Characterization and analysis of copper species on the surface of Y zeolite loaded copper

doi:10.16085/j.issn.1000-6613.2015.07.020

Abstract

Abstract: This paper reviewed the research progress in Cu species characterization and analysis about CuY, and focused recent progress in micro-structure analysis of CuY by X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), hydrogen temperature programmed reduction (H₂-TPR), in situ infrared spectroscopy (CO-IR and NO-IR), and electron spin resonance (ESR). The paper also reviewed that the CuY preparation has effect on the location of copper species and the performance of CuY, and pointed out that accurate and informed information about present state, valence state, location, content can be obtained by synthetically employing all above characterization methods. The future development could be focused on the preparation of CuY with optimum performance by choosing appropriate method to regulate and control present state, valence state, and the location of copper species.

Key words: CuY catalyst, surface, copper species, presence status, valence state, distributions, characterization analysis

摘要： 综述了铜负载Y分子筛(CuY)中Cu物种表征及分析的研究进展, 重点阐述了近年来X射线衍射分析(XRD)、透射电子显微镜分析(TEM)、X射线光电子能谱分析(XPS)、H₂程序升温还原(H₂-TPR)、原位红外光谱(CO-IR和NO-IR)、电子顺磁共振(ESR)等表征方法在CuY中Cu物种的微观结构分析方面取得的进展。还对制备方法对CuY中Cu物种落位和性能的影响进行了综述, 指出综合采用这些表征方法, 得到CuY中Cu物种状态、价态、落位及含量等更加全面、准确的信息, 进而选择合适的制备方法调控CuY中Cu物种存在状态、价态及落位, 制备出性能更佳的CuY是今后发展的方向。

关键词: CuY催化剂, 表面, 铜物种, 存在状态, 价态, 分布, 表征分析

CLC Number:

O643.36

WANG Yuchun, ZHENG Huayan, LI Mengyun, LI Zhong. Characterization and analysis of copper species on the surface of Y zeolite loaded copper[J]. Chemical Industry and Engineering Progree, 2015, 34(07): 1933-1940.

王玉春, 郑华艳, 李梦云, 李忠. 铜负载Y分子筛中Cu物种的表征及分析[J]. 化工进展, 2015, 34(07): 1933-1940.

