钯基乙炔选择性加氢催化剂研究进展

doi:10.16085/j.issn.1000-6613.2018-0428

化工进展 ›› 2019, Vol. 38 ›› Issue (03): 1353-1361.DOI: 10.16085/j.issn.1000-6613.2018-0428

钯基乙炔选择性加氢催化剂研究进展

徐浩(),徐逸琦,蒋亦舒,张群峰(),李小年()

浙江工业大学工业催化研究所，绿色化学合成技术国家重点实验室培训基地，浙江杭州 310014

收稿日期:2018-03-02 修回日期:2018-05-17 出版日期:2019-03-05 发布日期:2019-03-05
通讯作者: 张群峰,李小年
作者简介:徐浩（1992—），硕士研究生，研究方向为多相催化。E-mail：hasmsx@foxmail.com。|张群峰，副研究员，主要从事炭载钯硫化物催化剂的原位合成。E-mail：zhangqf@zjut.edu.cn|李小年，教授，博士生导师，主要从事工业催化剂技术创新及其在精细有机新材料绿色合成与煤/天然气绿色转化中的应用。E-mail：xnli@zjut.edu.cn
基金资助:
国家重点基础研究发展计划(2011CB710800);国家自然科学基金(21476207、21406199、21776258);浙江省科技厅项目(2015C1042)

Research progress in palladium-based catalysts for selective hydrogenation of acetylene

Hao XU(),Yiqi XU,Yishu JIANG,Qunfeng ZHANG(),Xiaonian LI()

State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology，Institute of Industrial Catalysis of Zhejiang University of Technology，Hangzhou 310014，Zhejiang, China

Received:2018-03-02 Revised:2018-05-17 Online:2019-03-05 Published:2019-03-05
Contact: Qunfeng ZHANG,Xiaonian LI

摘要/Abstract

摘要：

催化选择加氢去除乙烯中微量乙炔是石化工业重要的反应过程，工业钯基催化剂选择性低、催化剂使用寿命较短。本文综述了近年来国内外乙炔选择性加氢钯基催化剂的研究进展。主要探讨了过渡金属、金属氧化物与非金属配体助剂能调变钯粒子空间结构，隔离分散钯粒子并与钯粒子产生电子效应；阐明了钯粒子尺寸与织构形貌的调控能改变钯的晶面结构，影响钯对乙烯的吸脱附和对氢气的活化与解离性能；评述了单一氧化物、复合金属氧化物、碳材料等载体为催化剂提供合适的表面酸碱性并加强了与活性中心之间的相互作用，稳定钯粒子抑制其发生迁移与团聚。提高乙烯选择性与催化剂稳定性是该研究的重点与难点，负载型钯基催化剂的发展方向是构建高分散钯粒子，并在反应过程中保持稳定。

关键词: 加氢, 钯, 催化剂, 选择性, 载体

Abstract:

The selective hydrogenation of ethyne in an ethene-rich stream is a critical process in petrochemical industry. Supported palladium catalysts are generally used as the semi-hydrogenation catalysts. However， several problems still exist， including poor selectivity and short catalyst lifetime. This paper reviews recent researches of the palladium-based catalysts applied in selective hydrogenation of acetylene. The transition metals， metallic oxides and nonmetallic ligands can enhance the selectivity of ethylene by modifying the structure of the active sites， isolating the palladium nanoparticles and forming electron-transport between palladium particles and promoters. The particle size and texture of palladium determine the adsorption/desorption of ethylene and the activation/dissociation of hydrogen. In addition，the supports，such as single oxides，mixed metal oxides and carbon materials can provide appropriate surface acidity and basicity and strengthen the interaction between the supports and metals to prevent the palladium nanoparticles from migration and aggregation. Improving the selectivity of ethylene and stability of catalysts the key and difficult point in this field. The developing tendency of the supported palladium catalyst is to prepare highly dispersed palladium particles and to keep them stable in the reaction process.

Key words: hydrogenation, palladium, catalyst, selectivity, support

中图分类号:

O643

徐浩,徐逸琦,蒋亦舒,张群峰,李小年. 钯基乙炔选择性加氢催化剂研究进展[J]. 化工进展, 2019, 38(03): 1353-1361.

Hao XU,Yiqi XU,Yishu JIANG,Qunfeng ZHANG,Xiaonian LI. Research progress in palladium-based catalysts for selective hydrogenation of acetylene[J]. Chemical Industry and Engineering Progress, 2019, 38(03): 1353-1361.

