CIESC Journal ›› 2019, Vol. 70 ›› Issue (3): 937-943.doi: 10.11949/j.issn.0438-1157.20181083

• Catalysis, kinetics and reactors • Previous Articles     Next Articles

Preparation of palladium-based catalysts by complexing-solvothermal method and catalytic oxidation of m-xylene

Shuai HE1,2(),Feng GUO2(),Guojun KANG1(),Jian YU2,Xuefeng REN1,Guangwen XU3   

  1. 1. Key Laboratory of Coal-based CO2 Capture and Geological Storage, School of Chemical Engineering and Technology, China University of Mining and Technology, Xuzhou 221116, Jiangsu, China
    2. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
    3. Shenyang University of Chemical Technology, Shenyang 110142, Liaoning, China
  • Received:2018-09-26 Revised:2018-12-07 Online:2019-03-05 Published:2018-12-07
  • Contact: Feng GUO,Guojun KANG;;


The Pd/Al2O3 catalysts with a loading of 0.6% (mass fraction) were prepared by complexation-solvent thermal method, hydrothermal method and impregnation method. The effect of different preparation methods on the performance of the catalyst was evaluated by using m-xylene as the representative of volatile organic compounds (VOCs). The results showed that the most effective catalyst Pd/Al2O3-com was prepared by complexing-solvothermal. The m-xylene with volume fraction of 0.002% can completely converted to CO2 and H2O (T100) at 130℃ over Pd/Al2O3-com catalyst from the complexing-solvothermal method, which was lower about 30℃ than the catalyst (Pd/Al2O3-imp) from the impregnation method. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET) and scanning electron microscopy (SEM) techniques were performed to characterize the physico-chemical properties of synthesized Pd/Al2O3 catalysts. The results indicated that the Pd element of Pd/Al2O3-com was mainly dispersed on the surface of the support at the reduction state Pd0, while the Pd element of Pd/Al2O3-imp and Pd/Al2O3-hyd catalyst was at the form of Pd2+ with poor dispersion. Combined with the catalytic activity performance and evaluation results, a highly dispersed and reduction state form of Pd active component on the surface of the carrier resulted in a remarkable catalytic activity on m-xylene conversion. The Pd/Al2O3-com catalyst with these features exhibit good activity for removing VOCs under high concentration (0.02%-0.07%, vol) and wide space velocity (5×104-10×104 h-1) conditions, and thus meet well the requirements of industrial application.

Key words: palladium-based catalyst, catalytic oxidation, volatile organic compounds, complexing-solvothermal method, reduction

CLC Number: 

  • O 643.36


Experimental set-up for catalytic tests"


XRF analysis results for Pd/Al2O3 catalyst/%(mass)"



XRD patterns of Pd/Al2O3 catalyst from different preparation methods"


Adsorption isotherms and desorption isotherms of carrier and Pd/Al2O3 catalyst from different preparation methods"


Pore size distribution of carrier and Pd/Al2O3 catalyst from different preparation methods"


BET surface area, pore volume and pore diameter of carrier and catalysts"



XPS spectra of Pd/Al2O3 catalysts from different preparation methods"


SEM and EDS images of Pd/Al2O3catalysts from different preparation methods"


Catalytic performance of synthesized Pd/Al2O3 from different preparation methods"


Catalytic performance of Pd/Al2O3-com catalyst varied with concentrations and space velocities of m-xylene"


Stability performance of Pd/Al2O3-com(260℃,0.07%(vol.), GHSV:5×104 h-1)"