References

[1] Ibrahim K, Hall A. New occurrences of diagenetic faujasite in the Quaternary tuffs of northeast Jordan[J]. European Journal of Mineralogy, 1995, 7:1129-1135.
[2] 徐如人, 庞文琴, 于吉红, 等. 分子筛与多孔材料化学[M]. 北京:科学出版社, 2004:246-247.
[3] Song H, Wan X, Dai M, et al. Deep desulfurization of model gasoline by selective adsorption over Cu-Ce bimetal ion-exchanged Y zeolite[J]. Fuel Processing Technology, 2013, 116:52-62.
[4] Takahashi A, Yang R T, Munson C L, et al. Cu(Ⅰ)-Y-zeolite as a superior adsorbent for diene/olefin separation[J]. Langmuir, 2001, 17(26):8405-8413.
[5] Hernández-Maldonado A J, Yang F H, Qi G. et al. Desulfurization of transportation fuels by π-complexation sorbents:Cu(Ⅰ)-, Ni(Ⅱ)-, and Zn(Ⅱ)-zeolites[J]. Applied Catalysis B:Environmental, 2005, 56(1-2):111-126.
[6] Ochońska J, McClymont D, Jodłowski P J, et al. Copper exchanged ultrastable zeolite Y:A catalyst for NH₃-SCR of NO_x from stationary biogas engines[J]. Catalysis Today, 2012, 191(1):6-11.
[7] Kieger S, Delahay G, Coq B. Influence of co-cations in the selective catalytic reduction of NO by NH₃ over copper exchanged faujasite zeolites[J]. Applied Catalysis B:Environmental, 2000, 25(1):1-9.
[8] King S T. Reaction mechanism of oxidative carbonylation of methanol to dimethyl carbonate in Cu-Y zeolite[J]. Journal of Catalysis, 1996, 161(2):530-538.
[9] 王坤, 李忠李安民. 氧化羰基化合成碳酸二甲酯催化剂的研究进展[J]. 化工进展, 2013(11):2631-2637.
[10] 仇鹏王保伟. 羰基合成碳酸二甲酯的研究进展[J]. 化工进展, 2010, 29(6):56-62.
[11] 王佳臻, 郑华艳孟凡会, 等. 制备方法对CuY催化剂活性组分Cu落位及催化性能影响[C]//中国化学会第28届学术年会. 成都, 2012.
[12] 王瑞玉李忠. CuNaY分子筛的制备及其催化甲醇氧化羰基化[J]. 燃料化学学报, 2013, 32(11):1361-1366.
[13] Gentry S J, Hurst N W, Jones A. Temperature programmed reduction of copper ions in zeolites[J]. Journal of the Chemical Society, Faraday Transactions 1:Physical Chemistry in Condensed Phases, 1979, 75:1688-1699.
[14] Huang S Y, Chen P Z, Yan B, et al. Modification of Y zeolite with alkaline treatment:Textural properties and catalytic activity for diethyl carbonate synthesis[J]. Industrial & Engineering Chemistry Research, 2013, 52(19):6349-6356.
[15] Huang S, Wang Y, Wang Z, et al. Cu-doped zeolites for catalytic oxidative carbonylation:The role of Brønsted acids[J]. Applied Catalysis A:General, 2012, 417-418:236-242.
[16] Richter M, Fait M J G, Eckelt R, et al. Gas-phase carbonylation of methanol to dimethyl carbonate on chloride-free Cu-precipitated zeolite Y at normal pressure[J]. Journal of Catalysis, 2007, 245(1):11-24.
[17] Drake I J, Zhang Y, Briggs D, et al. The local environment of Cu⁺ in Cu-Y zeolite and its relationship to the synthesis of dimethyl carbonate[J]. The Journal of Physical Chemistry B, 2006, 110(24):11654-11664.
[18] Richter M, Fait M J G, Eckelt R, et al. Oxidative gas phase carbonylation of methanol to dimethyl carbonate over chloride-free Cu-impregnated zeolite Y catalysts at elevated pressure[J]. Applied Catalysis B:Environmental, 2007, 73(3-4):269-281.
[19] Nam J K, Choi M J, Cho D H, et al. The influence of support in the synthesis of dimethyl carbonate by Cu-based catalysts[J]. Journal of Molecular Catalysis A:Chemical, 2013, 370:7-13.
[20] 付廷俊, 郑华艳, 牛燕燕, 等. Ce, La和Cs离子对CuY催化甲醇氧化羰基化活性中心的影响[J]. 化学学报, 2011(15):1765-1772.
[21] 李忠, 付廷俊郑华艳. CuY制备方法对其催化甲醇氧化羰基化活性中心的影响[J]. 无机化学学报, 2011(8):1483-1490.
[22] 王佳臻, 郑华艳李忠. CuY催化剂中Cu活性中心落位调控及其催化性能的影响[C]//第十七届全国分子筛学术大会, 银川, 2013.
[23] Yi D, Huang H, Meng X, et al. Adsorption-desorption behavior and mechanism of dimethyl disulfide in liquid hydrocarbon streams on modified Y zeolites[J]. Applied Catalysis B:Environmental, 2014, 148-149:377-386.
[24] Zahmakiran M, Özkar S. Preparation and characterization of zeolite framework stabilized cuprous oxide nanoparticles[J]. Materials Letters, 2009, 63(12):1033-1036.
[25] Zahmakıran M, Durap F, Özkar S. Zeolite confined copper(0) nanoclusters as cost-effective and reusable catalyst in hydrogen generation from the hydrolysis of ammonia-borane[J]. International Journal of Hydrogen Energy, 2010, 35(1):187-197.
[26] Li X, Zhang X, Lei L. Preparation of CuNaY zeolites with microwave irradiation and their application for removing thiophene from model fuel[J]. Separation and Purification Technology, 2009, 64(3):326-331.