图/表 4

参考文献 49

1	骆红静, 吕晓东, 赵睿, 等 . 2016年世界和中国石化工业综述及展望[J]. 国际石油经济, 2017(5)： 51-60.
	LUO H J , LÜ X D , ZHAO R , et al . 2016 review and 2017 outlook of global and China petrochemical industry[J]. International Petroleum Economics, 2017(5): 51-60.
2	CHAI M , LIU X , LI L , et al . SiO₂-supported Au-Ni bimetallic catalyst for the selective hydrogenation of acetylene[J]. Chinese Journal of Catalysis, 2017, 38(8): 1338-1346.
3	李振宇, 王红秋, 黄格省, 等 . 我国乙烯生产工艺现状与发展趋势分析[J]. 化工进展, 2017, 36(3): 767-773.
	LI Z Y , WANG H Q , HUANG G S , et al . Research progress of ZSM-5 zeolite for hydrocarbon fuel catalytic cracking against carbon deposition[J]. Chemical Industry and Engineering Progress, 2017, 36(3): 767-773.
4	ARMBRÜSTER M , KOVNIR K , BEHRENS M , et al . Pd-Ga intermetallic compounds as highly selective semihydrogenation catalysts[J]. Journal of the American Chemical Society, 2010, 132(42): 14745-14747.
5	李菲菲, 孙逊, 孙立波, 等 . 负载型纳米金催化剂在乙炔选择性加氢反应中的研究进展[J]. 工业催化, 2016, 24(10): 21-27.
	LI F F , SUN X , SUN L B , et al . Progress in supported nanogold catalyst for selective hydrogenation of acetylene[J]. Industrial Catalysis, 2016, 24(10): 21-27.
6	YANG B , BURCH R , HARDACRE C , et al . Influence of surface structures, subsurface carbon and hydrogen, and surface alloying on the activity and selectivity of acetylene hydrogenation on Pd surfaces： a density functional theory study[J]. Journal of Catalysis, 2013, 305：264-276.
7	苑兴洲, 陈绍云, 陈恒, 等 . 甲烷在Cr改性Pd/Al₂O₃催化剂上的催化燃烧性能[J]. 化工进展, 2014, 33(12): 3258-3262.
	YUAN X Z , CHEN S Y , CHEN H , et al . Cr modified Pd/Al₂O₃ catalyst for methane combustion[J]. Chemical Industry and Engineering Progress, 2014, 33(12): 3258-3262.
8	KRAJČÍ M , HAFNER J . The (210） surface of intermetallic B20 compound GaPd as a selective hydrogenation catalyst: a DFT study[J]. Journal of Catalysis, 2012, 295：70-80.
9	ARMBRÜSTER M , BEHRENS M , CINQUINI F , et al . How to control the selectivity of palladium-based catalysts in hydrogenation reactions： the role of subsurface chemistry[J]. Chemcatchem, 2012, 4(8): 1048-1063.
10	PEI G X , LIU X Y , ZHANG T , et al . Ag alloyed Pd single-atom catalysts for efficient selective hydrogenation of acetylene to ethylene in excess ethylene[J]. ACS Catalysis, 2015, 5(6): 3717-3725.
11	车春霞, 沈立军, 谭都平, 等 . 乙炔选择性加氢反应催化机理的分子模拟研究[J]. 工业催化, 2012, 20(1): 49-53.
	CHE C X , SHEN L J , TAN D P , et al . Molecular simulation research on the catalytic mechanism of selective hydrogenation of acetylene[J]. Industrial Catalysis, 2012, 20(1): 49-53.
12	ZHOU H R , YANG X F , ZHANG T , et al . PdZn intermetallic nanostructure with Pd-Zn-Pd ensembles for highly active and chemoselective semi-hydrogenation of acetylene[J]. ACS Catalysis, 2016, 6(2): 1054-1061.
13	LIU Y N , HE Y F , FENG J T , et al . Catalytic performance of Pd-promoted Cu hydrotalcite-derived catalysts in partial hydrogenation of acetylene：effect of Pd-Cu alloy formation[J]. Catalysis Science＆Technology, 2016, 6(9): 3027-3037.
14	FENG J T , LIU Y N , YIN M , et al . Preparation and structure-property relationships of supported trimetallic PdAuAg catalysts for the selective hydrogenation of acetylene[J]. Journal of Catalysis, 2016, 344：854-864.
15	FU Q , LI W X , YAO Y X , et al . Interface-confined ferrous centers for catalytic oxidation[J]. Science, 2010, 328(5982): 1141-1144.
16	LU J L , FU B S , KUNG M C , et al . Coking- and sintering-resistant palladium catalysts achieved through atomic layer deposition[J]. Science, 2012, 335(6073): 1205-1208.
