Tunable Catalytic Performance of Single Pt Atom on Doped Graphene in Direct Dehydrogenation of Propane by Rational Doping: A Density Functional Theory Study

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	Tunable Catalytic Performance of Single Pt Atom on Doped Graphene in Direct Dehydrogenation of Propane by Rational Doping: A Density Functional Theory Study
	Sun, XY; Han, P; Li, B; Zhao, Z; Zhao, Z (reprint author), Shenyang Normal Univ, Inst Catalysis Energy & Environm, Coll Chem & Chem Engn, Shenyang 110034, Liaoning, Peoples R China.; Zhao, Z (reprint author), China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China.
	2018-01-25
发表期刊	JOURNAL OF PHYSICAL CHEMISTRY C
ISSN	1932-7447
卷号	122 期号:3 页码:1570-1576
摘要	The catalytic reaction pathways and performance of supported single Pt atom on nitrogen- and boron-doped graphene in the direct dehydrogenation of propane (PDH) are investigated by using first principles calculations. The different dopants on graphene have distinct effects on the electronic structure of the supported Pt atom. The nitrogen on the support withdraws electrons from Pt, but boron donates electrons to Pt. Consequently, the d-band center of Pt atom is modified by either nitrogen or boron doping. The nitrogen doping shifts the d-band center of Pt atom closer to the Fermi level compared with the boron doping and the pristine ones. On the other hand, the d-band center has a significant influence on the C-H bond dissociation energy and reaction barrier. Therefore, better reactivity of Pt is found on the support with more nitrogen dopants as the d-band center is closer to the Fermi level. Also the calculated dissociation energy and the first C-H bond activation barrier obey the BEP rule. The different ratios between nitrogen and boron on the codoped graphene can continuously adjust the electronic structure of supported Pt and deliver the dissociation energy and reaction barrier in between the pure nitrogen- and boron-doped cases. Among various investigated supports, the graphene doped by pyridine nitrogen is predicted to be the most effective for enhancing Pt catalytic performance. The current work shows the promising catalytic performance of supported single Pt atom in PDH. More importantly, the tunable properties of the supported metal catalysts on the carbon materials are achieved by the rational doping, which provides a practical strategy for the catalyst optimization.; The catalytic reaction pathways and performance of supported single Pt atom on nitrogen- and boron-doped graphene in the direct dehydrogenation of propane (PDH) are investigated by using first principles calculations. The different dopants on graphene have distinct effects on the electronic structure of the supported Pt atom. The nitrogen on the support withdraws electrons from Pt, but boron donates electrons to Pt. Consequently, the d-band center of Pt atom is modified by either nitrogen or boron doping. The nitrogen doping shifts the d-band center of Pt atom closer to the Fermi level compared with the boron doping and the pristine ones. On the other hand, the d-band center has a significant influence on the C-H bond dissociation energy and reaction barrier. Therefore, better reactivity of Pt is found on the support with more nitrogen dopants as the d-band center is closer to the Fermi level. Also the calculated dissociation energy and the first C-H bond activation barrier obey the BEP rule. The different ratios between nitrogen and boron on the codoped graphene can continuously adjust the electronic structure of supported Pt and deliver the dissociation energy and reaction barrier in between the pure nitrogen- and boron-doped cases. Among various investigated supports, the graphene doped by pyridine nitrogen is predicted to be the most effective for enhancing Pt catalytic performance. The current work shows the promising catalytic performance of supported single Pt atom in PDH. More importantly, the tunable properties of the supported metal catalysts on the carbon materials are achieved by the rational doping, which provides a practical strategy for the catalyst optimization.
部门归属	[sun, xiaoying ; han, peng ; zhao, zhen] shenyang normal univ, inst catalysis energy & environm, coll chem & chem engn, shenyang 110034, liaoning, peoples r china ; [zhao, zhen] china univ petr, state key lab heavy oil proc, beijing 102249, peoples r china ; [li, bo] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, liaoning, peoples r china
关键词	h Bond Activation Nanostructured Carbon Catalysts Total-energy Calculations Augmented-wave Method Heterogeneous Catalysis 1st Principles Basis-set Platinum Reactivity Surfaces
学科领域	Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
资助者	Liaoning Natural Science Foundation [201602676]; NSFC [91545117]; Special Fund of Liaoning Provincial Universities' Fundamental Scientific Research Projects [LQN201703]; Shenyang Normal University [51600308]; Engineering Technology Research Center of Catalysis for Energy and Environment; Major Platform for Science and Technology of the Universities in Liaoning Province; Liaoning Province Key Laboratory for Highly Efficient Conversion and Clean Utilization of Oil and Gas Resources; Engineering Research Center for Highly Efficient Conversion and Clean Use of Oil and Gas Resources of Liaoning Province
收录类别	SCI
语种	英语
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/79564
专题	中国科学院金属研究所
通讯作者	Zhao, Z (reprint author), Shenyang Normal Univ, Inst Catalysis Energy & Environm, Coll Chem & Chem Engn, Shenyang 110034, Liaoning, Peoples R China.; Zhao, Z (reprint author), China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China.
推荐引用方式 GB/T 7714	Sun, XY,Han, P,Li, B,et al. Tunable Catalytic Performance of Single Pt Atom on Doped Graphene in Direct Dehydrogenation of Propane by Rational Doping: A Density Functional Theory Study[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2018,122(3):1570-1576.
APA	Sun, XY,Han, P,Li, B,Zhao, Z,Zhao, Z ,&Zhao, Z .(2018).Tunable Catalytic Performance of Single Pt Atom on Doped Graphene in Direct Dehydrogenation of Propane by Rational Doping: A Density Functional Theory Study.JOURNAL OF PHYSICAL CHEMISTRY C,122(3),1570-1576.
MLA	Sun, XY,et al."Tunable Catalytic Performance of Single Pt Atom on Doped Graphene in Direct Dehydrogenation of Propane by Rational Doping: A Density Functional Theory Study".JOURNAL OF PHYSICAL CHEMISTRY C 122.3(2018):1570-1576.