Wangwang Zhang, Kelechi Uwakwe, Jingting Hu, Yan Wei, Juntong Zhu, Wu Zhou, Chao Ma, Liang Yu, Rui Huang, Dehui Deng
{"title":"在 WS2 封闭原子钯位点上进行乙炔加氢制乙烯的环境条件研究","authors":"Wangwang Zhang, Kelechi Uwakwe, Jingting Hu, Yan Wei, Juntong Zhu, Wu Zhou, Chao Ma, Liang Yu, Rui Huang, Dehui Deng","doi":"10.1038/s41467-024-53481-1","DOIUrl":null,"url":null,"abstract":"<p>Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production with minimal additional energy input, yet remains a great challenge due to the difficulty in the coactivation of acetylene and H<sub>2</sub> at room temperature. Herein, we report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface. The catalyst exhibits over 99% acetylene conversion with a high ethylene selectivity of 70% at 25 <sup>o</sup>C, and a record space-time yield of ethylene of 1123 mol<sub>C2H4</sub> mol<sub>Pd</sub><sup>−1</sup> h<sup>−1</sup> under ambient conditions, which is nearly four times that of the typical Pd<sub>1</sub>Ag<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst, and exhibiting superior stability of over 500 h. We demonstrate that the confinement of Pd-S coordination induces positively-charged atomic Pd<sup>δ+</sup>, which not only facilitates C<sub>2</sub>H<sub>2</sub> hydrogenation but also promotes C<sub>2</sub>H<sub>4</sub> desorption, thereby enabling a high conversion of C<sub>2</sub>H<sub>2</sub> to C<sub>2</sub>H<sub>4</sub> at room temperature while suppressing over-hydrogenation to C<sub>2</sub>H<sub>6</sub>.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":null,"pages":null},"PeriodicalIF":14.7000,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ambient-condition acetylene hydrogenation to ethylene over WS2-confined atomic Pd sites\",\"authors\":\"Wangwang Zhang, Kelechi Uwakwe, Jingting Hu, Yan Wei, Juntong Zhu, Wu Zhou, Chao Ma, Liang Yu, Rui Huang, Dehui Deng\",\"doi\":\"10.1038/s41467-024-53481-1\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production with minimal additional energy input, yet remains a great challenge due to the difficulty in the coactivation of acetylene and H<sub>2</sub> at room temperature. Herein, we report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface. The catalyst exhibits over 99% acetylene conversion with a high ethylene selectivity of 70% at 25 <sup>o</sup>C, and a record space-time yield of ethylene of 1123 mol<sub>C2H4</sub> mol<sub>Pd</sub><sup>−1</sup> h<sup>−1</sup> under ambient conditions, which is nearly four times that of the typical Pd<sub>1</sub>Ag<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> catalyst, and exhibiting superior stability of over 500 h. We demonstrate that the confinement of Pd-S coordination induces positively-charged atomic Pd<sup>δ+</sup>, which not only facilitates C<sub>2</sub>H<sub>2</sub> hydrogenation but also promotes C<sub>2</sub>H<sub>4</sub> desorption, thereby enabling a high conversion of C<sub>2</sub>H<sub>2</sub> to C<sub>2</sub>H<sub>4</sub> at room temperature while suppressing over-hydrogenation to C<sub>2</sub>H<sub>6</sub>.</p>\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.7000,\"publicationDate\":\"2024-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-024-53481-1\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-024-53481-1","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
Ambient-condition acetylene hydrogenation to ethylene over WS2-confined atomic Pd sites
Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production with minimal additional energy input, yet remains a great challenge due to the difficulty in the coactivation of acetylene and H2 at room temperature. Herein, we report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface. The catalyst exhibits over 99% acetylene conversion with a high ethylene selectivity of 70% at 25 oC, and a record space-time yield of ethylene of 1123 molC2H4 molPd−1 h−1 under ambient conditions, which is nearly four times that of the typical Pd1Ag3/Al2O3 catalyst, and exhibiting superior stability of over 500 h. We demonstrate that the confinement of Pd-S coordination induces positively-charged atomic Pdδ+, which not only facilitates C2H2 hydrogenation but also promotes C2H4 desorption, thereby enabling a high conversion of C2H2 to C2H4 at room temperature while suppressing over-hydrogenation to C2H6.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.