Direct dehydrogenation of ethylbenzene over nickel phosphide/carbon nanotube hybrid catalyst: Mechanistic insight into phosphor as electronic structure regulator
{"title":"Direct dehydrogenation of ethylbenzene over nickel phosphide/carbon nanotube hybrid catalyst: Mechanistic insight into phosphor as electronic structure regulator","authors":"Xueya Dai, Yunli Bai, Kunru Fan, Gang Sun, Xiangjie Zeng, Wei Qi","doi":"10.1016/j.cej.2025.166065","DOIUrl":null,"url":null,"abstract":"Development of non-noble metallic catalysts for alkane dehydrogenation is a hot topic in the field of catalysis, which relies on the in-depth understanding of the reaction mechanism and the accurate engineering of the electronic structure of the catalyst. In the present work, a novel phosphor modified nickel based catalyst (NiPx/oCNT) was prepared and employed for direct dehydrogenation (DDH) of ethylbenzene (EB) to styrene (ST). The NiPx/oCNT catalyst with well-designed electronic structure showed ST formation rate at 3.19 mmol g<ce:sup loc=\"post\">−1</ce:sup> h<ce:sup loc=\"post\">−1</ce:sup> with over 99.0 % ST selectivity with a decent deactivation rate of 0.02 h<ce:sup loc=\"post\">−1</ce:sup>. Comprehensive structure-function relationship characterizations and density functional theory calculations revealed that the electron density in d orbital of Ni decreased with the electronic structure regulation of phosphor, which effectively facilitated ST desorption and reduced the cracking side-reaction and consequent carbonous deposition. The present work not only developed a novel Ni-based catalyst for highly efficient EB DDH reactions but also testified an important concept of delicate electronic structure engineering for enhancing the catalytic performance of transition metal catalysts.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"10 1","pages":""},"PeriodicalIF":13.3000,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2025.166065","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Development of non-noble metallic catalysts for alkane dehydrogenation is a hot topic in the field of catalysis, which relies on the in-depth understanding of the reaction mechanism and the accurate engineering of the electronic structure of the catalyst. In the present work, a novel phosphor modified nickel based catalyst (NiPx/oCNT) was prepared and employed for direct dehydrogenation (DDH) of ethylbenzene (EB) to styrene (ST). The NiPx/oCNT catalyst with well-designed electronic structure showed ST formation rate at 3.19 mmol g−1 h−1 with over 99.0 % ST selectivity with a decent deactivation rate of 0.02 h−1. Comprehensive structure-function relationship characterizations and density functional theory calculations revealed that the electron density in d orbital of Ni decreased with the electronic structure regulation of phosphor, which effectively facilitated ST desorption and reduced the cracking side-reaction and consequent carbonous deposition. The present work not only developed a novel Ni-based catalyst for highly efficient EB DDH reactions but also testified an important concept of delicate electronic structure engineering for enhancing the catalytic performance of transition metal catalysts.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.