecting other functional groups. Compared with Pt/CNT, which easily hydrogenates both C=C and –NO2 groups of 4-nitrostyrene, the Pt&Fe2O3/CNT catalyst modified by NH3 exhibits higher activity and selectivity for –NO2 hydrogenation. Electrochemically, Pt functions as the anode for the hydrogen oxidation reaction, while Fe2O3 acts as the cathode, selectively reducing –NO2.
期刊介绍:
Chem, affiliated with Cell as its sister journal, serves as a platform for groundbreaking research and illustrates how fundamental inquiries in chemistry and its related fields can contribute to addressing future global challenges. It was established in 2016, and is currently edited by Robert Eagling.