Preparation of High Activity Oxidative DesulfurizationCatalyst with Polycation and Heteropolyanion Keggin Structure

doi:10.11944/j.issn.1000-0518.2017.11.170011

Chinese Journal of Applied Chemistry ›› 2017, Vol. 34 ›› Issue (11): 1301-1306.DOI: 10.11944/j.issn.1000-0518.2017.11.170011

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Preparation of High Activity Oxidative DesulfurizationCatalyst with Polycation and Heteropolyanion Keggin Structure

CHEN Lidong^a^*(),TONG Huan^a,WANG Xuyang^a,SONG Pengyue^a,LIU Di^a,JI Yanqing^a,YUE Qian^a,DING Wei^a,JIA Yixin^a,CHEN Yongying^b,JIANG Chunjie^a^*()

^aSchool of Chemistry and Chemical Engineering,Liaoning Normal University,Dalian,Liaoning 110629,China
^bSchool of Chemistry Engineering,Dalian University of Technology,Dalian,Liaoning 116024,China

Received:2017-01-06 Accepted:2017-04-14 Published:2017-11-08 Online:2017-11-08
Contact: CHEN Lidong,JIANG Chunjie
Supported by:
Supported by the Research Fund for the Doctoral Program of Liaoning Province of China(No.20131060)

Abstract

Abstract:

Design and development of high activity ultra-deep oxidation of desulfurization catalyst is one of the most important ways to meet the increasing stringent requirements of petrochemical industry for cleaning fuel standards in the future. Catalysts with Keggin structure aluminum hydroxide polyoxocations(Al₁₃), Al₁₃-SDS and HPW-Al₁₃-SDS(HPW=Keggin structure phosphotungstic acid, SDS=sodium dodecylsulfate) were prepared. The structures of these catalysts were characterized by Fourier transform infrared spectroscopy(FT-IR), X-ray diffraction(XRD), ultraviolet visible spectroscopy(UV-Vis), Brunauer-Emmett-Teller(BET) and thermogravimetry(TG). The preservation of the Keggin structure on HPW-Al₁₃-SDS catalyst was confirmed by IR and UV-Vis spectra. Catalytic oxidation desulfurization(ODS) reaction over HPW-Al₁₃-SDS with a model of oil(n-hexan solution of organic sulfur) was studied. In optimized condition, up to 99.5% conversion of sulfur was achieved. The efficiencies of ODS decrease from dibenzothiophene to benzothiophene. IR and XRD characterizations of HPW-Al₁₃-SDS catalyst after the reaction show that the catalysts form peroxo-tungsten complexes. The catalytic activity of the recycled HPW-Al₁₃-SDS is almost the same as freshly prepared, and can be recycled via easy separation. The catalyst used herein is an ideal model for ODS of organic sulfide.

Key words: phosphotungstic acid, aluminum hydroxide polyoxocations, oxidative desulfurization, organic sulfide, hydrogen peroxide

CHEN Lidong, TONG Huan, WANG Xuyang, SONG Pengyue, LIU Di, JI Yanqing, YUE Qian, DING Wei, JIA Yixin, CHEN Yongying, JIANG Chunjie. Preparation of High Activity Oxidative DesulfurizationCatalyst with Polycation and Heteropolyanion Keggin Structure[J]. Chinese Journal of Applied Chemistry, 2017, 34(11): 1301-1306.