17	YI H , DU H Y , HU Y L , et al . Precisely controlled porous alumina overcoating on Pd catalyst by atomic layer deposition: enhanced selectivity and durability in hydrogenation of 1,3-butadiene[J]. ACS Catalysis, 2015, 5(5): 2735-2739.
18	DING L B , YI H , HAUNG W H , et al . Activating edge sites on Pd catalysts for selective hydrogenation of acetylene via selective Ga₂O₃ decoration[J]. ACS Catalysis, 2016, 6(6): 3700-3707.
19	AHN I Y, KIM W J, MOON S H . Performance of La₂O₃- or Nb₂O₅-added Pd/SiO₂ catalysts in acetylene hydrogenation[J]. Applied Catalysis A：General, 2006, 308：75-81.
20	KIM W J, MOON S H . Modified Pd catalysts for the selective hydrogenation of acetylene[J]. Catalisis Today, 2012, 185(1): 2-16.
21	KIM E, SHIN E W , BARK C W , et al . Pd catalyst promoted by two metal oxides with different reducibilities： properties and performance in the selective hydrogenation of acetylene[J]. Applied Catalysis A：General, 2014, 471：80-83.
22	TRIMM D L , LIU I O Y , CANT N W . The effect of carbon monoxide on the oligomerization of acetylene in hydrogen over a Ni/SiO₂ catalyst[J]. Journal of Molecular Catalysis A：Chemical, 2009, 307(1/2): 13-20.
23	MCKENNA F M , WELLS R P K , ANDERSON J A . Enhanced selectivity in acetylene hydrogenation by ligand modified Pd/TiO₂ catalysts[J]. Chemical Communications, 2011, 47(8): 2351-2353.
24	MCCUE A J , MCKENNA F M , ANDERSON J A . Triphenylphosphine：a ligand for heterogeneous catalysis too？Selectivity enhancement in acetylene hydrogenation over modified Pd/TiO₂ catalyst[J]. Catalysis Science＆Technology, 2015, 5(4): 2449-2459.
25	MCKENNA F M , ANDERSON J A . Selectivity enhancement in acetylene hydrogenation over diphenyl sulphide-modified Pd/TiO₂ catalysts[J]. Journal of Catalysis, 2011, 281(2): 231-240.
26	HU M , WANG X Q . Effect of N₃ ^- species on selective acetylene hydrogenation over Pd/SAC catalysts[J]. Catalysis Today, 2016, 263：98-104.
27	PEI G X , LIU X Y , ZHANG T , et al . Promotional effect of Pd single atoms on Au nanoparticles supported on silica for the selective hydrogenation of acetylene in excess ethylene[J]. New Journal of Chemistry, 2014, 38(5): 2043-2051.
28	ZHOU H R , YANG X F , ZHANG T , et al . Pd/ZnO catalysts with different origins for high chemoselectivity in acetylene semi-hydrogenation[J]. Chinese Journal of Catalysis, 2016, 37(5): 692-699.
29	KRAJČÍ M , HAFNER J . Selective semi-hydrogenation of acetylene：atomistic scenario for reactions on the polar threefold surfaces of GaPd[J]. Journal of Catalysis, 2014, 312：232-248.
30	VILE G , ALBANI D , NACHTEGAAL M , et al . A stable single-site palladium catalyst for hydrogenations[J]. Angewandte Chemie-International Edition, 2015, 54(38): 11265-11269.
31	KIM S K, KIM C, MOON S H , et al . Performance of shape-controlled Pd nanoparticles in the selective hydrogenation of acetylene[J]. Journal of Catalysis, 2013, 306：146-154.
32	HE Y F , LIU Y N , LI D Q , et al . Fabrication of a PdAg mesocrystal catalyst for the partial hydrogenation of acetylene[J]. Journal of Catalysis, 2015, 330：61-70.
33	ELLIS I T , WOLF E H , JONES G , et al . Lithium and boron as interstitial palladium dopants for catalytic partial hydrogenation of acetylene[J]. Chemical Communications, 2017, 53(3): 601-604.
34	LUO Y , VILLASECA S A , ARMBRÜSTER M , et al . Addressing electronic effects in the semi-hydrogenation of ethyne by InPd₂ and intermetallic Ga-Pd compounds[J]. Journal of Catalysis, 2016, 338：265-272.