[27] Ren J, Liu S, Li Z, et al. Structural feature and catalytic performance of Cu-SiO₂-TiO₂ cogelled xerogel catalysts for oxidative carbonylation of methanol to dimethyl carbonate[J]. Catalysis Communications, 2011, 12(5):357-361.
[28] Alonso F, Melkonian T, Moglie Y, et al. Homocoupling of terminal alkynes catalysed by ultrafine copper nanoparticles on titania[J]. European Journal of Organic Chemistry, 2011(13):2524-2530.
[29] Yuan Y, Cao W, Weng W. CuCl₂ immobilized on amino-functionalized MCM-41 and MCM-48 and their catalytic performance toward the vapor-phase oxy-carbonylation of methanol to dimethylcarbonate[J]. Journal of Catalysis, 2004, 228(2):311-320.
[30] Lázaro Martínez J M, Rodríguez-Castellón E, Sánchez R M T, et al. XPS studies on the Cu(Ⅰ, Ⅱ)-polyampholyte heterogeneous catalyst:An insight into its structure and mechanism[J]. Journal of Molecular Catalysis A:Chemical, 2011, 339(1-2):43-51.
[31] 徐舒涛, 张维萍, 韩秀文, 等. 不同金属离子交换的FAU型分子筛的超极化¹²⁹Xe NMR研究[J]. 催化学报, 2009(9):945-950.
[32] Delahay D B G. Recent advances in Cu^I/IIY:Experiments and modeling[J]. Catalysis Reviews, 2006, 48:269-313.
[33] Maxwell I E, De Boer J J. Crystal structures and dehydrated divalent-copper-exchanged faujasite[J]. The Journal of Physical Chemistry, 1975, 79(17):1874-1879.
[34] Berthomieu D, Jardillier N, Delahay G, et al. Experimental and theoretical approaches to the study of TMI-zeolite (TMI=Fe, Co, Cu)[J]. Catalysis Today, 2005, 110(3-4):294-302.
[35] Torre-Abreu C, Henriques C, Ribeiro F R, et al. Selective catalytic reduction of NO on copper-exchanged zeolites:The role of the structure of the zeolite in the nature of copper-active sites[J]. Catalysis Today, 1999, 54(4):407-418.
[36] Antunes A P, Ribeiro M F, Silva J M, et al. Catalytic oxidation of toluene over CuNaHY zeolites:Coke formation and removal[J]. Applied Catalysis B:Environmental, 2001, 33(2):149-164.
[37] Kieger S, Delahay G, Coq B. et al. Selective catalytic reduction of nitric oxide by ammonia over Cu-FAU catalysts in oxygen-rich atmosphere[J]. Journal of Catalysis, 1999, 183(2):267-280.
[38] 李忠, 付廷俊, 王瑞玉, 等. 高活性甲醇氧化羰基化CuY催化剂的结构及催化活性中心[J]. 高等学校化学学报, 2011(6):1366-1372.
[39] Campos-Martín J M, Guerrero-Ruiz A, Fierro J L G. Changes of copper location in CuY zeolites induced by preparation methods[J]. Catalysis Letters, 1996, 41(1-2):55-61.
[40] Palomino G T, Bordiga S, Zecchina A, et al. XRD, XAS, and IR characterization of copper-exchanged Y zeolite[J]. The Journal of Physical Chemistry B, 2000, 104(36):8641-8651.
[41] 赵地顺. 催化剂评价与表征[M]. 北京:化学工业出版社, 2011:264-274.
[42] Singh R K, Kothiyal G P, Srinivasan A. Electron spin resonance and magnetic studies on CaO-SiO₂-P₂O₅-Na₂O-Fe₂O₃ glasses[J]. Journal of Non-crystalline Solids, 2008, 354(27):3166-3170.
[43] Moreno-González M, Blasco T, Góra-Marek K, et al. Study of propane oxidation on Cu-zeolite catalysts by in-situ EPR and IR spectroscopies[J]. Catalysis Today, 2014, 227:123-129.
[44] Seelan S, Sinha A K, Srinivas D, et al. Spectroscopic investigation and catalytic activity of copper(Ⅱ) phthalocyanine encapsulated in zeolite Y[J]. Journal of Molecular Catalysis A:Chemical, 2000, 157(1-2):163-171.
[45] Yahiro H, Ohmori Y, Shiotani M. Magnetic interaction between copper (Ⅱ) ion and paramagnetic NO and O₂ molecules in Y-type zeolite at low temperature:An EPR study[J]. Microporous and Mesoporous Materials, 2005, 83(1-3):165-171.
[46] Yu J S, Kevan L. Temperature dependence of copper(Ⅱ) migration and formation of new copper(Ⅱ) species during catalytic propylene oxidation on copper(Ⅱ)-exchanged Y zeolite and comparison with X zeolite[J]. The Journal of Physical Chemistry, 1990, 94(19):7612-7620.
[47] Ichikawa T, Kevan L. Location of cupric ions in Y zeolites by electron spin echo spectrometry:Contrast between sodium- and potassium-Y zeolites and comparison with X zeolites[J]. The Journal of Physical Chemistry, 1983, 87(22):4433-4437.
[48] Schoonheydt R A. Transition metal ions in zeolites:Siting and energetics of Cu²⁺[J]. Catalysis Reviews, 1993, 35(1):129-168.
[49] Conesa J C, Soria J. Electron spin resonance of copper-exchanged Y zeolites. Part 1.Behaviour of the cation during dehydration[J]. Journal of the Chemical Society, Faraday Transactions 1:Physical Chemistry in Condensed Phases, 1979, 75:406-422.