Study on catalytic properties of metal-supported ZIF-8 with computational chemistry

doi:10.3969/j.issn.0438-1157.2014.05.013

Abstract

Abstract: Metal-organic frameworks (MOFs) are a new family of nanoporous functional materials that have shown potential applications in catalysis, due to their unique structural features. In this work, a combination of molecular simulation and density functional theory (DFT) calculation were employed to investigate the catalytic properties of metal-supported ZIF-8 with different metals (Pd, Ag, Pt and Au). First, the radial distribution function between these metal particles and the different atoms in ZIF-8 was analyzed from Monte Carlo (MC) and molecular dynamics (MD) simulations in order to determine the possible locations of the metal particles. Then, DFT calculations were performed at the generalized gradient corrected approximation (GGA) level with PW91 functional and the double numerical plus polarization (DNP) basis set. The binding energy was calculated to evaluate the relative stability of the metal particles (Pd, Ag, Pt and Au) in each site of the framework. The results showed that there were three types of interaction modes between the metals and the framework: carbon-metal-carbon (C-M-C), metal-carbon (M-C) and metal-bond (M-bond) modes, where the first type was the most stable one. For the same interaction type, the order of the stability of ZIF-8 with different metals was: Pd > Ag > Pt > Au. At the same time, the catalytic activity of the metal-supported materials was also investigated using CO as probe molecule. The analysis of the Mulliken population and the electrostatic potential distributions of metals indicated that metal particles were the Lewis acid sites which were related to their capabilities of accepting an electron. The order of their catalytic activities was: Pd > Pt > Ag > Au. The results obtained in this work may provide useful information for the catalytic application of MOFs loaded with metals.

Key words: metal-organic frameworks, nanoscale, density functional theory, metal particles, catalysis, stability, model

摘要： 金属-有机骨架材料（metal-organic frameworks，MOFs）是一类新型纳米多孔功能材料。由于其独特的结构特征，在催化方面展现出潜在的应用价值。采用分子模拟结合密度泛函理论的计算方法系统地研究了ZIF-8在负载金属Pd、Ag、Pt、Au后的催化活性。结果表明，金属与材料之间主要有3种作用方式，其中以“碳-金属-碳”（C-M-C）形式最为稳定。并且对于同一种方式，ZIF-8负载金属后的稳定性顺序为：Pd >Ag >Pt >Au。同时，利用CO作为探针分子，系统地研究了负载金属后ZIF-8的催化活性，发现这些金属原子的Lewis酸性强弱与其电子接受能力有关，其催化活性顺序为：Pd >Pt >Ag >Au。这为研究利用MOF材料负载金属用于催化提供了参考信息。

关键词: 金属-有机骨架材料, 纳微尺度, 密度泛函理论, 金属粒子, 催化, 稳定性, 模型

CLC Number:

TQ032.4

BO Xiaofan, WU Pingyi, LIU Dahuan, YANG Qingyuan, MA Qintian, LAN Ling, WANG Shaohua, ZHANG Yi, ZHONG Chongli. Study on catalytic properties of metal-supported ZIF-8 with computational chemistry[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.013.

薄晓帆, 吴平易, 刘大欢, 阳庆元, 麻沁甜, 兰玲, 王少华, 张轶, 仲崇立. 负载金属的ZIF-8催化活性的计算化学研究[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.013.

