Haisheng Wei, Jing Li, Xiaorui Yan, Tiantian Liu, Kairui Li, Dan Feng and Yujing Ren
{"title":"Ptn 簇和 Zn1 单原子之间的长程协同效应促进高效选择性加氢反应","authors":"Haisheng Wei, Jing Li, Xiaorui Yan, Tiantian Liu, Kairui Li, Dan Feng and Yujing Ren","doi":"10.1039/D4QI02027H","DOIUrl":null,"url":null,"abstract":"<p >Supported platinum group metal (PGM) catalysts are extensively utilized in catalytic hydrogenations. However, the adsorption energies on single PGM surfaces present the inherent scaling properties, which often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy by confining few-atom Pt<small><sub><em>n</em></sub></small> clusters in Zn<small><sub>1</sub></small>-N<small><sub>3</sub></small> sites decorated with microporous carbon material (Pt<small><sub><em>n</em></sub></small>@Zn<small><sub>1</sub></small>-N–C) to break the scaling relationship in selective hydrogenations. In detail, Pt<small><sub><em>n</em></sub></small> clusters are more favorable for H<small><sub>2</sub></small> activation, while the Zn<small><sub>1</sub></small>-N<small><sub>3</sub></small> single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atoms. Benefiting from this long-range synergistic effect, the Pt<small><sub><em>n</em></sub></small>@Zn<small><sub>1</sub></small>-N–C catalyst displays superior catalytic performance in the selective hydrogenation of nitroarenes (>99% selectivity at ∼100% conversion, and sulfur compound-resistant hydrogenations) and excellent stability in the reverse water gas shift reaction (>99% selectivity over 40 hours at 600 °C). Our findings provide a confinement approach for further improving catalytic performance in selective hydrogenations.</p>","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":null,"pages":null},"PeriodicalIF":5.3000,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A long-range synergistic effect between Ptn clusters and Zn1 single atoms for efficient selective hydrogenations†\",\"authors\":\"Haisheng Wei, Jing Li, Xiaorui Yan, Tiantian Liu, Kairui Li, Dan Feng and Yujing Ren\",\"doi\":\"10.1039/D4QI02027H\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Supported platinum group metal (PGM) catalysts are extensively utilized in catalytic hydrogenations. However, the adsorption energies on single PGM surfaces present the inherent scaling properties, which often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy by confining few-atom Pt<small><sub><em>n</em></sub></small> clusters in Zn<small><sub>1</sub></small>-N<small><sub>3</sub></small> sites decorated with microporous carbon material (Pt<small><sub><em>n</em></sub></small>@Zn<small><sub>1</sub></small>-N–C) to break the scaling relationship in selective hydrogenations. In detail, Pt<small><sub><em>n</em></sub></small> clusters are more favorable for H<small><sub>2</sub></small> activation, while the Zn<small><sub>1</sub></small>-N<small><sub>3</sub></small> single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atoms. Benefiting from this long-range synergistic effect, the Pt<small><sub><em>n</em></sub></small>@Zn<small><sub>1</sub></small>-N–C catalyst displays superior catalytic performance in the selective hydrogenation of nitroarenes (>99% selectivity at ∼100% conversion, and sulfur compound-resistant hydrogenations) and excellent stability in the reverse water gas shift reaction (>99% selectivity over 40 hours at 600 °C). Our findings provide a confinement approach for further improving catalytic performance in selective hydrogenations.</p>\",\"PeriodicalId\":6,\"journal\":{\"name\":\"ACS Applied Nano Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-10-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Nano Materials\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/qi/d4qi02027h\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Nano Materials","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/qi/d4qi02027h","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
A long-range synergistic effect between Ptn clusters and Zn1 single atoms for efficient selective hydrogenations†
Supported platinum group metal (PGM) catalysts are extensively utilized in catalytic hydrogenations. However, the adsorption energies on single PGM surfaces present the inherent scaling properties, which often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy by confining few-atom Ptn clusters in Zn1-N3 sites decorated with microporous carbon material (Ptn@Zn1-N–C) to break the scaling relationship in selective hydrogenations. In detail, Ptn clusters are more favorable for H2 activation, while the Zn1-N3 single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atoms. Benefiting from this long-range synergistic effect, the Ptn@Zn1-N–C catalyst displays superior catalytic performance in the selective hydrogenation of nitroarenes (>99% selectivity at ∼100% conversion, and sulfur compound-resistant hydrogenations) and excellent stability in the reverse water gas shift reaction (>99% selectivity over 40 hours at 600 °C). Our findings provide a confinement approach for further improving catalytic performance in selective hydrogenations.
期刊介绍:
ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.