{"title":"环境等离子体催化二氧化碳加氢制甲醇的镍钴双金属界面工程设计","authors":"","doi":"10.1016/j.chempr.2024.06.022","DOIUrl":null,"url":null,"abstract":"<div><p>Plasma catalysis offers a flexible and decentralized solution for CO<sub>2</sub> hydrogenation to methanol under ambient conditions, avoiding the high temperatures and pressures required for thermal catalysis. However, the reaction mechanism, particularly plasma-assisted surface reactions, remains unclear, limiting the development of efficient catalysts for selective methanol synthesis. Here, we report a bimetallic Ni-Co catalyst effective in plasma-catalytic CO<sub>2</sub> hydrogenation to methanol at 35°C and 0.1 MPa, achieving 46% methanol selectivity and 24% CO<sub>2</sub> conversion. <em>In situ</em> plasma-coupled Fourier transform infrared characterization, along with density functional theory calculations, reveals that the engineered bimetallic sites act as primary active centers for methanol synthesis, promoting the rate-determining step in H-radical-induced reaction pathways by reducing steric hindrance effects. This work demonstrates the significant potential of bimetallic catalysts in plasma-catalytic CO<sub>2</sub> hydrogenation to methanol under ambient conditions, representing a major step toward sustainable CO<sub>2</sub> conversion and fuel production.</p></div>","PeriodicalId":268,"journal":{"name":"Chem","volume":null,"pages":null},"PeriodicalIF":19.1000,"publicationDate":"2024-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2451929424003012/pdfft?md5=54d35a2805c07a05ba8a1bec3eed2fcb&pid=1-s2.0-S2451929424003012-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Engineering Ni-Co bimetallic interfaces for ambient plasma-catalytic CO2 hydrogenation to methanol\",\"authors\":\"\",\"doi\":\"10.1016/j.chempr.2024.06.022\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Plasma catalysis offers a flexible and decentralized solution for CO<sub>2</sub> hydrogenation to methanol under ambient conditions, avoiding the high temperatures and pressures required for thermal catalysis. However, the reaction mechanism, particularly plasma-assisted surface reactions, remains unclear, limiting the development of efficient catalysts for selective methanol synthesis. Here, we report a bimetallic Ni-Co catalyst effective in plasma-catalytic CO<sub>2</sub> hydrogenation to methanol at 35°C and 0.1 MPa, achieving 46% methanol selectivity and 24% CO<sub>2</sub> conversion. <em>In situ</em> plasma-coupled Fourier transform infrared characterization, along with density functional theory calculations, reveals that the engineered bimetallic sites act as primary active centers for methanol synthesis, promoting the rate-determining step in H-radical-induced reaction pathways by reducing steric hindrance effects. This work demonstrates the significant potential of bimetallic catalysts in plasma-catalytic CO<sub>2</sub> hydrogenation to methanol under ambient conditions, representing a major step toward sustainable CO<sub>2</sub> conversion and fuel production.</p></div>\",\"PeriodicalId\":268,\"journal\":{\"name\":\"Chem\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":19.1000,\"publicationDate\":\"2024-08-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2451929424003012/pdfft?md5=54d35a2805c07a05ba8a1bec3eed2fcb&pid=1-s2.0-S2451929424003012-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chem\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2451929424003012\",\"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/S2451929424003012","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
等离子体催化为在环境条件下将二氧化碳加氢转化为甲醇提供了灵活、分散的解决方案,避免了热催化所需的高温和高压。然而,反应机理,尤其是等离子体辅助的表面反应仍不清楚,这限制了用于选择性甲醇合成的高效催化剂的开发。在此,我们报告了一种双金属 Ni-Co 催化剂,它能在 35°C 和 0.1 兆帕下有效地进行等离子体催化 CO2 加氢制甲醇,实现 46% 的甲醇选择性和 24% 的 CO2 转化率。原位等离子体耦合傅立叶变换红外表征以及密度泛函理论计算显示,工程化双金属位点可作为甲醇合成的主要活性中心,通过减少立体阻碍效应促进 H-自由基诱导反应途径中的速率决定步骤。这项工作证明了双金属催化剂在环境条件下等离子体催化 CO2 加氢制甲醇方面的巨大潜力,是实现可持续 CO2 转化和燃料生产的重要一步。
Engineering Ni-Co bimetallic interfaces for ambient plasma-catalytic CO2 hydrogenation to methanol
Plasma catalysis offers a flexible and decentralized solution for CO2 hydrogenation to methanol under ambient conditions, avoiding the high temperatures and pressures required for thermal catalysis. However, the reaction mechanism, particularly plasma-assisted surface reactions, remains unclear, limiting the development of efficient catalysts for selective methanol synthesis. Here, we report a bimetallic Ni-Co catalyst effective in plasma-catalytic CO2 hydrogenation to methanol at 35°C and 0.1 MPa, achieving 46% methanol selectivity and 24% CO2 conversion. In situ plasma-coupled Fourier transform infrared characterization, along with density functional theory calculations, reveals that the engineered bimetallic sites act as primary active centers for methanol synthesis, promoting the rate-determining step in H-radical-induced reaction pathways by reducing steric hindrance effects. This work demonstrates the significant potential of bimetallic catalysts in plasma-catalytic CO2 hydrogenation to methanol under ambient conditions, representing a major step toward sustainable CO2 conversion and fuel production.
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.