炭载体对Pt-C复合物非碱性条件下催化甘油氧化性能的影响

doi:10.11949/j.issn.0438-1157.20161026

化工学报 ›› 2017, Vol. 68 ›› Issue (2): 679-686.DOI: 10.11949/j.issn.0438-1157.20161026

• 催化、动力学与反应器 • 上一篇下一篇

炭载体对Pt-C复合物非碱性条件下催化甘油氧化性能的影响

雷佳契, 段学志, 钱刚, 周兴贵

化学工程联合国家重点实验室, 华东理工大学化工学院, 上海 200237

收稿日期:2016-07-21 修回日期:2016-12-16 出版日期:2017-02-05 发布日期:2017-02-05
通讯作者: 周兴贵
基金资助:
国家自然科学基金项目（21306046）；化学工程联合国家重点实验室开放课题项目（SKL-ChE-15C03）。

Effects of carbon support on glycerol oxidation over Pt-C composite catalysts in base-free conditions

LEI Jiaqi, DUAN Xuezhi, QIAN Gang, ZHOU Xinggui

State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2016-07-21 Revised:2016-12-16 Online:2017-02-05 Published:2017-02-05
Supported by:
supported by the National Natural Science Foundation of China (21306046) and the Open Project of State Key Laboratory of Chemical Engineering (SKL-ChE-15C03).

摘要/Abstract

摘要：

采用等量浸渍法制备了具有相似平均粒径的活性炭（AC）和碳纳米管（CNTs）负载的Pt催化剂，并比较研究了非碱性条件下两种催化剂催化甘油氧化反应的性能。结果表明，炭载体对Pt-C复合物催化甘油氧化反应的活性、选择性和稳定性有重要影响。相对于Pt/CNTs催化剂，Pt/AC催化剂中Pt 4f结合能较低，导致其表面氧的覆盖度相对较高，因而抑制了甘油的吸附，降低了甘油氧化反应的初始活性；Pt/AC催化剂会促进甘油醛进一步氧化成甘油酸以及C₃产物的氧化断键；Pt/AC催化剂失活的主要原因是氧中毒和中间产物的吸附，而Pt/CNTs催化剂的失活主要是由于甘油酸的吸附堵塞Pt表面的活性位造成的。

关键词: 甘油, 氧化, Pt-C复合物, 载体, 失活

Abstract:

Activated carbon (AC) and carbon nanotubes (CNTs) supported Pt catalysts with similar particle sizes prepared by incipient wetness impregnation method were used for study of base-free oxidation of glycerol. The results showed that carbon support of Pt-C composite catalysts had significant impact on reactivity, selectivity, and steady state of glycerol oxidation. Compared to Pt/CNTs catalyst, Pt/AC catalyst had a lower binding energy of Pt 4f leading to a higher oxygen coverage on catalyst surface which reduced glycerol adsorption and initial activity of glycerol oxidation. Pt/AC catalyst further favored oxidation of glyceraldehyde to glyceric acid and C-C bond cleavage of C₃ products. With regards to catalyst deactivation, oxygen poison and adsorption of intermediates were main factors to Pt/AC catalyst while blockage of Pt active sites by adsorption of glyceric acid was a significant contributor to Pt/CNTs catalyst.

Key words: glycerol, oxidation, Pt-C composite, support, deactivation

中图分类号:

TQ203.2

雷佳契, 段学志, 钱刚, 周兴贵. 炭载体对Pt-C复合物非碱性条件下催化甘油氧化性能的影响[J]. 化工学报, 2017, 68(2): 679-686.

LEI Jiaqi, DUAN Xuezhi, QIAN Gang, ZHOU Xinggui. Effects of carbon support on glycerol oxidation over Pt-C composite catalysts in base-free conditions[J]. CIESC Journal, 2017, 68(2): 679-686.

