doi:10.1007/s11705-016-1583-1

Frontiers of Chemical Science and Engineering

2016, Vol. 10

Issue (3): 417-424 https://doi.org/10.1007/s11705-016-1583-1

本期目录

Effect of thermal pretreatment on the surface structure of PtSn/SiO₂ catalyst and its performance in acetic acid hydrogenation

Guozhen Xu,Jian Zhang(

),Shengping Wang,Yujun Zhao(

),Xinbin Ma

Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Centre of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

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Abstract：

The effect of thermal pretreatment on the active sites and catalytic performances of PtSn/SiO₂ catalyst in acetic acid (AcOH) hydrogenation was investigated in this article. The catalysts were characterized by N₂ physical adsorption, X-ray diffraction, transmission electron microscopy, pyridine Fourier-transform infrared spectra, and H₂-O₂ titration on its physicochemical properties. The results showed that Pt species were formed primarily in crystalline structure and no PtSn_x alloy was observed. Meanwhile, with the increment of thermal pretreatment temperature, Pt dispersion showed a decreasing trend due to the aggregation of Pt particles. Simultaneously, the amount of Lewis acid sites was remarkably influenced by such thermal pretreatment owning to the consequent physicochemical property variation of Sn species. Interestingly, the catalytic activity showed the similar variation trend with that of Lewis acid sites, confirming the important roles of Lewis acid sites in AcOH hydrogenation. Moreover, a balancing effect between exposed Pt and Lewis acid sites was obtained, resulting in the superior catalytic performance in AcOH hydrogenation.

Key words： thermal pretreatment acetic acid hydrogenation ethanol PtSn/SiO₂

收稿日期: 2016-04-19 出版日期: 2016-08-23

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Corresponding Author(s): Jian Zhang,Yujun Zhao

引用本文:

. [J]. Frontiers of Chemical Science and Engineering, 2016, 10(3): 417-424.
Guozhen Xu, Jian Zhang, Shengping Wang, Yujun Zhao, Xinbin Ma. Effect of thermal pretreatment on the surface structure of PtSn/SiO₂ catalyst and its performance in acetic acid hydrogenation. Front. Chem. Sci. Eng., 2016, 10(3): 417-424.

链接本文:

https://academic.hep.com.cn/fcse/CN/10.1007/s11705-016-1583-1
https://academic.hep.com.cn/fcse/CN/Y2016/V10/I3/417

