Electronic interaction between single Pt atom and vacancies on boron nitride nanosheets and its influence on the catalytic performance in the direct dehydrogenation of propane

doi:10.1016/S1872-2067(18)63196-1

IMR OpenIR

	Electronic interaction between single Pt atom and vacancies on boron nitride nanosheets and its influence on the catalytic performance in the direct dehydrogenation of propane
	Sun, Xiaoying 1; Liu, Meijun 1; Huang, Yaoyao 1; Li, Bo 3; Zhao, Zhen 1,2
通讯作者	Zhao, Zhen(zhenzhao@cup.edu.cn)
	2019-06-01
发表期刊	CHINESE JOURNAL OF CATALYSIS
ISSN	0253-9837
卷号	40 期号:6 页码:819-825
摘要	The electronic metal-support interaction (EMSI) is one of most intriguing phenomena in heterogeneous catalysis. In this work, this subtle effect is clearly demonstrated by density functional theory (DFT) calculations of single Pt atom supported on vacancies in a boron nitride nanosheet. Moreover, the relation between the EMSI and the performance of Pt in propane direct dehydrogenation (PDH) is investigated in detail. The charge state and partial density of states of single Pt atom show distinct features at different anchoring positions, such as boron and nitrogen vacancies (B-vac and N-vac respectively). Single Pt atom become positively and negatively charged on B-vac and N-vac, respectively. Therefore, the electronic structure of Pt can be adjusted by rational deposition on the support. Moreover, Pt atoms in different charge states have been shown to have different catalytic abilities in PDH. The DFT calculations reveal that Pt atoms on B-vac (Pt-B-vac) have much higher reactivity towards reactant/product adsorption and C-H bond activation than Pt supported on N-vac (Pt-N-vac), with larger adsorption energy and lower barrier along the reaction pathway. However, the high reactivity of Pt-B-vac also hinders propene desorption, which could lead to unwanted deep dehydrogenation. Therefore, the results obtained herein suggest that a balanced reactivity for C-H activation in propane and propene desorption is required to achieve optimum yields. Based on this descriptor, a single Pt atom on a nitrogen vacancy is considered an effective catalyst for PDH. Furthermore, the deep dehydrogenation of the formed propene is significantly suppressed, owing to the large barrier on Pt-N-vac. The current work demonstrates that the catalytic properties of supported single Pt atoms can be tuned by rationally depositing them on a boron nitride nanosheet and highlights the great potential of single-atom catalysis in the PDH reaction. (C) 2019, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
关键词	Propane Direct dehydrogenation Platinum Boron nitride Single atom catalysis Density functional theory Electronic metel-support interaction
资助者	National Science Foundation of China ; Natural Science Foundation of Liaoning Province ; Fundamental Research Funds for Colleges and Universities in Liaoning Province ; Startup Foundation for Doctors of Shenyang Normal University
DOI	10.1016/S1872-2067(18)63196-1
收录类别	SCI
语种	英语
资助项目	National Science Foundation of China[91545117] ; Natural Science Foundation of Liaoning Province[201602676] ; Fundamental Research Funds for Colleges and Universities in Liaoning Province[LQN201703] ; Startup Foundation for Doctors of Shenyang Normal University[B5201620]
WOS研究方向	Chemistry ; Engineering
WOS类目	Chemistry, Applied ; Chemistry, Physical ; Engineering, Chemical
WOS记录号	WOS:000468376800003
出版者	SCIENCE PRESS
引用统计	被引频次：30[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/133558
专题	中国科学院金属研究所
通讯作者	Zhao, Zhen
作者单位	1.Shenyang Normal Univ, Inst Catalysis Energy & Environm, Coll Chem & Chem Engn, Shenyang 110034, Liaoning, Peoples R China 2.China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China 3.Chinese Acad Sci, Inst Met Res, Shenyang 110016, Liaoning, Peoples R China
推荐引用方式 GB/T 7714	Sun, Xiaoying,Liu, Meijun,Huang, Yaoyao,et al. Electronic interaction between single Pt atom and vacancies on boron nitride nanosheets and its influence on the catalytic performance in the direct dehydrogenation of propane[J]. CHINESE JOURNAL OF CATALYSIS,2019,40(6):819-825.
APA	Sun, Xiaoying,Liu, Meijun,Huang, Yaoyao,Li, Bo,&Zhao, Zhen.(2019).Electronic interaction between single Pt atom and vacancies on boron nitride nanosheets and its influence on the catalytic performance in the direct dehydrogenation of propane.CHINESE JOURNAL OF CATALYSIS,40(6),819-825.
MLA	Sun, Xiaoying,et al."Electronic interaction between single Pt atom and vacancies on boron nitride nanosheets and its influence on the catalytic performance in the direct dehydrogenation of propane".CHINESE JOURNAL OF CATALYSIS 40.6(2019):819-825.