Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube

doi:10.1002/smll.202401532

IMR OpenIR

	Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube
	Zhang, Xuefei 1,2,3; Dai, Xueya 2; Xie, Zailai 1; Qi, Wei 2
通讯作者	Xie, Zailai(zlxie@fzu.edu.cn) ; Qi, Wei(wqi@imr.ac.cn)
	2024-05-03
发表期刊	SMALL
ISSN	1613-6810
页码	8
摘要	Borocarbonitride (BCN) catalysts, boasting multiple redox sites, have shown considerable potential in alkane oxidative dehydrogenation (ODH) to olefin molecules. However, their catalytic efficiency still lags behind that of leading commercial catalysts, primarily due to the limited reactivity of oxygen functional groups. In this study, a groundbreaking hybrid catalyst is developed, featuring BCN nanotubes (BCNNTs) encapsulated with manganese (Mn) clusters, crafted through a meticulous supramolecular self-assembly and postcalcination strategy. This novel catalyst demonstrates a remarkable enhancement in activity, achieving 30% conversion and approximate to 100% selectivity toward styrene in ethylbenzene ODH reactions. Notably, its performance surpasses both pure BCNNTs and those hosting Mn nanoparticles. Structural and kinetic analyses unveil a robust interaction between BCNNTs and the Mn component, substantially boosting the catalytic activity of BCNNTs. Furthermore, density functional theory (DFT) calculations elucidate that BCNNTs encapsulated with Mn clusters not only stabilize key intermediates (& horbar;B & horbar;O & horbar;O & horbar;B & horbar;) but also enhance the nucleophilicity of active sites through electron transfer from the Mn cluster to the BCNNTs. This electron transfer mechanism effectively lowers the energy barrier for & horbar;C & horbar;H cleavage, resulting in a 13% improvement in catalytic activity compared to pure BCNNTs. Manganese (Mn) cluster promoters enhance the catalytic activity of borocarbonitride in ethylbenzene oxidative dehydrogenation with approximate to 100% styrene selectivity, superior to these of unmodified and Mn particle-modified borocarbonitride materials, and the nature of activity improvement and reaction mechanism is revealed by combining with structural characterizations and density functional theory calculations. image
关键词	borocarbonitride nanotubes heterogeneous catalysis Mn modfication oxidative dehydrogenation strong interaction
资助者	Natural Science Foundation of Liaoning Province of China ; NSFC of China
DOI	10.1002/smll.202401532
收录类别	SCI
语种	英语
资助项目	Natural Science Foundation of Liaoning Province of China ; NSFC of China[22072018] ; NSFC of China[22372039] ; NSFC of China[21761132010] ; NSFC of China[91645114] ; NSFC of China[U23A20545] ; [2020-YQ-02]
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS类目	Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS记录号	WOS:001217087300001
出版者	WILEY-V C H VERLAG GMBH
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/186037
专题	中国科学院金属研究所
通讯作者	Xie, Zailai; Qi, Wei
作者单位	1.Fuzhou Univ, Key Lab Adv Carbon Based Funct Mat, Fuzhou 350016, Fujian, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Fuzhou Univ, Coll Chem Engn, Fuzhou 350016, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Xuefei,Dai, Xueya,Xie, Zailai,et al. Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube[J]. SMALL,2024:8.
APA	Zhang, Xuefei,Dai, Xueya,Xie, Zailai,&Qi, Wei.(2024).Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube.SMALL,8.
MLA	Zhang, Xuefei,et al."Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube".SMALL (2024):8.