不同Pt前体制备Pt/CeO<sub>2</sub>催化剂对其结构及性能的影响

席康; 王勇; 谢晶; 王宁; 周瑛; 朱秋莲; 卢晗锋

doi:10.11949/0438-1157.20190468

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不同Pt前体制备Pt/CeO₂催化剂对其结构及性能的影响

催化、动力学与反应器 | 更新时间：2020-06-24

- 不同Pt前体制备Pt/CeO₂催化剂对其结构及性能的影响
- Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts
- 化工学报 2019年70卷第11期页码：4278-4288
- 作者机构：
  
  浙江工业大学化学工程学院，浙江杭州 310014
- 作者简介：
  
  席康（1996—），男，硕士研究生，1648812238@qq.com
  卢晗锋（1977—），男，博士，教授，luhf@zjut.edu.cn
- 基金信息：
  
  国家自然科学基金项目(21506194;21676255);浙江省自然科学基金项目(Y16B070025)
- DOI：10.11949/0438-1157.20190468
  中图分类号： TQ 133.3;TQ 138.2⁺6
- 收稿：2019-05-06，
  
  修回：2019-06-15，
  
  纸质出版：2019-11-05
- 稿件说明：
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席康, 王勇, 谢晶, 王宁, 周瑛, 朱秋莲, 卢晗锋. 不同Pt前体制备Pt/CeO₂催化剂对其结构及性能的影响[J]. 化工学报, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468.

XI Kang, WANG Yong, XIE Jing, WANG Ning, ZHOU Ying, ZHU Qiulian, LU Hanfeng. Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts[J]. CIESC Journal, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468.
席康, 王勇, 谢晶, 王宁, 周瑛, 朱秋莲, 卢晗锋. 不同Pt前体制备Pt/CeO₂催化剂对其结构及性能的影响[J]. 化工学报, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468. DOI：

XI Kang, WANG Yong, XIE Jing, WANG Ning, ZHOU Ying, ZHU Qiulian, LU Hanfeng. Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts[J]. CIESC Journal, 2019, 70(11): 4278-4288 DOI: 10.11949/0438-1157.20190468. DOI：

摘要

Pt与载体间的相互作用会影响到本征Pt纳米粒子的催化活性，不同Pt前体制备Pt/CeO

催化剂会使其表现出完全不同的催化性能。分别采用金属胶体粒子原位沉积法、浸渍法以及浸渍还原的方式制备了Pt/CeO

催化剂，通过X 射线衍射、程序升温还原、X射线光电子能谱以及高分辨透射电镜对催化剂进行表征，在CO氧化以及甲苯燃烧反应中评价催化剂活性。结果表明，胶体粒子原位沉积法制备Pt/CeO

催化剂，能够将优先合成好的Pt纳米粒子直接以金属态Pt

的形式负载到载体表面，且保证其高度均匀分散，丰富的表面Pt

很好地充当了CO、甲苯反应时的活化位点，催化剂表现出优异的性能；浸渍还原法中，Pt纳米粒子之间会发生团聚现象，同时部分Pt又以Pt

的形式与CeO

之间形成了Pt-O-Ce相互作用，载体表面暴露Pt

含量的下降是催化剂表现出较弱活性的主要原因；浸渍法中，以Pt离子对Pt进行负载，Pt完全以Pt

的形式参与到Pt-O-Ce键成键中，表面Pt

缺失，催化剂表现出明显的失活现象。Pt/CeO

催化剂中，起主要活性作用的是金属态Pt

，胶体粒子原位沉积法能够实现Pt

的直接负载，对于提高Pt基催化剂中Pt的利用率，降低Pt资源消耗都具有重要意义。

Abstract

The interaction between Pt and the carrier affects the catalytic activity of the intrinsic Pt nanoparticles. Herein

Pt/CeO

catalyst was successfully prepared

via

a facile Pt colloidal particle deposition method

and its physicochemical properties and catalytic performance in CO oxidation and toluene combustion were investigated. XRD