1 LuC, WeyM, ChenL. Application of polyol process to prepare AC-supported nanocatalyst for VOC oxidation[J]. Applied Catalysis A: General, 2007, 325(1): 163-174.
2 AzizA, ParkH, KimS, et al. Phenol and ammonium removal by using Fe-ZSM-5 synthesized by ammonium citrate iron source [J]. International Journal of Environmental Science and Technology, 2016, 13(12): 2805-2816.
3 ScirèS, LiottaL F. Supported gold catalysts for the total oxidation of volatile organic compounds[J]. Applied Catalysis B: Environmental, 2012, 125(2): 222-246.
4 LiaoY, JiaL, ChenR, et al. Charcoal-supported catalyst with enhanced thermal-stability for the catalytic combustion of volatile organic compounds[J]. Applied Catalysis A: General, 2016, 522: 32-39.
5 芮泽宝, 纪红兵. 有机废气催化燃烧过程中多尺度效应和催化剂设计[J]. 化工学报, 2018, 69(1): 317-326.
RuiZ B, JiH B. Multi-scale effect and catalyst design in catalytic combustion of organic waste gas[J]. CIESC Journal, 2018, 69(1): 317-326.
6 TidahyH, SiffertS, LamonierJ, et al. New Pd/hierarchical macro-mesoporous ZrO2, TiO2 and ZrO2-TiO2 catalysts for VOCs total oxidation[J]. Applied Catalysis A: General, 2006, 310: 61-69.
7 GilA, VicentemA, LambertJ F, et al. Platinum catalysts supported on Al-pillared clays: application to the catalytic combustion of acetone and methyl-ethyl-ketone[J]. Catalysis Today, 2001, 68(1/2/3): 41-51.
8 PozanG S. Effect of support on the catalytic activity of manganese oxide catalysts for toluene combustion[J]. Journal of Hazardous Materials, 2012, 221: 124-130.
9 TangW, DengY, LiW, et al. Importance of porous structure and synergistic effect on the catalytic oxidation activities over hierarchical Mn-Ni composite oxides[J]. Catalysis Science & Technology, 2016, 6(6): 1710-1718.
10 HuC, ZhuQ, JiangZ, et al. Catalytic combustion of dilute acetone over Cu-doped ceria catalysts[J]. Chemical Engineering Journal, 2009, 152(2/3): 583-590.
11 PanH, LiZ, XiaQ, et al. Catalytic activity of copper based catalysts pretreated with H2 reduction for catalytic combustion of styrene[J]. Catalysis Communications, 2009, 10(8): 1166-1169.
12 SedjameH, FontaineC, LafayeG, et al. On the promoting effect of the addition of ceria to platinum based alumina catalysts for VOCs oxidation[J]. Applied Catalysis B: Environmental, 2014, 144: 233-242.
13 HosseiniM, HaghighiM, KahforoushanD, et al. Sono-dispersion of ceria and palladium in preparation and characterization of Pd/Al2O3-clinoptilolite-CeO2 nanocatalyst for treatment of polluted air via low temperature VOC oxidation[J]. Process Safety and Environmental Protection, 2017, 106: 284-293.
14 LiuY, DaiH, DengJ, et al. Mesoporous Co3O4-supported gold nanocatalysts: highly active for the oxidation of carbon monoxide, benzene, toluene, and o-xylene[J]. Journal of Catalysis, 2014, 309: 408-418.
15 Bal ZhinimaevB S, KovalyovE V, KaichevV V, et al. Catalytic abatement of VOC over novel Pt fiber glass catalysts[J]. Topics in Catalysis, 2017, 60(1/2): 73-82.
16 BeckI E, BukhtiyarovV I, ParkharukovI Y, et al. Platinum nanoparticles on Al2O3: correlation between the particle size and activity in total methane oxidation[J]. Journal of Catalysis, 2009, 268(1): 60-67.
17 KomvokisV G, MartiM, DelimitisA, et al. Catalytic decomposition of N2O over highly active supported Ru nanoparticles (≤3 nm) prepared by chemical reduction with ethylene glycol[J]. Applied Catalysis B: Environmental, 2011, 103(1/2): 62-71.
18 HuangS, ZhangC, HeH. Complete oxidation of o-xylene over Pd/Al2O3 catalyst at low temperature[J]. Catalysis Today, 2008, 139(1/2): 15-23.
