One-pot solvent evaporation induced self-assembly synthesis of Pd-Ba-Zn/γ-Al2O3 catalyst with homogeneous distribution of the promoters and its hydrogenation performance of anthraquinone

doi:10.16085/j.issn.1000-6613.2017-1035

Abstract

Abstract: Two 0.4%Pd-2.5%Ba-3.0%Zn/γ-Al₂O₃ catalysts with homogeneous distribution and surface distribution of Ba-and Zn-promoters were prepared via one-pot solvent evaporation induced self-assembly method and incipient-wetness impregnation method,respectively. The catalysts were evaluated in anthraquinone hydrogenation reaction for preparing hydroanthraquinone. Effects of the introduction of the two promoters and their distribution methods on the microstructures and catalytic performance of the catalysts were comparatively studied by XRD,TEM,SEM,EDS,N₂ adsorption-desorption,XPS and high performance liquid chromatography. The results showed that,both of the maximum hydrogenation efficiency and stability of the catalysts increase after introducing the promoters. When distribution of the promoters was changed from surface distribution to homogeneous distribution,the stability of the catalyst is further improved,but its hydrogenation efficiency and recycling rate of anthraquinone is almost the same. In comparison with the conventional preparation process of the catalyst with surface distribution of the promoters,Ba-and Zn-were simultaneously introduced when preparing its precursor of γ-Al₂O₃ with homogeneous distribution of the promoters. The new method has significant advantages of avoiding the impregnation towards the precursors of the promoters and the subsquent drying,calcination processes,and thus greatly simplifies the preparation process,dramatically reduces the energy consumption,and significantly improves the preparation efficiency.

Key words: hydrogenation, 2-ethylanthraquinone, Pd-Ba-Zn/γ-Al₂O₃ catalyst, surface distribution of promoter, homogeneous distribution of promoter

摘要： 分别采用一锅溶剂蒸发诱导自组装法和等体积浸渍法制备了Ba-、Zn-助剂体相分布和表相分布的0.4% Pd-2.5% Ba-3.0% Zn/γ-Al₂O₃催化剂，并将其用于催化蒽醌加氢制氢蒽醌反应。采用XRD、TEM、SEM、EDS、N₂吸附-脱附、XPS和高效液相色谱等表征与测试手段，对比研究了上述助剂引入及其分布方式对催化剂微结构和催化性能的影响。结果表明：添加Ba-、Zn-助剂后催化剂的最高氢化效率和氢化稳定性均有提高；Ba-、Zn-助剂由常规的表相分布变为体相分布后，催化剂的稳定性进一步提高，而氢化效率和蒽醌循环回收率基本相当。和常规助剂表相分布催化剂的制备过程相比，制备助剂体相分布的催化剂时，Ba-、Zn-在制备载体前体时一步引入，省去了分步浸渍助剂前体盐和后续的干燥、焙烧等过程，因而制备工艺大大简化、能耗大幅度降低、制备效率显著提高。

关键词: 加氢, 2-乙基蒽醌, Pd-Ba-Zn/&gamma, -Al₂O₃催化剂, 助剂表相分布, 助剂体相分布

CLC Number:

TQ426.94

YAN Runhua, CAI Weiquan, ZHUO Junlin, WANG Xin, LI Minzhe. One-pot solvent evaporation induced self-assembly synthesis of Pd-Ba-Zn/γ-Al₂O₃ catalyst with homogeneous distribution of the promoters and its hydrogenation performance of anthraquinone[J]. Chemical Industry and Engineering Progress, 2018, 37(03): 1014-1020.

严润华, 蔡卫权, 卓俊琳, 王昕, 李旻哲. 一锅溶剂蒸发诱导自组装法制备助剂体相分布的Pd-Ba-Zn/γ-Al₂O₃催化剂及其蒽醌加氢性能[J]. 化工进展, 2018, 37(03): 1014-1020.