TEM

XPS and H

-TPR were used to identify the states of Pt particles on the support surface

as well as their effect on the performance of the catalysts. Formation of metallic Pt

which provided the active sites for CO oxidation and toluene combustion is one of the factors controlling catalyst activity. Pt/CeO

catalyst prepared by colloidal particle deposition was found to be more advantageous than conventional impregnation and impregnation-reduction in producing very finely dispersed metallic Pt

that did not noticeably agglomerate even after thermal treatment at 400℃ for longer duration. The CO oxidation and toluene combustion activity additionally demonstrate that the sample shows a remarkably better performance as compared to its impregnated counterparts. By contrast

all of Pt atoms were anchored with the surface oxygen of CeO

by forming Pt-O-Ce bond during the oxidative treatment in impregnation method

resulting in the absence of metallic Pt

. This change is evidence of the appearance of Pt

species

which is supported by the H

-TPR and XPS data

and could be the main reason behind the deactivation of the Pt/CeO

catalyst. Compared with impregnation method

the dispersion of metallic Pt

rised while less Pt-O-Ce bonds existed on the support surface

and a higher Pt

/Pt

ratio could be maintained even under the high thermal treatment in impregnation reduction method. The catalytic activity test of CO oxidation and toluene combustion show that the sample exhibits the better catalytic performance due to the increase of surface metallic Pt

but it is unavoidable for the sample to show a decline in catalytic activity compared with its colloidal particle depositional counterpart. Hence

it is concluded that the state and the dispersion of Pt nanoparticles on the support surface depended on the prepared method

and they are the decisive factors to promote the catalytic activity of Pt/CeO

upon the oxidative treatment

especially the abundant surface metallic Pt

. Based on characterization results

the colloidal particle deposition method is proposed to realize the direct load of metallic Pt

and gives the homogeneous dispersion of Pt nanoparticles

possessing a superiority in improving the catalytic performance.

关键词

Keywords

references

Ma Y , Chen M , Song C , et al . Catalytic oxidation of toluene, acetone and ethyl acetate on a new Pt-Pd/stainless steel wire mesh catalyst [J]. Acta Physico-Chimica Sinica , 2008 , 24 : 1132 - 1136 .

Zheng C H , Shen J L , Zhang Y X , et al . Quantitative assessment of industrial VOC emissions in China: historical trend, spatial distribution, uncertainties, and projection [J]. Atmospheric Environment , 2017 , 150 : 116 - 125 .

Li M , Liu H , Geng G N , et al . Anthropogenic emission inventories in China: a review [J]. National Science Review , 2017 , 4 : 834 - 866 .

Gentner D R , Harley R A , Miller A M , et al . Diurnal and seasonal variability of gasoline-related volatile organic compound emissions in Riverside, California [J]. Environmental Science & Technology , 2009 , 43 : 4247 - 4252 .

Li W B , Chu W B , Zhuang A , et al . Catalytic oxidation of toluene on Mn-containing mixed oxides prepared in reverse microemulsions [J]. Catalysis Today , 2004 , 93 / 94 / 95 : 205 - 209 .

Xiao L H , Sun K P , Xu X L , et al . Catalytic combustion of methane over CeO 2 -MO x (M=La 3+ , Ca 2+ ) solid solution promoted Pd/gamma-Al 2 O 3 catalysts [J]. Acta Physico-Chimica Sinica , 2008 , 24 : 2108 - 2113 .

Aguero F N , Barbero B P , Gambaro L , et al . Catalytic combustion of volatile organic compounds in binary mixtures over MnO x /Al 2 O 3 catalyst [J]. Applied Catalysis B-Environmental , 2009 , 91 : 108 - 112 .

Morales M R , Barbero B P , Cadus L E . Total oxidation of ethanol and propane over Mn-Cu mixed oxide catalysts [J]. Applied Catalysis B-Environmental , 2006 , 67 : 229 - 236 .

Grbic B , Radic N , Terlecki-Baricevic A . Kinetics of deep oxidation of n -hexane and toluene over Pt/Al 2 O 3 catalysts- oxidation of mixture [J]. Applied Catalysis B-Environmental , 2004 , 50 : 161 - 166 .

Li N , Chen Q Y , Luo M F , et al . Kinetics study of CO oxidation reaction over Pt/TiO 2 catalysts [J]. Acta Physico-Chimica Sinica , 2013 , 29 : 1055 - 1062 .

Shen M Q , Lv L F , Wang J Q , et al . Study of Pt dispersion on Ce based supports and the influence on the CO oxidation reaction [J]. Chemical Engineering Journal , 2014 , 255 : 40 - 48 .

Chen X , Zhao Z L , Zhou Y , et al . A facile route for spraying preparation of Pt/TiO 2 monolithic catalysts toward VOCs combustion [J]. Applied Catalysis A-General , 2018 , 566 : 190 - 199 .

Liu H H , Wang Y , Jia A P , et al . Oxygen vacancy promoted CO oxidation over Pt/CeO 2 catalysts: a reaction at Pt-CeO 2 interface [J]. Applied Surface Science , 2014 , 314 : 725 - 734 .