References

[1]	YU Fengli,WANG Rui.Study on Oxidative Desulfurization Catalyzed by Organic-Inorganic Heteropolyacids as Phase Transfer Catalyst[J]. Acta Chim Sin,2014,72(1):105-113(in Chinese). 于凤丽,王睿. 有机-无机型杂多酸相转移催化氧化脱硫性能研究[J]. 化学学报,2014,72(1):105-113.
[2]	Li C,Jiang Z X,Gao J B,et al.Ultra-Deep Desulfurization of Diesel:Oxidation with a Recoverable Catalyst Assembled in Emulsion[J]. Chem-Eur J,2004,10(9):2277-2280.
[3]	Lv H Y,Ren W Z,Liao W P,et al. Aerobic Oxidative Desulfurization of Model Diesel Using a B-Type Anderson Catalyst [(C18H37)2N(CH3)2]3Co(OH)6Mo6O18·3H2O[J]. Appl Catal B:Environ,2013,138/139(1):79-83.
[4]	CHEN Lidong,LIU Di,NIU Siqi,et al.Oxidative Desulfurization of Organic Sulfides over Phosphotungstic Acid/Nano-ZSM-5 Composite Catalyst[J]. Chinese J Appl Chem,2016,33(3):364-366 (in Chinese). 陈立东,刘迪,牛思祺,等. 磷钨酸纳米ZSM-5复合催化剂的氧化脱硫反应性[J]. 应用化学,2016,33(3): 364-366.
[5]	Xue X L,Zhao W,Ma B C,et al.Efficient Oxidation of Sulfides Catalyzed by a Temperature-responsive Phase Transfer Catalyst [(C18H37)2(CH3)2N]7PW11O39 with Hydrogen Peroxide[J]. Catal Commun,2012,29(1):73-76.
[6]	PENG Ge,HU Changwen,CHEN Lidong,et al.Synthesis of Novel Inorganic Nanoclusters Between Keggin-type Cation [AlO4Al12(OH)24(H2O)12]7+ and Heteropolyoxometalates[J]. Chinese J Chem Univ,2001,22(10):1629-1631(in Chinese). 彭革,胡长文,陈立东,等. Keggin结构阳离子[AlO4Al12(OH)24(H2O)12]7+与杂多阴离子构筑的新型无机纳米簇凝胶[J]. 高等学校化学学报,2001,22(10):1629-1631.
[7]	Holland B T,Isbester P K,Blanford C F,et al.Synthesis of Ordered Aluminophosphate and Galloaluminophosphate Mesoporous Materials with Anion-Exchange Properties Utilizing Polyoxometalate Cluster/Surfactant Salts as Precursors[J]. J Am Chem Soc,1997,119(29):6796-6803.
[8]	Son J H,Choi H,Kwon Y U.Porous Crystal Formation from Polyoxometalate Building Blocks:Single-Crystal Structure of [AlO4Al12(OH)12(H2O)24][Al(OH)6Mo6O18]2(OH)2·29.5H2O[J]. J Am Chem Soc,2000,112(30):7432-7433.
[9]	WANG Xuyang,SONG Pengyue,WANG Xiangsheng,et al.In-situ Characterization and Reactivity of Heteropoly Acid-based Catalysts for Deep Hydrodesulfurization of Fluid Catalytic Cracking Gasoline[J]. Chinese J Appl Chem,2014,31(8):990-992(in Chinese). 王旭阳,宋鹏月,王祥生,等. 多酸基深度加氢脱硫催化剂的原位表征和反应性能[J]. 应用化学,2014,31(8):990-992.
[10]	Chen L D,Wang X S,Guo X W,et al.In Situ Nanocrystalline HZSM-5 Zeolites Encaged Heteropoly Acid H3PMo12O40 and Ni Catalyst for Hydroconversion of n-Octane[J]. Chem Eng Sci,2007,62(16):4469-4478.
[11]	JIANG Chunjie,SUN Shengnan,WANG Xuyang,et al.Synthesis of Dimethyl Ether from Methanol over Heteropoly Acid/Nanocrystalline HZSM-5 Complex Solid Acidic Catalyst[J]. Acta Chim Sin,2013,71(5):810-814(in Chinese). 姜春杰,孙胜男,王旭阳,等. 甲醇脱水制二甲醚的杂多酸/纳米HZSM-5复合固体酸催化剂[J]. 化学学报,2013,71(5):810-814.
[12]	Yu X D,Guo Y N,Xu L L,et al.A Novel Preparation of Mesoporous CsxH3-xPW12O40/TiO2 Nanocomposites with Enhanced Photocatalytic Activity[J]. Colloids Surf A,2008,316(1/2/3):110-118.
[13]	Mizuno N,Misono M.Heterogeneous Catalysis[J]. Chem Rev,1998,98(1):199-218.
[14]	Otsuki S,Nonaka T,Takashima N,et al.Oxidative Desulfurization of Light Gas Oil and Vacuum Gas Oil by Oxidation and Solvent Extraction[J]. Energy Fuels,2000,14(6):1232-1239.
[15]	Kuang W X,Rives A,Ben T,et al.Isomerization of n-Hexane over Silica Supported Heteropoly Acids Promoted by the Reduced Ce Ni Oxides[J]. J Colloid Interface Sci,2002,248(1):123-129.
[16]	Muñoz M,Romanelli G,Botto I L,et al.Al13 [X Mo/WOn](X=Al,Co,V,P) Composites as Catalysts in Clean Oxidation of Aromatic Sulfides[J]. Appl Catal B:Environ,2010,73(1/2):311-316.
[17]	Xi Z W,Zhou N,Sun Y,et al.Reaction-Controlled Phase-Transfer Catalysis for Propylene Epoxidation to Propylene[J]. Science,2001,292(5519):1139-1141.
[18]	Nisar A,Lu Y,Zhuang J,et al.Polyoxometalate Nanocone Nanoreactors:Magnetic Manipulation and Enhanced Catalytic Performance[J]. Angew Chem Int Ed,2011,50(4):3187-3192.

Preparation of High Activity Oxidative DesulfurizationCatalyst with Polycation and Heteropolyanion Keggin Structure

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