CONDENSED MATTER: ELECTRONIC STRUCTURE, ELECTRICAL, MAGNETIC, AND OPTICAL PROPERTIES |
Prev
Next
|
|
|
Effect of metal catalyst on the mechanism of hydrogen spillover in three-dimensional covalent-organic frameworks |
Xiu-Ying Liu(刘秀英)1, Jing-Xin Yu(于景新)1, Xiao-Dong Li(李晓东)1, Gui-Cheng Liu(刘桂成)2, Xiao-Feng Li(李晓凤)3, Joong-Kee Lee2 |
1 College of Science, Henan University of Technology, Zhengzhou 450000, China; 2 Center for Energy Convergence Research, Green City Research Institute, Korea Institute of Science and Technology(KIST), Seoul 02792, Republic of Korea; 3 College of Physical and Electronic Information, Luoyang Normal University, Luoyang 471022, China |
|
|
Abstract Hydrogen spillover mechanism of metal-supported covalent-organic frameworks COF-105 is investigated by means of the density functional theory, and the effects of metal catalysts M4 (Pt4, Pd4, and Ni4) on the whole spillover process are systematically analyzed. These three metal catalysts exhibit several similar phenomena: (i) they prefer to deposit on the tetra (4-dihydroxyborylphenyl) silane (TBPS) cluster with surface-contacted configuration; (ii) only the H atoms at the bridge site can migrate to 2,3,6,7,10,11-hexahydroxy triphenylene (HHTP) and TBPS surfaces, and the migration process is an endothermic reaction and not stable; (iii) the introduction of M4 catalyst can greatly reduce the diffusion energy barrier of H atoms, which makes it easier for the H atoms to diffuse on the substrate surface. Differently, all of the H2 molecules spontaneously dissociate into H atoms onto Pt4 and Pd4 clusters. However, the adsorbed H2 molecules on Ni4 cluster show two types of adsorption states: one activated state with stretched H-H bond length of 0.88 Å via the Kubas interaction and five dissociated states with separated hydrogen atoms. Among all the M4 catalysts, the orders of the binding energy of M4 deposited on the substrate and average chemisorption energy per H2 molecule are Pt4 > Ni4 > Pd4. On the contrary, the orders of the migration and diffusion barriers of H atoms are Pt4 < Ni4 < Pd4, which indicates that Pt4 is the most promising catalyst for the hydrogen spillover with the lowest migration and diffusion energy barriers. However, the migration of H atoms from Pt4 toward the substrate is still endothermic. Thus direct migration of H atom from metal catalyst toward the substrate is thermodynamically unfavorable.
|
Received: 07 October 2016
Revised: 06 November 2016
Accepted manuscript online:
|
PACS:
|
73.22.-f
|
(Electronic structure of nanoscale materials and related systems)
|
|
36.40.-c
|
(Atomic and molecular clusters)
|
|
71.15.Mb
|
(Density functional theory, local density approximation, gradient and other corrections)
|
|
Fund: Project supported by the National Natural Science Foundation of China (Grant Nos. 11304079, 11304140, 11404094, and 11504088), the China National Scholarship Foundation (Grant No. 201508410255), the Foundation for Young Core Teachers of Higher Education Institutions of Henan Province of China, the Foundation for Young Core Teachers of Henan University of Technology in China, the Korea Institute of Science and Technology (KIST) Institutional Program (Grant No. 2E26291) and Flag Program (Grant No. 2E26300), and the Research Grants of NRF funded by the National Research Foundation under the Ministry of Science, ICT & Future, Korea (Grant No. NRF-2015H1D3A1036078). |
Corresponding Authors:
Gui-Cheng Liu
E-mail: log67@163.com
|
Cite this article:
Xiu-Ying Liu(刘秀英), Jing-Xin Yu(于景新), Xiao-Dong Li(李晓东), Gui-Cheng Liu(刘桂成), Xiao-Feng Li(李晓凤), Joong-Kee Lee Effect of metal catalyst on the mechanism of hydrogen spillover in three-dimensional covalent-organic frameworks 2017 Chin. Phys. B 26 027302
|
[1] |
Zhang F, Zhao P, Meng N and Maddy J 2016 Int. J. Hydrogen Energy 41 14535
|
[2] |
Hu Y H 2013 Int. J. Energy Res. 37 683
|
[3] |
Ruan W, Wu D L, Luo W L, Yu X G and Xie A D 2014 Chin. Phys. B 23 023102
|
[4] |
Schlapbach L and Züttel A 2001 Nature 414 353
|
[5] |
Liu X Y, Wang C Y, Tang Y J, Sun W G and Wu W D 2010 Chin. Phys. B 19 036103
|
[6] |
Côté A P, Benin A I, Ockwig N W, O'Keeffe M, Matzger A J and Yaghi O M 2005 Science 310 1166
|
[7] |
Spitler E L and Dichtel W R 2010 Nat. Chem. 2 672
|
[8] |
Liu X Y, He J, Yu J X, Li Z X and Fan Z Q 2014 Chin. Phys. B 23 067303
|
[9] |
Guo J H, Zhang H, Tang Y J and Cheng X L 2013 Phys. Chem. Chem. Phys. 15 2873
|
[10] |
Klontzas E, Tylianakis E and Froudakis G E 2008 J. Phys. Chem. C 112 9095
|
[11] |
Wong-Foy A G, Matzger A J and Yaghi O M 2006 J. Am. Chem. Soc. 128 3494
|
[12] |
Lachawiec A J Jr, Qi G and Yang R T 2005 Langmuir 21 11418
|
[13] |
Tsao C S, Liu Y, Chuang H Y, Tseng H H, Chen T Y, Chen C H, Yu M S, Li Q, Lueking A and Chen S H 2011 J. Phys. Chem. Lett. 2 2322
|
[14] |
Lachawiec A J Jr and Yang R T 2008 Langmuir 24 6159
|
[15] |
Pham V H, Dang T T, Singh K, Hur S H, Shin E W, Kim J S, Lee M A, Baeck S H and Chung J S 2013 J. Mater. Chem. A 1 1070
|
[16] |
Li Y W and Yang R T 2006 J. Am. Chem. Soc. 128 726
|
[17] |
Li Y W and Yang R T 2008 AIChE J. 54 269
|
[18] |
Kalidindi S B, Oh H, Hirscher M, Esken D, Wiktor C, Turner S, Van Tendeloo G and Fischer R A 2012 Chem. Eur. J. 18 10848
|
[19] |
Prins R 2012 Chem. Soc. 112 2714
|
[20] |
Suri M, Dornfeld M and Ganz E 2009 J. Chem. Phys. 131 174703
|
[21] |
Ganz E and Dornfeld M 2012 J. Phys. Chem. C 116 3661
|
[22] |
Ganz E and Dornfeld M 2014 J. Phys. Chem. C 118 5657
|
[23] |
Chen L, Cooper A C, Pez G P and Cheng H 2007 J. Phys. Chem. C 111 5514
|
[24] |
Kresse G and Hafner J 1993 Phys. Rev. B 48 13115
|
[25] |
Kresse G and Furthmüller J 1996 Comput. Mater. Sci. 6 15
|
[26] |
Perdew J P, Burke K and Ernzerhof M 1996 Phys. Rev. Lett. 77 3865
|
[27] |
Blöchl P E 1994 Phys. Rev. B 50 17953
|
[28] |
Henkelman G, Uberuaga B P and Jónsson H 2000 J. Chem. Phys. 113 9901
|
[29] |
Sigal A, Rojas M I and Leiva E P M 2011 Phys. Rev. Lett. 107 158701
|
[30] |
Zhou C, Wu J, Nie A, Forrey R C, Tachibana A and Cheng H 2007 J. Phys. Chem. C 111 12773
|
[31] |
Cabria I, López M J, Fraile S and Alonso J A 2012 J. Phys. Chem. C 116 21179
|
[32] |
Wu H Y, Fan X F, Kuo J L and Deng W Q 2011 J. Phys. Chem. C 115 9241
|
No Suggested Reading articles found! |
|
|
Viewed |
|
|
|
Full text
|
|
|
|
|
Abstract
|
|
|
|
|
Cited |
|
|
|
|
Altmetric
|
blogs
Facebook pages
Wikipedia page
Google+ users
|
Online attention
Altmetric calculates a score based on the online attention an article receives. Each coloured thread in the circle represents a different type of online attention. The number in the centre is the Altmetric score. Social media and mainstream news media are the main sources that calculate the score. Reference managers such as Mendeley are also tracked but do not contribute to the score. Older articles often score higher because they have had more time to get noticed. To account for this, Altmetric has included the context data for other articles of a similar age.
View more on Altmetrics
|
|
|