References

[1] CHEN H M,HUANG D P,SU X Y,et al. Fabrication of Pd/γ-Al₂O₃ catalysts for hydrogenation of 2-ethyl-9,10-anthraquinoneassisted by plant-mediated strategy[J]. Chemical Engineering Journal,2015,262:356-363.
[2] 王伟建,潘智勇,李文林,等. 蒽醌法流化床与固定床的发展趋势[J]. 化工进展,2016,35(6):1766-1773. WANG W J,PAN Z Y,LI W L,et al. Recent advances in development of the fluidized bed and fixed bed in theanthraquinone route[J]. Chemical Industry and Engineering Progress,2016,35(6):1766-1773.
[3] GUO Y Y,DAI C N,LEI Z G,et al. Synthesis of hydrogen peroxide over Pd/SiO₂/COR monolith catalysts by anthraquinone method[J]. Catalysis Today,2016,276:36-45.
[4] 陈雪莹,乔明华,贺鹤勇. 载体对负载型Ni-B催化剂催化2-乙基蒽醌加氢制H₂O₂反应性能的影响[J]. 催化学报,2011,32(2):325-332. CHEN X Y,QIAO M H,HE H Y. Effects of supports on catalytic properties of the supported Ni-B catalysts forselective hydrogenation of 2-ethylanthraquinone to H₂O₂[J]. Chinese Journal of Catalysis,2011,32(2):325-332.
[5] 刘春雪,米镇涛,王莅. 2-戊基蒽醌氢化本征动力学研究[J]. 高校化学工程学报,2007,21(3):530-533. LIU C X,MI Z T,WANG L. Intrinsic kinetic study on hydrogenation of 2-amylanthraquinone[J]. Journal of Chemical Engineering of Chinese Universities,2007,21(3):530-533.
[6] 王丰,徐贤伦.添加ZrO₂的Pd/Al₂O₃催化剂及其催化蒽醌加氢性能[J].化工进展,2012,31(1):107-111. WANG F,XU X L. ZrO₂ doped Pd/Al₂O₃ catalyst and its catalytic performance onanthraquinone hydrogenation[J]. Chemical Industry and Engineering Progress,2012,31(1):107-111.
[7] 丁彤,秦永宁,马智. 过渡金属对Pd/γ-Al₂O₃催化剂活性的影响[J]. 催化学报,2002,23(3):227-230. DING T,QIN Y N,MA Z. Effect of transition metal on the activity of γ-Al₂O₃-supported Pd catalyst[J]. Chinese Journal of Catalysis,2002,23(3):227-230.
[8] 杜书伟,王榕,林炳裕,等. BaO对蒽醌氢化制过氧化氢Pd/Al₂O₃催化剂性能的影响[J]. 催化学报,2008,29(5):463-467. DU S W,WANG R,LIN B Y,et al. Effect of BaO on the performance of Pd/Al₂O₃ catalyst for H₂O₂ production from anthraquinone hydrogenation[J]. Chinese Journal of Catalysis,2008,29(5):463-467.
[9] Fulvio P F,Brosey R I,Jaroniec M. Synthesis of mesoporous alumina from boehmite in the presence of triblockcopolymer[J]. ACS Applied Materials & Interfaces,2010,2(2):588-593.
[10] 汪泽华,蔡卫权,郭蕾,等. P123辅助SB粉溶胶制备大孔径介孔γ-Al₂O₃及其对甲基蓝的强化吸附性能[J]. 化工学报,2012,63(8):2623-2628. WANG Z H,CAI W Q,GUO L,et al. P123-assisted synthesis of enlarged mesoporous γ-Al₂O₃from SB pseudoboehmite sol and its performance towards methyl blue[J]. CIESC Journal,2012,63(8):2623-2628.
[11] 卓俊琳,蔡卫权,罗晓雷. 一锅水热-浸渍法制备Pd-Fe/SiO₂催化剂及其蒽醌加氢性能增强[J]. 化工进展,2016,35(12):3913-3918. ZHUO J L,CAI W Q,LUO X L. One-pot hydrothermal-impregnation synthesis of Pd-Fe/SiO₂catalyst with enhanced catalytic performance towards 2-ethylanthraquinone hydrogenation[J]. Chemical Industry and Engineering Progress,2016,35(12):3913-3918.