19 胡凌霄, 王莲, 王飞, 等. Pd/γ-Al2O3催化剂催化氧化邻-二甲苯[J]. 物理化学学报, 2017, 33(8): 1681-1688.
HuL X, WangL, WangF, et al. Catalytic oxidation of o-xylene over Pd/ γ -Al2O3 catalysts[J]. Acta Physico-Chimica Sinica, 2017, 33 (8): 1681-1688.
20 ÖztürkS, KösemenA, KösemenZ A, et al. Electrochemically growth of Pd doped ZnO nanorods on QCM for room temperature VOC sensors[J]. Sensors and Actuators B: Chemical, 2016, 222: 280-289.
21 KimJ, ParlJ, KimH S, et al. A new route to preparation of palladium catalysts for VOC combustion[J]. Journal of Industrial and Engineering Chemistry, 2012, 18(1): 425-428.
22 OńskaM J, KrólA, C E K, et al. Zeolites Y modified with palladium as effective catalysts for low-temperature methanol incineration[J]. Applied Catalysis B: Environmental, 2015, 166: 353-365.
23 HuangS, ZhangC, HeH. Effect of pretreatment on Pd/Al2O3 catalyst for catalytic oxidation of o-xylene at low temperature[J].Journal of Environmental Sciences, 2013, 25(6): 1206-1212.
24 BarakatT, RookeJ C, CousinR, et al. Investigation of the elimination of VOC mixtures over a Pd-loaded V-doped TiO2 support[J]. New Journal of Chemistry, 2014, 38(5): 266-274.
25 DemoulinO, RupprechterG, SeunierI, et al. Investigation of parameters influencing the activation of a Pd/γ-Alumina catalyst during methane combustion[J]. The Journal of Physical Chemistry B, 2005, 109(43): 20454-20462.
26 PadillaJ M, Del AngelG, NavarreteJ. Improved Pd/γ-Al2O3-Ce catalysts for benzene combustion[J]. Catalysis Today, 2008, 133/134/135: 541-547.
27 KimS C, ShimW G. Properties and performance of Pd based catalysts for catalytic oxidation of volatile organic compounds[J]. Applied Catalysis B: Environmental, 2009, 92(3/4): 429-436.
28 HuangH, LeungD Y C. Complete oxidation of formaldehyde at room temperature using TiO2 supported metallic Pd nanoparticles[J]. ACS Catalysis, 2011, 1(4): 348-354.
29 WangY, ZhangC, HeH. Insight into the role of Pd state on Pd-based catalysts in o-xylene oxidation at low temperature[J]. ChemCatChem, 2018, 10(5): 998-1004.
30 夏燎原, 吴义强, 胡云楚. 锡掺杂介孔分子筛在木材阻燃中的烟气转化作用[J]. 无机材料学报, 2013, 28(5): 532-536.
XiaL Y, WuY Q, HuC Y. Study on smoke catalytic conversion by Sn-substituted mesoporous silica composite in wood fire retardance[J]. Journal of Inorganic Materials, 2013, 28(5): 532-536.
31 叶青, 霍飞飞, 王海平, 等. xAu/α-MnO2催化剂的结构及催化氧化VOCs气体性能[J]. 高等学校化学学报, 2013, 34(5): 1187-1194.
YeQ, HuoF F, WangH P, et al. Structure of xAu/α-MnO2 catalyst and performance of catalytic oxidation of VOCs[J]. Chemical Journal of Chinese Universities, 2013, 34(5): 1187-1194.
32 ShimW G, LeeJ W, KimS C. Analysis of catalytic oxidation of aromatic hydrocarbons over supported palladium catalyst with different pretreatments based on heterogeneous adsorption properties[J]. Applied Catalysis B: Environmental, 2008, 84(1/2): 133-141.
33 KundakovicL, Flytzani-StephanoulosM. Reduction characteristics of copper oxide in cerium and zirconium oxide systems[J]. Applied Catalysis A: General, 1998, 171(1): 13-29.
34 陈静, 张庆红, 方文浩, 等. 水滑石负载钯催化剂上的醇无氧脱氢反应[J]. 催化学报, 2010, 31(8): 1061-1070.
ChenJ, ZhangQ H, FangW H, et al. Oxidant-free dehydrogenation of alcohols over hydrotalcite-supported palladium catalysts[J]. Chinese Journal of Catalysis, 2010, 31(8): 1061-1070.
35 HiraiH, ChawanyaH, ToshimaN. Colloidal palladium protected with poly (N-vinyl-2-pyrrolidone) for selective hydrogenation of cyclopentadiene[J]. Reactive Polymers, 1985, 3(2): 127-141.