Cui H Z , Yao J L , Ben L I , et al . Study on performance of low loading Pt/γ-AlOOH for VOCs catalytic combustion [J]. Modern Chemical Industry , 2017 , 37 : 93 - 97, 99 .

Xie X J , Chen W K , Sun B Z , et al . Adsorption behavior of NO on Cu 3 Pt(111) surface [J]. Acta Physico-Chimica Sinica , 2010 , 26 : 3047 - 3051 .

Becker E , Carlsson P A , Skoglundh M . Methane oxidation over alumina and ceria supported platinum [J]. Topics in Catalysis , 2009 , 52 : 1957 - 1961 .

Oran U , Uner D . Mechanisms of CO oxidation reaction and effect of chlorine ions on the CO oxidation reaction over Pt/CeO 2 and Pt/CeO 2 /gamma-Al 2 O 3 catalysts [J]. Applied Catalysis B-Environmental , 2004 , 54 : 183 - 191 .

Peng R S , Sun X B , Li S J , et al . Shape effect of Pt/CeO 2 catalysts on the catalytic oxidation of toluene [J]. Chemical Engineering Journal , 2016 , 306 : 1234 - 1246 .

Zhou J F , Zhao M , Peng N , et al . Performance effect of Pt/MO x -SiO 2 (M=Ce, Zr, Al) catalysts for CO and C 3 H 8 oxidation [J]. Acta Physico-Chimica Sinica , 2012 , 28 : 1448 - 1454 .

Meher S K , Cargnello M , Troiani H , et al . Alcohol induced ultra-fine dispersion of Pt on tuned morphologies of CeO 2 for CO oxidation [J]. Applied Catalysis B-Environmental , 2013 , 130 : 121 - 131 .

Gao Y X , Wang W D , Chang S J , et al . Morphology effect of CeO 2 support in the preparation, metal-support interaction, and catalytic performance of Pt/CeO 2 catalysts [J]. Chemcatchem , 2013 , 5 : 3610 - 3620 .

Wu X Q , Zong R L , Zhu Y F . Enhanced MnO 2 nanorods to CO and volatile organic compounds oxidative activity by platinum nanoparticles [J]. Acta Physico-Chimica Sinica , 2012 , 28 : 437 - 444 .

Cargnello M , Doan-Nguyen V V T , Gordon T R , et al . Control of metal nanocrystal size reveals metal-support interface role for ceria catalysts [J]. Science , 2013 , 341 : 771 - 773 .

Feng L , Hoang D T , Tsung C K , et al . Catalytic properties of Pt cluster-decorated CeO 2 nanostructures [J]. Nano Research , 2011 , 4 : 61 - 71 .

Liu H L , Lei M , Shao S B , et al . Preferential CO oxidation on Ce-promoted Pt/gamma-Al 2 O 3 catalysts under H 2 -rich atmosphere [J]. Chinese Journal of Catalysis , 2007 , 28 : 1077 - 1082 .

Jung S , Suzuki A , Tsuboi H , et al . An elucidation of the interaction between Pt particles and CeO 2 surfaces using tight-binding quantum chemistry method [J]. Topics in Catalysis , 2010 , 53 : 700 - 706 .

Lee J , Ryou Y S , Chan X J , et al . How Pt interacts with CeO 2 under the reducing and oxidizing environments at elevated temperature: the origin of improved thermal stability of Pt/CeO 2 compared to CeO 2 [J]. Journal of Physical Chemistry C , 2016 , 120 : 25870 - 25879 .

Maache R , Brahmi R , Pirault-Roy L , et al . Oxygen storage capacity of Pt-CeO 2 and Pt-Ce 0.5 Zr 0.5 O 2 catalysts [J]. Topics in Catalysis , 2013 , 56 : 658 - 661 .

Nagai Y , Hirabayashi T , Dohmae K , et al . Sintering inhibition mechanism of platinum supported on ceria-based oxide and Pt-oxide-support interaction [J]. Journal of Catalysis , 2006 , 242 : 103 - 109 .

Hatanaka M , Takahashi N , Takahashi N , et al . Reversible changes in the Pt oxidation state and nanostructure on a ceria-based supported Pt [J]. Journal of Catalysis , 2009 , 266 : 182 - 190 .

Jin J H , Li C , Tsang C W , et al . Catalytic combustion of methane over Pt-Ce oxides under scarce oxygen condition [J]. Industrial & Engineering Chemistry Research , 2016 , 55 : 2293 - 2301 .

Royer S , Duprez D . Catalytic oxidation of carbon monoxide over transition metal oxides [J]. ChemCatChem , 2011 , 3 : 24 - 65 .