References 39

[1]	Czaja A, Trukhan N, Muller U. Industrial applications of metal-organic frameworks [J]. Chem. Soc. Rev., 2009, 38: 1284-1293
[2]	Meilikhov M, Yusenko K, Esken D, Turner S, Tendeloo G, Fischer R. Metals@MOFs - loading MOFs with metal nanoparticles for hybrid functions [J]. Eur. J. Inorg. Chem., 2010, 24: 3701-3714
[3]	Jiang H L, Akita T, Tshida T, Haruta M, Xu X. Synergistic catalysis of Au@Ag core-shell nanoparticles stabilized on metal-organic framework [J]. J. Am. Chem. Soc., 2011, 133: 1304-1306
[4]	Gu X J, Lu Z H, Jiang H L, Akita T, Xu X. Synergistic catalysis of metal-organic framework-immobilized Au-Pd nanoparticles in dehydrogenation of formic acid for chemical hydrogen storage [J]. J. Am. Chem. Soc., 2011, 133: 11822-11825
[5]	Esken D, Turner S, Lebedev O, Tendeloo G, Fischer R. Au@ZIFs: stabilization and encapsulation of cavity-size matching gold clusters inside functionalized zeolite imidazolate frameworks, ZIFs [J]. Chem. Mater., 2010, 22: 6393-6401
[6]	Lu G, Li S Z, Farha O, Hauser B, Qi X Y, Wang Y, Wang X, Han S Y, Liu X G, Duchene J, Zhang H, Zhang Q C, Chen X D, Ma J, Loo S, Wei W, Yang Y H, Hupp J, Huo F W. Imparting functionality to a metal-organic framework material by controlled encapsulation of nanoparticles [J]. Nat. Chem., 2012, 4: 310-316
[7]	Li P Z, Aranishi K, Xu X. ZIF-8 immobilized nickel nanoparticles: highly effective catalysts for hydrogen generation from hydrolysis of ammonia borane [J]. Chem. Commun., 2012, 48: 3173-3175
[8]	EI-Shall M, Abdelsayed V, Khder A, Hassan H, EI-Kaderi H, Rrich T. Metallic and bimetallic nanocatalysts incorporated into highly porous coordination polymer MIL-101 [J]. J. Mater. Chem., 2009, 19: 7625-7631
[9]	Jiang H L, Qu Q. Porous metal-organic frameworks as platforms for functional applications [J]. Chem. Commun., 2011, 47: 3351-3370
[10]	Liu H L, Liu Y L, Li Y W, Tang Z Y, Jiang H F. Metal-organic framework supported gold nanoparticles as a highly active heterogeneous catalyst for aerobic oxidation of alcohols [J]. J. Phys. Chem. C, 2010, 114: 13362-13369
[11]	Jiang H L, Liu B, Akita T, Haruta M, Sakurai H, Xu Q. Au@ZIF-8: CO oxidation over gold nanoparticles deposited to metal-organic framework [J]. J. Am. Chem. Soc., 2009, 131: 11302-11303
[12]	Lee J, Farha O, Roberts J, Scheidt K, Nguyen S, Hupp J. Metal- organic framework materials as catalysts [J]. Chem. Soc. Rev., 2009, 38: 1450-1459
[13]	Yoon M, Srirambalaji R, Kim K. Homochiral metal-organic frameworks for asymmetric heterogeneous catalysis [J]. Chem. Rev., 2012, 112: 1196-1231
[14]	Park K, Ni Z, Cote A, Choi J, Huang R, Uribe-Romo F, Chae H, Keeffe M, Yaghi O. Exceptional chemical and thermal stability of zeolitic imidazolate frameworks [J]. Proc. Natl. Acad. Sci. USA, 2006, 103: 10186-10191
[15]	Phan A, Doonan C, Uribe-Romo F, Knobler C, Keeffe M, Yaghi O. Synthesis, structure, and carbon dioxide capture properties of zeolitic imidazolate frameworks [J]. Acc. Chem. Res., 2010, 43: 58-67
[16]	Mayo S, Olafson B, Goddard Ⅲ W. DREIDING: a generic force field for molecular simulations [J]. J. Phys. Chem., 1990, 94: 8897-8809
[17]	Rappé A, Casewit C, Colwell K, Goddard Ⅲ W, Skiff W. UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations [J]. J. Am. Chem. Soc., 1992, 114: 10024-10039
[18]	Yang Q, Wiersum A D, Llewellyn P L, Guillerm V, Serre C, Maurin G. Functionalizing porous zirconium terephthalate UiO-66(Zr) for natural gas upgrading: a computational exploration [J]. Chem. Commun., 2011, 47: 9603-9605
[19]	Huang H L, Zhang W J, Liu D H, Liu B, Chen G J, Zhong C L. Effect of temperature on gas adsorption and separation in ZIF-8: a combined experimental and molecular simulation study [J]. Chem. Eng. Sci., 2011, 66: 6297-6305
[20]	Zheng C C, Liu D H, Yang Q Y, Zhong C L, Mi J G. Computational study on the influences of framework charges on CO2 uptake in metal-organic frameworks [J]. Ind. Eng. Chem. Res., 2009, 48: 10479-10484