36 RobertsG W, SatterfieldC N. Effectiveness factor for porous catalysts Langmuir-Hinshelwood kinetic expressions [J]. Industrial & Engineering Chemistry Fundamentals, 1966, 5(3): 317-325.
37 KratzerP, BreningW. Highly excited molecules from Eley-Rideal reactions[J]. Surface Science Letters, 1991, 254(1/2/3): 275-280.
38 SaqlainM A, HussainA, SiddiqM, et al. A DFT+U study of the mars van Krevelen mechanism of CO oxidation on Au/TiO2 catalysts[J]. Applied Catalysis A: General, 2016, 519: 27-33.
[1] Junqiang WU, Wenming JIANG, Shilin DU, Yang LIU. Experiment on drag reduction of heavy oil in horizontal pipeline by water annular conveying [J]. CIESC Journal, 2019, 70(5): 1734-1741.
[2] Yongjian WU, Chunhuan LUO, Lin WEI, Tanjin ZHU, Qingquan SU. Utilization of converter off-gas based on chemical-looping combustion [J]. CIESC Journal, 2019, 70(5): 1923-1931.
[3] Wensheng LIANG, Jiangtao LIU, Yue ZHAO, Wei HUANG, Zhijun ZUO. Theoretical calculation of effect of NiO and Ni catalysts for benzoic acid pyrolysis [J]. CIESC Journal, 2019, 70(4): 1429-1435.
[4] Desheng LI, Chao ZHANG, Shihai DENG, Zhifeng HU, Jinlong LI, Yuanhui LIU. Experimental study on effective nitrate removal from sewage by ZVI-based catalyzed reduction [J]. CIESC Journal, 2019, 70(3): 1065-1074.
[5] Dehui LEI, Tongjiang PENG, Hongjuan SUN, Guangping TANG, Jianzhao YANG, Yazhou REN, Lili WANG. Influence of reduction temperature of graphene oxide on cross sensitivity between humidity and formaldehyde [J]. CIESC Journal, 2019, 70(1): 309-318.
[6] Lulu PAN, Danjing WU, Weiping LIU. Electrical performance of MFC-MEC coupling system and treatment of heavy metal wastewater containing cadmium [J]. CIESC Journal, 2019, 70(1): 242-250.
[7] LI Yi, ZHANG Xiaosong. Influencing factors of direct oxygen enrichment device based on electro-osmosis [J]. CIESC Journal, 2018, 69(S2): 388-393.
[8] LI Dianxin, HU Nan, HUANG Chao, DING Dexin, LI Guangyue, WANG Yongdong. Experimental study on U(Ⅵ) bioreduction by incubated sulfate reducing bacteria sediment in groundwater [J]. CIESC Journal, 2018, 69(8): 3619-3625.
[9] WU Yuhui, YANG Yuesuo, ZHAO Chuanqi, ZHANG Xi, CHEN Yu, XU Bin. A review on effects of extracellular polymeric substances on contaminants fate & transport in soil and water environment [J]. CIESC Journal, 2018, 69(8): 3303-3317.
[10] JING Jiaqiang, YIN Ran, MA Xiaoliang, SUN Jie, WU Xi. Drag characteristics of air-mixed heavy oil in horizontal pipes [J]. CIESC Journal, 2018, 69(8): 3398-3407.
[11] PU Ge, DU Jiantai, ZHANG Zhang, ZHANG Dinghai, WU Bang, HUANG Beibei, ZHU Tuanhui. Experimental study of selective non-catalytic reduction process with methylamine as reducing agent [J]. CIESC Journal, 2018, 69(7): 3234-3241.
[12] FAN Peng, CHEN Jie, GUAN Xiaohong, QIAO Junlian. Enhanced nitrobenzene removal by persulfate-assisted zerovalent iron [J]. CIESC Journal, 2018, 69(5): 2175-2182.
[13] CHANG Jing, HU Xiude, TIAN Hongjing, YUAN Fuqi, XU Jingwen, GUO Qingjie. Simulation and experimental study on smelter off-gas desulfurization using calcium-based desulfurizer [J]. CIESC Journal, 2018, 69(5): 2233-2241.
[14] QI Hang, ZHANG Wei, GONG Liang. Liquid film flow and heat transfer model under spray impact [J]. CIESC Journal, 2018, 69(5): 2014-2022.
[15] HUA Feng, FANG Zhou, QIU Tong. Recirculation and reaction hybrid intelligent modeling and simulation for industrial ethylene cracking furnace [J]. CIESC Journal, 2018, 69(3): 923-930.
Full text