Hinokuma S , Okamoto M , Ando E , et al . Structure and CO oxidation activity of Pt/CeO 2 catalysts prepared using arc-plasma [J]. Bulletin of the Chemical Society of Japan , 2012 , 85 : 144 - 149 .

Zheng B , Liu G , Geng L L , et al . Role of the FeO x support in constructing high-performance Pt/FeO x catalysts for low-temperature CO oxidation [J]. Catalysis Science & Technology , 2016 , 6 : 1546 - 1554 .

Zhou A B , Wang J , Wang H , et al . Effect of active oxygen on the performance of Pt/CeO 2 catalysts for CO oxidation [J]. Journal of Rare Earths , 2018 , 36 : 257 - 264 .

Ding K , Gulec A , Johnson A M , et al . Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts [J]. Science , 2015 , 350 : 189 - 192 .

Huang H , Dai Q G , Wang X Y . Morphology effect of Ru/CeO 2 catalysts for the catalytic combustion of chlorobenzene [J]. Applied Catalysis B-Environmental , 2014 , 158 : 96 - 105 .

Peng R S , Li S J , Sun X B , et al . Size effect of Pt nanoparticles on the catalytic oxidation of toluene over Pt/CeO 2 catalysts [J]. Applied Catalysis B-Environmental , 2018 , 220 : 462 - 470 .

Bera P , Gayen A , Hegde M S , et al . Promoting effect of CeO 2 in combustion synthesized Pt/CeO 2 catalyst for CO oxidation [J]. Journal of Physical Chemistry B , 2003 , 107 : 6122 - 6130 .

Damyanova S , Pawelec B , Arishtirova K , et al . The effect of CeO 2 on the surface and catalytic properties of Pt/CeO 2 -ZrO 2 catalysts for methane dry reforming [J]. Applied Catalysis B-Environmental , 2009 , 89 : 149 - 159 .

Wang Z , Wang Q , Liao Y C , et al . Comparative study of CeO 2 and doped CeO 2 with tailored oxygen vacancies for CO oxidation [J]. Chemphyschem , 2011 , 12 : 2763 - 2770 .

Pfau A , Schierbaum K D . The electronic-structure of stoichiometric and reduced CeO 2 surfaces-an XPS, UPS and HREELS study [J]. Surface Science , 1994 , 321 : 71 - 80 .

Xiao W D , Guo Q L , Wang E G . Transformation of CeO 2 (111) to Ce 2 O 3 (0001) films [J]. Chemical Physics Letters , 2003 , 368 : 527 - 531 .

Vayssilov G N , Lykhach Y , Migani A , et al . Support nanostructure boosts oxygen transfer to catalytically active platinum nanoparticles [J]. Nature Materials , 2011 , 10 : 310 - 315 .

Manuel L J , Gilbank A L , Garcia T , et al . The prevalence of surface oxygen vacancies over the mobility of bulk oxygen in nanostructured ceria for the total toluene oxidation [J]. Applied Catalysis B-Environmental , 2015 , 174 : 403 - 412 .

Zhou B , Xi K , Fan L J , et al . A comparative study on Ce-Pr and Ce-Mn mixed oxide catalysts toward soot catalytic combustion [J]. Applied Catalysis A-General , 2018 , 562 : 1 - 10 .

Reyes P , Pecchi G , Morales M , et al . The nature of the support and the metal precursor on the resistance to sulphur poisoning of Pt supported catalysts [J]. Applied Catalysis A-General , 1997 , 163 : 145 - 152 .

Zhu H Y , Wu Z L , Su D , et al . Constructing hierarchical interfaces: TiO 2 -supported PtFe-FeO x nanowires for room temperature CO oxidation [J]. Journal of the American Chemical Society , 2015 , 137 : 10156 - 10159 .

Chen C Y , Zhu J , Chen F , et al . Enhanced performance in catalytic combustion of toluene over mesoporous beta zeolite-supported platinum catalyst [J]. Applied Catalysis B-Environmental , 2013 , 140 : 199 - 205 .

Liu K , Wang A Q , Zhang T . Recent advances in preferential oxidation of CO reaction over platinum group metal catalysts [J]. ACS Catalysis , 2012 , 2 : 1165 - 1178 .

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不同Pt前体制备Pt/CeO2催化剂对其结构及性能的影响

Effect of Pt precursor on structure and performance of Pt/CeO2 catalysts

DOI：10.11949/0438-1157.20190468

摘要

Abstract

关键词

Keywords

references

不同Pt前体制备Pt/CeO₂催化剂对其结构及性能的影响

Effect of Pt precursor on structure and performance of Pt/CeO₂ catalysts