[21]	Liu Y, Liu H L, Hu Y, Jiang J W. Density functional theory for adsorption of gas mixtures in metal-organic frameworks [J]. J. Phys. Chem. B, 2010, 114: 2820-2827
[22]	Zhu Y J, Zhou J H, Hu J, Liu H L, Hu Y. Computer simulation of gas adsorption in modified COF-108: the impregnation of C60 into COF-108 [J]. Mol. Simulat., 2012, 38: 595-603
[23]	Liu B, Sun C Y, Chen G J. Molecular simulation studies of separation of CH4/H2 mixture in metal-organic frameworks with interpenetration and mixed-ligand [J]. Chem. Eng. Sci., 2011, 66: 3012-3019
[24]	Materials Studio[M]. 4.3V. San Diego, CA: Accelrys, Inc., 2008
[25]	Psofogiannakis G, Froudakis G. Theoretical explanation of hydrogen spillover in metal-organic frameworks [J]. J. Phys. Chem. C, 2011, 115: 4047-4053
[26]	Hou X J, Li H Q. Unraveling the high uptake and selectivity of CO2 in the zeolitic imidazolate frameworks ZIF-68 and ZIF-69 [J]. J. Phys. Chem. C, 2010, 114: 13501-13508
[27]	Wang J G, Liu C J, Fang Z P, Liu Y, Han Z Q. DFT study of structural and electronic properties of PdO/HZSM-5 [J]. J. Phys. Chem. B, 2004, 108: 1653-1659
[28]	Hirsch T, Ojamae L. Quantum-chemical and force-field investigations of ice Ih: computation of proton-ordered structures and prediction of their lattice energies [J]. J. Phys. Chem. B, 2004, 108: 15856-15864
[29]	Benco L, Bucko T, Hafner J, Toulhoat, H. Ab initio simulation of Lewis sites in mordenite and comparative study of the strength of active sites via CO adsorption [J]. J. Phys. Chem. B, 2004, 108: 13656- 13666
[30]	Sun B Z, Chen W K, Zheng J D, Lu C H. Roles of oxygen vacancy in the adsorption properties of CO and NO on Cu2O(1 1 1) surface: results of a first-principles study [J]. Appl. Surf. Sci., 2008, 255: 3141-3148
[31]	Zhang R, Ling L, Li Z, Wang B. Solvent effects on Cu2O(1 1 1) surface properties and CO adsorption on Cu2O(1 1 1) surface: a DFT study [J]. Appl. Catal. A-Gen.,2011, 400: 142-147
[32]	Chizallet C, Lazare L, Bazer-Bachi D, Bonnier F, Lecocq V, Soyer E, Quoineaud A, Bats N. Catalysis of transesterification by a nonfunctionalized metal-organic framework: acido-basicity at the external surface of ZIF-8 probed by FTIR and ab initio calculations [J]. J. Am. Chem. Soc., 2010, 132: 12365-12377
[33]	Liu D H, Zhong C L. Characterization of Lewis acid sites in metal-organic frameworks using density functional theory [J]. J. Phys. Chem. Lett., 2010, 1: 97-101
[34]	Treesukol P, Srisuk K, Limtrakul J, Truong T. Nature of the metal-support interaction in bifunctional catalytic Pt/H-ZSM-5 zeolite [J]. J. Phys. Chem. B, 2005, 109: 11940-11945
[35]	Schroder F, Eshen D, Cokoja M, Berg M, Lebedew O, Tendeloo G, Walaszek B, Buntkowsky G, Limbach H, Chaudret B, Fischer R. Ruthenium nanoparticles inside porous [Zn4O(bdc)3] by hydrogenolysis of adsorbed [Ru(cod)(cot)]: a solid-state reference system for surfactant-stabilized ruthenium colloids [J]. J. Am. Chem. Soc., 2008, 130: 6119-6130
[36]	Jiang Ling(江陵), Wang Guichang(王贵昌), Guan Naijia(关乃佳), Wu Yang(吴杨), Cai Zunsheng(蔡遵生), Pan Yinming(潘荫明), Zhao Xuezhuang(赵学庄), Huang Wei(黄伟), Li Yongwang(李永旺), Sun Yuhan(孙予罕), Zhong Bing(钟炳). DFT studies of CO adsorption and activation on some transition metal surfaces [J]. Acta Phys. -Chim. Sin. (物理化学学报), 2003, 19: 393-397
[37]	Aray Y, Rodriguez J, Coll S, Rodriguez-Arias E, Vega D. Nature of the Lewis acid sites on molybdenum and ruthenium sulfides: an electrostatic potential study [J]. J. Phys. Chem. B, 2005, 109: 23564-23570
[38]	Aray Y, Rodriguez J, Vidal A, Coll S. Nature of the NiMoS catalyst edge sites: an atom in molecules theory and electrostatic potential studies [J]. J. Mol. Catal. A: Chem., 2007, 271: 105-116
[39]	Yin Ming(殷明), Shu Yuanjie(舒远杰), Xiong Ying(熊鹰), Luo Shikai(罗世凯), Wang Ping(王苹), Long Xinping(龙新平), Zhu Zuliang(朱祖良). Theoretical studies on structures and properties of nitroimidazole compounds [J]. Acta. Chim. Sinica(化学学报), 2008, 66: 2117-2123