[1] LING Lixia, ZHANG Riguang, WANG Baojun, XIE Kechang. Pyrolysis Mechanisms of Quinoline and Isoquinoline with Density Functional Theory[J]. , 2009, 17(5): 805 -813 .
[2] LEI Zhigang, LONG Aibin, JIA Meiru, LIU Xueyi. Experimental and Kinetic Study of Selective Catalytic Reduction of NO with NH3 over CuO/Al2O3/Cordierite Catalyst[J]. , 2010, 18(5): 721 -729 .
[3] SU Haifeng, LIU Huaikun, WANG Fan, LÜXiaoyan, WEN Yanxuan. Kinetics of Reductive Leaching of Low-grade Pyrolusite with Molasses Alcohol Wastewater in H2SO4[J]. , 2010, 18(5): 730 -735 .
[4] WANG Jianlin, XUE Yaoyu, YU Tao, ZHAO Liqiang. Run-to-run Optimization for Fed-batch Fermentation Process with Swarm Energy Conservation Particle Swarm Optimization Algorithm[J]. , 2010, 18(5): 787 -794 .
[5] SUN Fubao, MAO Zhonggui, ZHANG Jianhua, ZHANG Hongjian, TANG Lei, ZHANG Chengming, ZHANG Jing, ZHAI Fangfang. Water-recycled Cassava Bioethanol Production Integrated with Two-stage UASB Treatment[J]. , 2010, 18(5): 837 -842 .
[6] Gao Ruichang, Song Baodong and Yuan Xiaojing( Chemical Engineering Research Center, Tianjin University, Tianjin 300072). LIQUID FLOW DISTRIBUTION IN GAS - LIQUID COUNTER - CONTACTING PACKED COLUMN[J]. , 1999, 50(1): 94 -100 .
[7] Su Yaxin, Luo Zhongyang and Cen Kefa( Institute of Thermal Power Engineering , Zhejiang University , Hangzhou 310027). A STUDY ON THE FINS OF HEAT EXCHANGERS FROM OPTIMIZATION OF ENTROPY GENERATION[J]. , 1999, 50(1): 118 -124 .
[8] Luo Xiaoping(Department of Industrial Equipment and Control Engineering , South China University of Technology, Guangzhou 510641)Deng Xianhe and Deng Songjiu( Research Institute of Chemical Engineering, South China University of Technology, Guangzhou 5106. RESEARCH ON FLOW RESISTANCE OF RING SUPPORT HEAT EXCHANGER WITH LONGITUDINAL FLUID FLOW ON SHELL SIDE[J]. , 1999, 50(1): 130 -135 .
[9] Jin Wenzheng , Gao Guangtu , Qu Yixin and Wang Wenchuan ( College of Chemical Engineering, Beijing Univercity of Chemical Technology, Beijing 100029). MONTE CARLO SIMULATION OF HENRY CONSTANT OF METHANE OR BENZENE IN INFINITE DILUTE AQUEOUS SOLUTIONS[J]. , 1999, 50(2): 174 -184 .

LI Qingzhao;ZHAO Changsui;CHEN Xiaoping;WU Weifang;LI Yingjie


Combustion of pulverized coal in O2/CO2 mixtures and its pore structure development

[J]. , 2008, 59(11): 2891 -2897 .