IB金属对Ni/SiO2催化剂乙炔选择性加氢反应性能的影响

doi:10.1016/S1872-2067(20)63568-9

摘要/Abstract

摘要： 乙烯是合成聚乙烯的原料,其主要来源是石油裂解气,其中少量的乙炔杂质会严重毒化生产聚乙烯的催化剂,因此需要将其去除.对于乙炔选择加氢反应,传统工业上使用的是Pd基催化剂,尽管其乙炔转化率很高,但对乙烯的选择性很低.我们前期的研究发现,IB族金属(Au,Ag和Cu)与Pd形成的合金单原子催化剂可以有效地提高乙烯的选择性.作为与Pd同组的非贵金属,Ni催化剂在多种催化加氢反应中显示出优异活性,而在乙炔选择加氢反应中,Ni是否能够替代贵金属Pd尚无定论.本文系统地研究了IB金属对Ni/SiO₂催化剂乙炔选择性加氢性能的影响.与Pd/SiO₂催化剂不同,单金属Ni/SiO₂催化剂在低温下不具有活性.将IB金属添加到Ni/SiO₂催化剂中,可以显著提高其催化活性以及对乙烯的选择性.其中,AuNi_x/SiO₂和CuNi_x/SiO₂催化剂的催化活性随还原温度升高而提高,而AgNi_x/SiO₂催化剂对预处理温度不敏感.通过调变IB/Ni原子比和还原温度优化了催化剂的催化性能,发现优化后的三种催化剂(CuNi_0.125/SiO₂、AgNi_0.5/SiO₂和AuNi_0.5/SiO₂)的活性和选择性随反应温度升高表现出相似的变化趋势.催化稳定性考察结果显示,CuNi_0.125/SiO₂催化剂表现出最高选择性和稳定性;尽管AuNi_0.5/SiO₂的初始活性最高,但是稳定性最低.
采用XRD、TPR和微量吸附量热等表征手段对不同IB金属对Ni基催化剂性质的影响进行了系统考察.以Cu-Ni_x/SiO₂催化剂为例,H₂-TPR测试结果表明,Cu-Ni双金属纳米颗粒的形成使得还原温度低于相应的单金属催化剂,表明铜和镍之间存在明显的相互作用.此外,通过TPR获得的CuNi_x/SiO₂催化剂上的氢气消耗量与理论耗氢量相吻合,表明在还原处理的过程中双金属催化剂中的CuO和NiO可以被完全还原.乙炔的微量吸附量热结果表明,在CuNi_0.125/SiO₂,AgNi_0.5/SiO₂,AuNi_0.5/SiO₂和Ni_0.5/SiO₂催化剂上的初始吸附热分别为187,196,304和103 kJ/mol,即它们的初始乙炔吸附强度顺序为AuNi_0.5/SiO₂ > AgNi_0.5/SiO₂ > CuNi_0.125/SiO₂ > Ni_0.5/SiO₂.该结果与三者的初始催化活性顺序一致,表明IB金属的加入可以增强乙炔在催化剂表面的吸附,从而提高催化活性.

关键词: 乙炔, 乙烯, 选择加氢, Ni, IB金属

Abstract: The IB metal (Au, Ag and Cu) alloyed Pd single atom catalysts had been proved to be efficient in promoting the selectivity for hydrogenation of acetylene to ethylene. As a base metal in the same group as Pd, the Ni-based catalysts are also active for hydrogenation reactions. Herein, the effects of the IB metals on the Ni/SiO₂ catalyst for the selective hydrogenation of acetylene were systematically studied. Different from the Pd/SiO₂ catalyst, the monometallic Ni/SiO₂ catalyst is not active at low temperatures. The addition of the IB metals to the Ni/SiO₂ catalysts can greatly enhance the activity. Besides, the catalytic activity of the AgNi_{x/SiO₂ and CuNix/SiO₂ catalysts increase with the reduction temperature, while the AgNi_x/SiO₂ catalysts are not sensitive to the pretreatment temperature. The origin of the effect of the different IB metals on the Ni-based catalysts for selective hydrogenation of acetylene is discussed based on the characterizations by XRD, TPR and microcalorimetric measurements.}

Key words: Acetylene, Selective hydrogenation, Ethylene, Ni, IB metals

刘华, 柴梦倩, 裴广贤, 刘晓艳, 李林, 康磊磊, 王爱琴, 张涛. IB金属对Ni/SiO₂催化剂乙炔选择性加氢反应性能的影响[J]. 催化学报, 2020, 41(7): 1099-1108.