[12] Li M,Wu X D,Liu S,et al. Effects of baria on propane oxidation activity of Pd/Al₂O₃ catalyst:Pd-BaO interaction and reactionroutes[J]. Progress in Natural Science:Materials International,2014,24(3):280-286.
[13] Yang M,Li S L,Chen G W. High-temperature steam reforming of methanol over ZnO-Al₂O₃ catalysts[J]. Applied Catalysis B:Environmental,2011,101(3):409-416.
[14] Yang M,Men Y,Li S L,et al. Hydrogen production by steam reforming of dimethyl ether over ZnO-Al₂O₃ bi-functionalcatalyst[J]. International Journal of Hydrogen Energy,2012,37(10):8360-8369.
[15] KRUK M,JARONIEC M. Gas adsorption characterization of ordered organic-inorganic nanocomposite materials[J]. Chemistry of Materials,2001,13(10):3169-3183.
[16] Tang P G,Chai Y Y,Feng J T,et al. Highly dispersed Pd catalyst for anthraquinone hydrogenation supported on alumina derived from a pseudoboehmite precursor[J]. Applied Catalysis A:General,2014,469:312-319.
[17] Tanikawa K,Egawa C. Effect of barium addition on CO oxidation activity of palladium catalysts[J]. Applied Catalysis A:General,2011,403:12-17.
[18] Wang Z Q,Yang L,Zhang R,et al. Selective hydrogenation of phenylacetylene over bimetallic Pd-Cu/Al₂O₃ and Pd-Zn/Al₂O₃ catalysts[J]. Catalysis Today,2016,264:37-43.
[19] Kamachi T,Ogata T,Mori E,et al. Computational exploration of the mechanism of the hydrogenation step of the anthraquinone process for hydrogen peroxide production[J]. Journal of Physical Chemistry C,2015,119(16):8748-8754.
[20] Han Y,He Z Y,Wang S L,et al. Performance of facet-controlled Pd nanocrystals in 2-ethylanthraquinone hydrogenation[J]. Catalysis Science & Technology,2015,5(5):2630-2639.
[21] OMAR S,PALOMAR J,GÓMEZ-SAINERO L M,et al. Density functional theory analysis of dichloromethane and hydrogen interaction with Pd clusters:first step to simulate catalytic hydrodechlorination[J]. Journal of Physical Chemistry C,2011,115(29):14180-14192.
[22] YUAN E X,WANG L,ZHANG X W,et al. Density functional theory analysis of anthraquinone derivative hydrogenation over palladium catalyst[J]. ChemPhysChem,2016,17(23):3974-3984.
[23] Yang Y,KIM D S,Knez M,et al. Influence of temperature on evolution of coaxial ZnO/Al₂O₃ one-dimensional heterostructures:from core-shell nanowires to spinel nanotubes and porous nanowires[J]. Journal of Physical Chemistry C,2008,112(11):4068-4074.
[24] LI X T,SU H J,REN G Y,et al. A highly stable Pd/SiO₂/cordierite monolith catalyst for 2-ethyl-anthraquinone hydrogenation[J]. RSC Advances,2015,5(122):100968-100977.