35	MCCUE A J , GUERRERO-RUIZ A , RODRÍGUEZ-RAMOS I , et al . Palladium sulphide—A highly selective catalyst for the gas phase hydrogenation of alkynes to alkenes[J]. Journal of Catalysis, 2016, 340：10-16.
36	MCCUE A J , GUERRERO-RUIZ A , RAMIREZ-BARRIA C , et al . Selective hydrogenation of mixed alkyne/alkene streams at elevated pressure over a palladium sulfide catalyst[J]. Journal of Catalysis, 2017, 355：40-52.
37	SANGKHUM T , MEKASUWANDUMRONG O , PANPRANOT J , et al . Effect of Fe-modified α-Al₂O₃ on the properties of Pd/α-Al₂O₃ catalysts in selective acetylene hydrogenation[J]. Reaction Kinetics and Catalysis Letters, 2009, 97(1): 115-123.
38	徐爽, 台宝泉, 李晓燕, 等 . 二硫化物修饰改性乙炔加氢催化剂研究[J]. 石油化工高等学校学报, 2014, 27(4): 1-5.
	XU S , TAI B Q , LI X Y , et al . Study on acetylene hydrogenation catalysts modified by disulfide[J]. Journal of Petrochemical Universities, 2014, 27(4): 1-5.
39	KOMEILI S , RAVANCHI M T , TAEB A . The influence of alumina phases on the performance of the Pd-Ag/Al₂O₃ catalyst in tail-end selective hydrogenation of acetylene[J]. Applied Catalysis A：General，2015, 502：287-296.
40	RAVANCHI M T , FADAEERAYENI S , FARD M R . The effect of calcination temperature on physicochemical properties of alumina as a support for acetylene selective hydrogenation catalyst[J]. Research on Chemical Inter2018-0428tes, 2015, 42(5): 4797-4811.
41	李冰杰, 史秀锋, 刘秀芳, 等 . ZnAl水滑石负载钯催化剂的制备及催化性能[J]. 化工进展, 2014, 33(10): 2661-2664.
	LI B J , SHI X F , LIU X F , et al . Preparation of hydrotalcite-supported palladium catalysts and their catalytic performances[J]. Chemical Industry and Engineering Progress, 2014, 33(10): 2661-2664.
42	FENG J T , MA X Y, LI D Q , et al . Enhancement of metal dispersion and selective acetylene hydrogenation catalytic properties of a supported Pd catalyst[J]. Industrial ＆ Engineering Chemistry Research, 2011, 50(4): 1947-1954.
43	MA X Y, CHAI Y Y , EVANS D , et al . Preparation and selective acetylene hydrogenation catalytic properties of supported Pd catalyst by the in situ precipitation-reduction method[J]. The Journal of Physical Chemistry C, 2011, 115(17): 8693-8701.
44	JIN Q , HE Y F , FENG J T , et al . Highly selective and stable PdNi catalyst derived from layered double hydroxides for partial hydrogenation of acetylene[J]. Applied Catalysis A：General, 2015, 500：3-11.
45	OOSTHUIZEN R S , NYAMORI V O . Carbon nanotubes as supports for palladium and bimetallic catalysts for use in hydrogenation reactions[J]. Platinum Metals Review, 2011, 55(3): 154-169.
46	BENAVIDEZ A D , BURTON P D , DATYE A K , et al . Improved selectivity of carbon-supported palladium catalysts for the hydrogenation of acetylene in excess ethylene[J]. Applied Catalysis A：General, 2014, 482(26): 108-115.
47	LU H M , XU B L , FAN Y N , et al . The influence of Pd particles distribution position on Pd/CNTs catalyst for acetylene selective hydrogenation[J]. Catalysis Letters, 2014, 144(12): 2198-2203.
48	CHESNOKOV V V , PODYACHEVA O Y , RICHARDS R M . Influence of carbon nanomaterials on the properties of Pd/C catalysts in selective hydrogenation of acetylene[J]. Materials Research Bulletin, 2017, 88：78-84.
49	HUANG X H , XIA Y J , LU J L , et al . Enhancing both selectivity and coking-resistance of a single-atom Pd₁/C₃N₄ catalyst for acetylene hydrogenation[J]. Nano Research, 2017, 10(4): 1302-1312.

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钯基乙炔选择性加氢催化剂研究进展

Research progress in palladium-based catalysts for selective hydrogenation of acetylene

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