Hua Liu, Mengqian Chai, Guangxian Pei, Xiaoyan Liu, Lin Li, Leilei Kang, Aiqin Wang, Tao Zhang. Effect of IB-metal on Ni/SiO₂ catalyst for selective hydrogenation of acetylene[J]. Chinese Journal of Catalysis, 2020, 41(7): 1099-1108.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(20)63568-9

https://www.cjcatal.com/CN/Y2020/V41/I7/1099

参考文献

[1] W. T. McGown, C. Kemball, D. A. Whan, M. S. Scurrell, J. Chem. Soc., Faraday Trans. 1, 1977, 73, 632-647.
[2] W. Huang, J. R. Mccormick, R. F. Lobo, J. G. Chen, J. Catal., 2007, 246, 40-51.
[3] A. Borodziński, G. C. Bond, Catal. Rev. Sci. Eng., 2006, 48, 91-144.
[4] A. Borodziński, G. C. Bond, Catal. Rev. Sci. Eng., 2008, 50, 379-469.
[5] K. Georgios, M. B. Boucher, A. D. Jewell, E. A. Lewis, T. J. Lawton, A. E. Baber, H. L. Tierney, F. S. Maria, E. C. H. Sykes, Science, 2012, 335, 1209-1212.
[6] A. Marc, K. Kirill, B. Malte, T. Detre, G. Yuri, S. G. Robert, J. Am. Chem. Soc., 2010, 132, 14745-14747.
[7] G. X. Pei, X. Y. Liu, A. Wang, A. F. Lee, M. A. Isaacs, L. Li, X. Pan, X. Yang, X. Wang, Z. Tai, K. Wilson, T. Zhang, ACS Catal., 2015, 5, 3717-3725.
[8] G. X. Pei, X. Y. Liu, A. Wang, L. Li, Y. Huang, T. Zhang, New J. Chem., 2014, 38, 2043-2051.
[9] G. X. Pei, X. Y. Liu, X. Yang, L. Zhang, A. Wang, L. Li, H. Wang, X. Wang, T. Zhang, ACS Catal., 2017, 7, 1491-1500.
[10] M. Armbruster, M. Friedrich, M. Heggen, R. Cardoso-Gil, J. Am. Chem. Soc., 2011, 133, 9112-9118.
[11] H. Zhou, X. Yang, L. Li, X. Liu, Y. Huang, X. Pan, A. Wang, J. Li, T. Zhang, ACS Catal., 2016, 6, 1054-1061.
[12] A. J. McCue, C. J. McRitchie, A. M. Shepherd, J. A. Anderson, J. Catal., 2014, 319, 127-135.
[13] W. A. A. van Barneveld, V. Ponec, Rec. Trav. Chim., 1974, 93, 243-246.
[14] G. A. Martin, J. A. Dalmon. J. Catal., 1982, 75, 233-242.
[15] A. G. Boudjahem, M. Chettibi, S. Monteverdi, M. M. Bettahar, J. Nanosci. Nanotechnol., 2009, 9, 3546-3554.
[16] M. Chai, X. Liu, L. Li, G. Pei, Y. Ren, Y. Su, H. Cheng, A. Wang, T. Zhang, Chin. J. Catal., 2017, 38, 1338-1346.
[17] G. X. Pei, X. Y. Liu, A. Wang, Y. Su, L. Li, T. Zhang, Appl. Catal. A, 2017, 545, 90-96.
[18] Y. Liu, J. Zhao, J. Feng, Y. He, Y. Du, D. Li, J. Catal., 2018, 359, 251-260.
[19] S. A. Nikolaev, V. V. Smirnov, A. Y. Vasil'kov, V. L. Podshibikhin, Kinet. Catal., 2010, 51, 375-379.
[20] Y. Chai, G. Wu, X. Liu, Y. Ren, W. Dai, C. Wang, Z. Xie, N. Guan, L. Li, J. Am. Chem. Soc., 2019, 141, 9920-9927.
[21] F. Studt, F. Abild-Pedersen, T. Bligaard, R. Z. Sørensen, C. H. Christensen, J. K. Nørskov, Science, 2008, 320, 1320-1322.
[22] F. Studt, F. Abild-Pedersen, T. Bligaard, R. Z. Sørensen, C. H. Christensen, J. K. Nørskov, Angew. Chem., 2008, 120, 9439-9442.
[23] B. Blaise, P. R. Javier, J. Am. Chem. Soc., 2010, 132, 4321-4327.
[24] B. Yang, R. Burch, C. Hardacre, P. Hu, P. Hughes, Catal. Sci. Technol., 2017, 7, 1508-1514.
[25] B. Yang, R. Burch, C. Hardacre, G. Headdock, P. Hu, R. Burch, ACS Catal., 2012, 2, 1027-1032.
[26] H. Wei, X. Wei, X. Yang, G. Yin, A. Wang, X. Liu, T. Zhang, Chin. J. Catal., 2015, 36, 160-167.