参考文献 31

[1]	HUBER G W, IBPRRA S, CORMA A. Synthesis of transportation fuels from biomass:chemistry, catalysts, and engineering[J]. Chem. Rev., 2006, 106(9):4044-4098.
[2]	BEHR A, EILTING J, IRAWADI K, et al. Improved utilisation of renewable resources:new important derivatives of glycerol[J]. Green Chem., 2008, 10(1):13-30.
[3]	CZERNIK S, FRENCH R, FEIK C, et al. Hydrogen by catalytic steam reforming of liquid byproducts from biomass thermoconversion processes[J]. Ind. Eng. Chem. Res., 2002, 41:4209-4215.
[4]	ZHOU C H, BELTRAMINI N J, FAN Y X, et al. Chemoselective catalytic conversion of glycerol as a biorenewable source to valuable commodity chemicals[J]. Chem. Soc. Rev., 2008, 37(3):527-549.
[5]	KATRYNIOK B, KIMURA H, SKRZYNSKA E, et al. Selective catalytic oxidation of glycerol:perspectives for high value chemicals[J]. Green Chem., 2011, 13(8):1960-1979.
[6]	DAVIS W R, TOMSHO J, NIKAM S, et al. Inhibition of HIV-1 reverse transcriptase-catalyzed DNA strand transfer reactions by 4-chlorophenylhydrazone of mesoxalic acid[J]. Biochemistry, 2000, 39(46):14279-14291.
[7]	KIMURA H, TSUTO K. Catalytic synthesis of DL-serine and glycine from glycerol[J]. J. Am. Oil Chem. Soc., 1993, 70(10):1027-1030.
[8]	ZOPE B N, HIBBITTS D D, NEUROCK M, et al. Reactivity of the gold/water interface during selective oxidation catalysis[J]. Science, 2010, 330(6000):74-78.
[9]	VILLA A, VEITH G M, PRATI L. Selective oxidation of glycerol under acidic conditions using gold catalysts[J]. Angew. Chem. Int. Ed., 2010, 49(26):4499-4502.
[10]	TSUJI A, RAO K T V, NISHIMURA S, et al. Selective oxidation of glycerol by using a hydrotalcite-supported platinum catalyst under atmospheric oxygen pressure in water[J]. ChemSusChem, 2011, 4(4):542-548.
[11]	LIU S S, SUN K Q, XU B Q. Specific selectivity of Au-catalyzed oxidation of glycerol and other C3-polyols in water without the presence of a base[J]. ACS Catal., 2014, 4(7):2226-2230.
[12]	YUAN Z F, GAO Z K, XU B Q. Acid-base property of the supporting material controls the selectivity of Au catalyst for glycerol oxidation in base-free water[J]. Chinese J. Catal., 2015, 36(9):1543-1551.
[13]	BRETT G L, HE Q, HAMMOND C, et al. Selective oxidation of glycerol by highly active bimetallic catalysts at ambient temperature under base-free conditions[J]. Angew. Chem. Int. Ed., 2011, 50(43):10136-10139.
[14]	HIRASAWA S, WATANABE H, KIZUKA T, et al. Performance, structure and mechanism of Pd-Ag alloy catalyst for selective oxidation of glycerol to dihydroxyacetone[J]. J. Catal., 2013, 300:205-216.
[15]	GARCIA R, BESSON M, GALLEZOT P. Chemoselective catalytic oxidation of glycerol with air on platinum metals[J]. Appl. Catal. A:Gen., 1995, 127(1/2):165-176.
[16]	LEI J Q, DUAN X Z, QIAN G, et al. Size effects of Pt nanoparticles supported on carbon nanotubes for selective oxidation of glycerol in a base-free condition[J]. Ind. Eng. Chem. Res., 2014, 53(42):16309-16315.
[17]	LEI J Q, DUAN X Z, QIAN G, et al. Insights into activated carbon-supported platinum catalysts for base-free oxidation of glycerol[J]. Ind. Eng. Chem. Res., 2016, 55(2):420-427.
[18]	RODRIGUES E G, PEREIRA M F, CHEN X W, et al. Selective oxidation of glycerol over platinum-based catalysts supported on carbon nanotubes[J]. Ind. Eng. Chem. Res., 2013, 52(49):17390-17398.
[19]	GAO J, LIANG D, CHEN P, et al. Oxidation of glycerol with oxygen in a base-free aqueous solution over Pt/AC and Pt/MWNTs catalysts[J]. Catal. Lett., 2009, 130(1/2):185-191.
[20]	DAN L, GAO J, WANG J H, et al. Selective oxidation of glycerol with oxygen in a base-free aqueous solution over MWNTs supported Pt catalysts[J]. Appl. Catal. B:Environ., 2011, 106:423-432.
[21]	SERP P, CORRIAS M, KALCK P. Carbon nanotubes and nanofibers in catalysis[J]. Appl. Catal. A:Gen., 2003, 253(2):337-358.
[22]	ROY A K, HSIEH C T. Pulse microwave-assisted synthesis of Pt nanoparticles onto carbon nanotubes as electrocatalysts for proton exchange membrane fuel cells[J]. Electrochimica Acta, 2013, 87:63-72.
[23]	ZENG J H, SU F B, LEE J Y, et al. Method for preparing highly dispersed Pt catalysts on mesoporous carbon support[J]. J. Mater. Sci., 2007, 42:7191-7197.
[24]	ZHANG M Y, NIE R F, WANG L, et al. Selective oxidation of glycerol over carbon nanofibers supported Pt catalysts in a base-free aqueous solution[J]. Chem. Commun., 2015, 59:5-9.
[25]	LI Y, ZAERA F. Sensitivity of the glycerol oxidation reaction to the size and shape of the platinum nanoparticles in Pt/SiO2 catalysts[J]. J. Catal., 2015, 326:116-126.
[26]	KNUPP S L, LI W Z, PASCHOS O, et al. The effect of experimental parameters on the synthesis of carbon nanotube/nanofiber supported platinum by polyol processing techniques[J]. Carbon, 2008, 46(10):1276-1284.
[27]	CHEN W Y, JI J, DUAN X Z, et al. Unique reactivity in Pt/CNTs catalyzed hydrolytic dehydrogenation of ammonia borane[J]. Chem. Commun., 2014, 50:2142-2144.
[28]	CARRETTIN S, MCMORN P, JOHNSTON P, et al. Oxidation of glycerol using supported Pt, Pd and Au catalysts[J]. Phys. Chem. Chem. Phys., 2003, 5(6):1329-1336.
[29]	MALLAT T, BAIKER A. Oxidation of alcohols with molecular oxygen on platinum metal catalysts in aqueous solutions[J]. Catal. Today, 1994, 19(2):247-283.
[30]	MARKUSSE A P, KUSTER B F M, KONINGSBERGER D C, et al. Platinum deactivation:in situ EXAFS during aqueous alcohol oxidation reaction[J]. Catal. Lett., 1998, 55(3):141-145.
[31]	BESSON M, GALLEZOT P. Selective oxidation of alcohols and aldehydes on metal catalysts[J]. Catal. Today, 2000, 57:127-141.

炭载体对Pt-C复合物非碱性条件下催化甘油氧化性能的影响

Effects of carbon support on glycerol oxidation over Pt-C composite catalysts in base-free conditions

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