[1]赵吉晓,蔡文静,焦志锋,等.Pd-Cu/SiC催化苯乙炔选择性加氢性能[J].常州大学学报(自然科学版),2022,34(05):23-29.[doi:10.3969/j.issn.2095-0411.2022.05.004]
　ZHAO Jixiao,CAI Wenjing,JIAO Zhifeng,et al.Selective Hydrogenation of Phenylacetylene over Pd-Cu/SiC Catalysts[J].Journal of Changzhou University(Natural Science Edition),2022,34(05):23-29.[doi:10.3969/j.issn.2095-0411.2022.05.004]
点击复制

Pd-Cu/SiC催化苯乙炔选择性加氢性能()
分享到：

常州大学学报(自然科学版)[ISSN:2095-0411/CN:32-1822/N]

卷:
第34卷
期数:
2022年05期
页码:
23-29
栏目:
化学化工
出版日期:
2022-09-28

文章信息/Info

Title:
Selective Hydrogenation of Phenylacetylene over Pd-Cu/SiC Catalysts
文章编号:
2095-0411(2022)05-0023-07
作者:
赵吉晓1; 蔡文静1; 焦志锋1; 郭向云1; 2
(1.常州大学石油化工学院,江苏常州213164;2.中国科学院山西煤炭化学研究所,山西太原030001)
Author(s):
ZHAO Jixiao1;  CAI Wenjing1;  JIAO Zhifeng1;  GUO Xiangyun1; 2
(1.School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China; 2.Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China)
关键词:
苯乙炔;  选择性加氢;  SiC;  Cu-Pd合金
Keywords:
phenylacetylene;  selective hydrogenation;  SiC;  Cu-Pd alloy
分类号:
TQ 426.8
DOI:
10.3969/j.issn.2095-0411.2022.05.004
文献标志码:
A
摘要:
利用液相还原法制备了Pd-Cu/SiC双金属催化剂,并将其用于苯乙炔选择性加氢制备苯乙烯。结果表明,催化剂中Pd/Cu质量比对活性和选择性有明显影响,其中Pd0.5-Cu2.5/SiC催化剂具有突出的催化活性和选择性,贵金属Pd的TOF值达到2 972 h-1。加氢过程中Pd将氢气解离为活性氢,随后活性氢溢流到SiC的表面,与吸附在SiC表面的苯乙炔进行反应。根据XPS结果,双金属催化剂中Pd的部分电子转移给了Cu。这种电子转移使Pd对H2的吸附和解离能力减弱,使催化剂表面活性氢浓度降低,进而抑制了苯乙烯的过度加氢。通过加入过渡金属Cu构建双金属催化剂能够有效减少贵金属Pd的使用量,降低催化剂成本。
Abstract:
Pd-Cu/SiC bimetallic catalysts were prepared by a liquid-phase reduction method and used in the selective hydrogenation of phenylacetylene to styrene. The results show that the mass ratio of Pd/Cu has obvious influence on the catalytic performances, and Pd0.5-Cu2.5/SiC catalyst exhibits the best catalytic activity and selectivity, and the TOF value based on Pd can reach as high as 2 972 h-1. During hydrogenation, H2 dissociates on the surface of Pd to form active hydrogen, and then the active hydrogen overflows to SiC and reacts with phenylacetylene adsorbed on the surface of SiC. XPS results illustrate that the electrons can transfer from Pd to Cu, which decrease the H2 dissociation ability of Pd and hence inhibit the over hydrogenation of styrene. This strategy of constructing bimetallic catalyst by adding transition metal Cu can effectively cut the usage of Pd and reduce the cost of the catalyst.

参考文献/References:

[1] HOSSAIN M M, ATANDA L, AL-YASSIR N, et al. Kinetics modeling of ethylbenzene dehydrogenation to styrene over a mesoporous alumina supported iron catalyst[J]. Chemical Engineering Journal, 2012, 207/208: 308-321.
[2] 王丽丽, 何娇龙, 张淼, 等. 苯乙炔选择性加氢研究进展[J]. 内蒙古民族大学学报(自然科学版), 2018, 33(2): 109-112.
[3] LÃPEZ N, VARGAS-FUENTES C. Promoters in the hydrogenation of alkynes in mixtures:insights from density functional theory[J]. Chemical Communications, 2012, 48(10): 1379-1391.
[4] HU J W, ZHOU Z M, ZHANG R, et al. Selective hydrogenation of phenylacetylene over a nano-Pd/α-Al2O3 catalyst[J]. Journal of Molecular Catalysis A: Chemical, 2014, 381: 61-69.
[5] MARKOV P V, BRAGINA G O, RASSOLOV A V, et al. Pd-Cu catalyst prepared from heterobimetallic PdCu2(OAc)6: an XRD-EXAFS study and activity/selectivity in the liquid-phase hydrogenation of a C≡C bond[J]. Mendeleev Communications, 2016, 26(6): 502-504.
[6] FURUKAWA S, ENDO M, KOMATSU T. Bifunctional catalytic system effective for oxidative dehydrogenation of 1-butene and n-butane using Pd-based intermetallic compounds[J]. ACS Catalysis, 2014, 4(10): 3533-3542.
[7] ELLERT O G, TSODIKOV M V, NIKOLAEV S A, et al. Bimetallic nanoalloys in heterogeneous catalysis of industrially important reactions:synergistic effects and structural organization of active components[J]. Russian Chemical Reviews, 2014, 83(8): 718-732.
[8] VAN DEELEN T W, HERNÁNDEZ MEJÍA C, DE JONG K P. Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity[J]. Nature Catalysis, 2019, 2(11): 955-970.
[9] JIAO Z F, GUO X N, ZHAI Z Y, et al. The enhanced catalytic performance of Pd/SiC for the hydrogenation of furan derivatives at ambient temperature under visible light irradiation[J]. Catalysis Science & Technology, 2014, 4(8): 2494-2498.
[10] HAO C H, GUO X N, SANKAR M, et al. Synergistic effect of segregated Pd and Au nanoparticles on semiconducting SiC for efficient photocatalytic hydrogenation of nitroarenes[J]. ACS Applied Materials & Interfaces, 2018, 10(27): 23029-23036.
[11] 蔡文静, 焦志锋, 张成都, 等. Pd/SiC催化苯乙炔选择性加氢性能[J]. 石油化工, 2021, 50(7): 629-634.
[12] SHESTERKINA A A, KIRICHENKO O A, KOZLOVA L M, et al. Liquid-phase hydrogenation of phenylacetylene to styrene on silica-supported Pd-Fe nanoparticles[J]. Mendeleev Communications, 2016, 26(3): 228-230.
[13] TAO F F. Synthesis, catalysis, surface chemistry and structure of bimetallic nanocatalysts[J]. Chemical Society Reviews, 2012, 41(24): 7977-7979.
[14] OBRAZTSOVA I I, EREMENKO N K, SIMENYUK G Y, et al. Bimetallic catalysts for the hydrogenation of aromatic nitro compounds[J]. Solid Fuel Chemistry, 2012, 46(6): 364-367.
[15] JIN G Q, GUO X Y. Synthesis and characterization of mesoporous silicon carbide[J]. Microporous and Mesoporous Materials, 2003, 60(1/2/3): 207-212.
[16] JIAO Z F, ZHAO J X, GUO X N, et al. Turning the product selectivity of nitrile hydrogenation from primary to secondary amines by precise modification of Pd/SiC catalysts using NiO nanodots[J]. Catalysis Science & Technology, 2019, 9(9): 2266-2272.
[17] 王沾祺, 周志明, 张锐, 等. Pd-Cu/γ-Al2O3催化苯乙炔选择性加氢反应[J]. 物理化学学报, 2014, 30(12): 2315-2322.
[18] YANG F, ZHANG Y, LIU P F, et al. Pd-Cu alloy with hierarchical network structure as enhanced electrocatalysts for formic acid oxidation[J]. International Journal of Hydrogen Energy, 2016, 41(16): 6773-6780.
(责任编辑:谭晓荷)

相似文献/References:

[1]朱 劼,李 丹,丁雪洁,等.温敏高分子修饰氧化石墨烯负载钌催化剂的制备及选择加氢活性[J].常州大学学报(自然科学版),2019,31(06):1.
　ZHU Jie,LI Dan,DING Xuejie,et al.A Ru Catalyst Supported on Temperature-Sensitive Polymer Grafted Graphene Oxide and Its Catalytic Activity in Selective Hydrogenation Activity[J].Journal of Changzhou University(Natural Science Edition),2019,31(05):1.

备注/Memo

备注/Memo:
收稿日期: 2022-04-16。
基金项目: 山西省优秀人才科技创新资助项目(201605D211012)。
作者简介: 赵吉晓(1992—), 女, 河南洛阳人, 博士, 讲师。E-mail: zhaojixiao@cczu.edu.cn
更新日期/Last Update: 1900-01-01