One-pot solvent evaporation induced self-assembly synthesis of Pd-Ba-Zn/γ-Al₂O₃ catalyst with homogeneous distribution of the promoters and its hydrogenation performance of anthraquinone

一锅溶剂蒸发诱导自组装法制备助剂体相分布的Pd-Ba-Zn/γ-Al₂O₃催化剂及其蒽醌加氢性能

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	SHI Yongxing, LIN Gang, SUN Xiaohang, JIANG Weigeng, QIAO Dawei, YAN Binhang. Research progress on active sites in Cu-based catalysts for CO₂ hydrogenation to methanol [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 287-298.
[2]	MAO Shanjun, WANG Zhe, WANG Yong. Group recognition hydrogenation: From concept to application [J]. Chemical Industry and Engineering Progress, 2023, 42(8): 3917-3922.
[3]	WANG Lanjiang, LIANG Yu, TANG Qiong, TANG Mingxing, LI Xuekuan, LIU Lei, DONG Jinxiang. Synthesis of highly dispersed Pt/HY catalyst by rapid pyrolysis of platinum precursors and its performance for deep naphthalene hydrogenation [J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4159-4166.
[4]	WANG Xiaohan, ZHOU Yasong, YU Zhiqing, WEI Qiang, SUN Jinxiao, JIANG Peng. Synthesis and hydrocracking performance of Y molecular sieves with different crystal sizes [J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4283-4295.
[5]	CHU Tiantian, LIU Runzhu, DU Gaohua, MA Jiahao, ZHANG Xiao’a, WANG Chengzhong, ZHANG Junying. Preparation and chemical degradability of organoguanidine-catalyzed dehydrogenation type RTV silicone rubbers [J]. Chemical Industry and Engineering Progress, 2023, 42(7): 3664-3673.
[6]	CHEN Yixin, ZHEN Yaoyao, CHEN Ruihao, WU Jiwei, PAN Limei, YAO Chong, LUO Jie, LU Chunshan, FENG Feng, WANG Qingtao, ZHANG Qunfeng, LI Xiaonian. Preparation of platinum based nanocatalysts and their recent progress in hydrogenation [J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2904-2915.
[7]	LI Dongxian, WANG Jia, JIANG Jianchun. Producing biofuels from soapstock via pyrolysis and subsequent catalytic vapor-phase hydrotreating process [J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2874-2883.
[8]	XU Xian, CUI Louwei, LIU Jie, SHI Junhe, ZHU Yonghong, LIU Jiaojiao, LIU Tao, ZHENG Hua’an, LI Dong. Effect of raw material composition on the development of semicoke mesophase structure [J]. Chemical Industry and Engineering Progress, 2023, 42(5): 2343-2352.
[9]	LI Ling, MA Chaofeng, LU Chunshan, YU Wanjin, SHI Nengfu, JIN Jiamin, ZHANG Jianjun, LIU Wucan, LI Xiaonian. Progress on the synthesis of 1,1,2-trifluoroethene and the catalysts [J]. Chemical Industry and Engineering Progress, 2023, 42(4): 1822-1831.
[10]	GE Weitong, LIAO Yalong, LI Mingyuan, JI Guangxiong, XI Jiajun. Preparation and dechlorination kinetics of Pd-Fe/MWCNTs bimetallic catalyst [J]. Chemical Industry and Engineering Progress, 2023, 42(4): 1885-1894.
[11]	XIAO Yaoxin, ZHANG Jun, HU Sheng, SHAN Rui, YUAN Haoran, CHEN Yong. Cu-Zn catalyzed hydrogenation of furfural with methanol as hydrogen donor [J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1341-1352.
[12]	ZHANG Mengxu, WANG Hongqin, LI Jin, AN Nihong, DAI Yunsheng, QIAN Yin, SHEN Yafeng. Preparation of PtSn/MgAl₂O₄-sheet catalyst and its PDH reaction performance [J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1365-1372.
[13]	ZHANG Dazhou, LU Wenxin, SHANG Kuanxiang, HU Yuan, ZHU Fan, ZHANG Zongfei. Reaction network analysis of dimethyl oxalate hydrogenation to methyl glycolate and recent progress in the heterogeneous catalysts [J]. Chemical Industry and Engineering Progress, 2023, 42(1): 204-214.
[14]	HUANG Wei, CHU Zheng, REN Lei, LI Shan. Application of carbon-based solid acid in hydrogenation of nitrobenzene to p-aminophenol [J]. Chemical Industry and Engineering Progress, 2023, 42(1): 272-281.
[15]	LU Ziwei, LIAO Xiangzhou, SU Xiaoli, SUI Zhijun. Deactivation of Pd-Cu catalyst for hydrodechlorination of trifluorotrichloroethane [J]. Chemical Industry and Engineering Progress, 2023, 42(1): 282-288.