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1	Goldemberg J. Ethanol for a sustainable energy future. Science, 2007, 315(5813): 808–810 https://doi.org/10.1126/science.1137013
2	Goldemberg J. Special issue on sustainability and energy. Perspectives: Ethanol for a sustainable energy future. Science, 2007, 317(5843): 1325
3	Gong J, Yue H, Zhao Y, Zhao S, Zhao L, Lv J, Wang S, Ma X. Synthesis of ethanol via syngas on Cu/SiO2 catalysts with balanced Cu0-Cu+ sites. Journal of the American Chemical Society, 2012, 134(34): 13922–13925 https://doi.org/10.1021/ja3034153
4	Zhang S, Duan X, Ye L, Lin H, Xie Z, Yuan Y. Production of ethanol by gas phase hydrogenation of acetic acid over carbon nanotube-supported Pt-Sn nanoparticles. Catalysis Today, 2013, 215: 260–266 https://doi.org/10.1016/j.cattod.2013.05.002
5	Zhang K, Zhang H, Ma H, Ying W, Fang D. Effect of Sn addition in gas phase hydrogenation of acetic acid on alumina supported PtSn catalysts. Catalysis Letters, 2014, 144(4): 691–701 https://doi.org/10.1007/s10562-014-1210-z
6	Rachmady W, Vannice M A. Acetic acid reduction to acetaldehyde over iron catalysts II. Characterization by Mossbauer spectroscopy, DRIFTS, TPD, and TPR. Journal of Catalysis, 2002, 208(1): 170–179 https://doi.org/10.1006/jcat.2002.3561
7	Rachmady W, Vannice M A. Acetic acid reduction by H2 on bimetallic Pt-Fe catalysts. Journal of Catalysis, 2002, 209(1): 87–98 https://doi.org/10.1006/jcat.2002.3623
8	Margitfalvi J L, Vankó G, Borbáth I, Tompos A, Vértes A. Characterization of Sn-Pt/SiO2 catalysts used in selective hydrogenation of crotonaldehyde by Mössbauer spectroscopy. Journal of Catalysis, 2000, 190(2): 474–477 https://doi.org/10.1006/jcat.1999.2775
9	Serrano-Ruiz J C, Huber G W, Sanchez-Castillo M A, Dumesic J A, Rodriguez-Reinoso F, Sepulveda-Escribano A. Effect of Sn addition to Pt/CeO2-Al2O3 and Pt/Al2O3 catalysts: An XPS, Sn-119 Mossbauer and microcalorimetry study. Journal of Catalysis, 2006, 241(2): 378–388 https://doi.org/10.1016/j.jcat.2006.05.005
10	Taniya K, Jinno H, Kishida M, Ichihashi Y, Nishiyama S. Preparation of Sn-modified silica-coated Pt catalysts: A new PtSn bimetallic model catalyst for selective hydrogenation of crotonaldehyde. Journal of Catalysis, 2012, 288: 84–91 https://doi.org/10.1016/j.jcat.2012.01.006
11	Onyestyák G, Harnos S, Kaszonyi A, Štolcová M, Kalló D. Acetic acid hydroconversion to ethanol over novel InNi/Al2O3 catalysts. Catalysis Communications, 2012, 27: 159–163 https://doi.org/10.1016/j.catcom.2012.07.021
12	Rachmady W, Vannice M A. Acetic acid reduction by H2 over supported Pt catalysts: A DRIFTS and TPD/TPR Study. Journal of Catalysis, 2002, 207(2): 317–330 https://doi.org/10.1006/jcat.2002.3556
13	Chen L G, Li Y P, Zhang X H, Zhang Q, Wang T J, Ma L L. Mechanistic insights into the effects of support on the reaction pathway for aqueous-phase hydrogenation of carboxylic acid over the supported Ru catalysts. Applied Catalysis A, General, 2014, 478: 117–128 https://doi.org/10.1016/j.apcata.2014.03.038
14	Brewster T P, Miller A J M, Heinekey D M, Goldberg K I. Hydrogenation of carboxylic acids catalyzed by half-sandwich complexes of iridium and rhodium. Journal of the American Chemical Society, 2013, 135(43): 16022–16025 https://doi.org/10.1021/ja408149n
15	Goguet A, Schweich D, Candy J P. Preparation of a Pt/SiO2 catalyst: II. Temperature-programmed decomposition of the adsorbed platinum tetrammine hydroxide complex under flowing hydrogen, oxygen, and argon. Journal of Catalysis, 2003, 220(2): 280–290 https://doi.org/10.1016/S0021-9517(03)00189-1
16	Miller J T, Schreier M, Kropf A J, Regalbuto J R. A fundamental study of platinum tetraammine impregnation of silica: 2. The effect of method of preparation, loading, and calcination temperature on (reduced) particle size. Journal of Catalysis, 2004, 225(1): 203–212 https://doi.org/10.1016/j.jcat.2004.04.007
17	Emeis C A. Determination of integrated molar extinction coefficients for infrared absorption bands of pyridine adsorbed on solid acid catalysts. Journal of Catalysis, 1993, 141(2): 347–354 https://doi.org/10.1006/jcat.1993.1145
18	Li D, Zeng L, Li X Y, Wang X, Ma H Y, Assabumrungrat S, Gong J L. Ceria-promoted Ni/SBA-15 catalysts for ethanol steam reforming with enhanced activity and resistance to deactivation. Applied Catalysis B: Environmental, 2015, 176: 532–541 https://doi.org/10.1016/j.apcatb.2015.04.020
19	Kwak D H, Lee Y W, Han S B, Hwang E T, Park H C, Kim M C, Park K W. Ultrasmall PtSn alloy catalyst for ethanol electro-oxidation reaction. Journal of Power Sources, 2015, 275: 557–562 https://doi.org/10.1016/j.jpowsour.2014.11.050
20	Zhu H, Anjum D H, Wang Q, Abou-Hamad E, Emsley L, Dong H, Laveille P, Li L, Samal A K, Basset J M. Sn surface-enriched Pt-Sn bimetallic nanoparticles as a selective and stable catalyst for propane dehydrogenation. Journal of Catalysis, 2014, 320: 52–62 https://doi.org/10.1016/j.jcat.2014.09.013
21	Oudenhuijzen M K, Kooyman P J, Tappel B, van Bokhoven J A, Koningsberger D C. Understanding the influence of the pretreatment procedure on platinum particle size and particle-size distribution for SiO2 impregnated with [Pt2+(NH3)4](NO3−)2: A Combination of HRTEM, Mass spectrometry, and Quick EXAFS. Journal of Catalysis, 2002, 205(1): 135–146 https://doi.org/10.1006/jcat.2001.3433
22	Liu Z, Jackson G S, Eichhorn B W. PtSn intermetallic, core-shell, and alloy nanoparticles as CO-tolerant electrocatalysts for H2 oxidation. Angewandte Chemie International Edition, 2010, 49(18): 3173–3176 https://doi.org/10.1002/anie.200907019
23	Wang Z Q, Li G Y, Liu X Y, Huang Y Q, Wang A Q, Chu W, Wang X D, Li N. Aqueous phase hydrogenation of acetic acid to ethanol over Ir-MoOx/SiO2 catalyst. Catalysis Communications, 2014, 43: 38–41 https://doi.org/10.1016/j.catcom.2013.09.007
24	Neri G, Rizzo G, Arico A S, Crisafulli C, De Luca L, Donato A, Musolino M G, Pietropaolo R. One-pot synthesis of naturanol from α-pinene oxide on bifunctional Pt-Sn/SiO2 heterogeneous catalysts Part I: The catalytic system. Applied Catalysis A, General, 2007, 325(1): 15–24 https://doi.org/10.1016/j.apcata.2007.02.026
25	Sun J, Zhu K, Gao F, Wang C, Liu J, Peden C H, Wang Y. Direct conversion of bio-ethanol to isobutene on nanosized ZnxZryOz mixed oxides with balanced acid-base sites. Journal of the American Chemical Society, 2011, 133(29): 11096–11099 https://doi.org/10.1021/ja204235v
26	Zhan H M, Huang S Y, Li Y, Lv J, Wang S P, Ma X B. Elucidating the nature and role of Cu species in enhanced catalytic carbonylation of dimethyl ether over Cu/H-MOR. Catalysis Science & Technology, 2015, 5(9): 4378–4389 https://doi.org/10.1039/C5CY00460H
27	Pallassana V, Neurock M. Reaction paths in the hydrogenolysis of acetic acid to ethanol over Pd(111), Re(0001), and PdRe alloys. Journal of Catalysis, 2002, 209(2): 289–305 https://doi.org/10.1006/jcat.2002.3585
28	Rachmady W, Vannice M A. Acetic acid reduction to acetaldehyde over iron catalysts: I. kinetic behavior. Journal of Catalysis, 2002, 208(1): 158–169 https://doi.org/10.1006/jcat.2002.3560

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[1]	. [J]. Front. Chem. Sci. Eng., 2017, 11(1): 139-142.
[2]	. [J]. Front. Chem. Sci. Eng., 2017, 11(1): 107-116.
[3]	. [J]. Front. Chem. Sci. Eng., 2017, 11(1): 133-138.
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[15]	. [J]. Front. Chem. Sci. Eng., 2016, 10(1): 16-38.

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