[27] Q. Zheng, M. D. Wales, M. G. Heidlage, M. Rezac, H. Wang, S. H. Bossmann, J. Catal., 2015, 330, 222-237.
[28] M. T. Tsay, F. W. Chang, Appl. Catal. A, 2000, 203, 15-22.
[29] S. D. Robertson, B. D. Mcnicol, J. H. D. Baas, S. C. Kloet, J. W. Jenkins, J. Catal., 1975, 37, 424-431.
[30] P. P. Upare, M.-G. Jeong, Y. K. Hwang, D. H. Kim, Y. D. Kim, D. W. Hwang, Appl. Catal. A, 2015, 491, 127-135.
[31] C. Fang, S. Kuboon, P. Khemthong, T. Butburee, P. Chakthranont, V. Itthibenchapong, Int. J. Hydrogen Energy, 2019, DOI:/10.1016/j.ijhydene.2019.03.272.
[32] J. Zelin, S. A. Regenhardt, C. I. Meyer, H. A. Duarte, V. Sebastian, A. J. Marchi, Chem. Eng. Sci., 2019, 206, 315-326.
[33] R. Arnaldo, R. Giulia, F. Riccardo, F. Alessandro, B. C. Curley, L. D. Lloyd, J. Chem. Phys., 2005, 122, 277-308.
[34] G. Treglia, B. Legrand, Phys. Rev. B, 1987, 35, 4338-4344.
[35] S. Mukherjee, J. L. Morán-López, Surf. Sci. Lett., 1987, 188, L742-L748.
[36] Q. Fu, T. Wagner, Surf. Sci. Rep., 2007, 62, 431-498.
[37] A. V. Ruban, H. L. Skriver, J. K. Nørskov, Phys. Rev. B, 1999, 59, 15990-16000. Borodziński, G. C. Bond, Catal. Rev. Sci. Eng., 2006, 48, 91-144.
[4] A. Borodziński, G. C. Bond, Catal. Rev. Sci. Eng., 2008, 50, 379-469.
[5] K. Georgios, M. B. Boucher, A. D. Jewell, E. A. Lewis, T. J. Lawton, A. E. Baber, H. L. Tierney, F. S. Maria, E. C. H. Sykes, Science, 2012, 335, 1209-1212.
[6] A. Marc, K. Kirill, B. Malte, T. Detre, G. Yuri, S. G. Robert, J. Am. Chem. Soc., 2010, 132, 14745-14747.
[7] G. X. Pei, X. Y. Liu, A. Wang, A. F. Lee, M. A. Isaacs, L. Li, X. Pan, X. Yang, X. Wang, Z. Tai, K. Wilson, T. Zhang, ACS Catal., 2015, 5, 3717-3725.
[8] G. X. Pei, X. Y. Liu, A. Wang, L. Li, Y. Huang, T. Zhang, New J. Chem., 2014, 38, 2043-2051.
[9] G. X. Pei, X. Y. Liu, X. Yang, L. Zhang, A. Wang, L. Li, H. Wang, X. Wang, T. Zhang, ACS Catal., 2017, 7, 1491-1500.
[10] M. Armbruster, M. Friedrich, M. Heggen, R. Cardoso-Gil, J. Am. Chem. Soc., 2011, 133, 9112-9118.
[11] H. Zhou, X. Yang, L. Li, X. Liu, Y. Huang, X. Pan, A. Wang, J. Li, T. Zhang, ACS Catal., 2016, 6, 1054-1061.
[12] A. J. McCue, C. J. McRitchie, A. M. Shepherd, J. A. Anderson, J. Catal., 2014, 319, 127-135.
[13] W. A. A. van Barneveld, V. Ponec, Rec. Trav. Chim., 1974, 93, 243-246.
[14] G. A. Martin, J. A. Dalmon. J. Catal., 1982, 75, 233-242.
[15] A. G. Boudjahem, M. Chettibi, S. Monteverdi, M. M. Bettahar, J. Nanosci. Nanotechnol., 2009, 9, 3546-3554.
[16] M. Chai, X. Liu, L. Li, G. Pei, Y. Ren, Y. Su, H. Cheng, A. Wang, T. Zhang, Chin. J. Catal., 2017, 38, 1338-1346.
[17] G. X. Pei, X. Y. Liu, A. Wang, Y. Su, L. Li, T. Zhang, Appl. Catal. A, 2017, 545, 90-96.
[18] Y. Liu, J. Zhao, J. Feng, Y. He, Y. Du, D. Li, J. Catal., 2018, 359, 251-260.
[19] S. A. Nikolaev, V. V. Smirnov, A. Y. Vasil'kov, V. L. Podshibikhin, Kinet. Catal., 2010, 51, 375-379.
[20] Y. Chai, G. Wu, X. Liu, Y. Ren, W. Dai, C. Wang, Z. Xie, N. Guan, L. Li, J. Am. Chem. Soc., 2019, 141, 9920-9927.
[21] F. Studt, F. Abild-Pedersen, T. Bligaard, R. Z. Sørensen, C. H. Christensen, J. K. Nørskov, Science, 2008, 320, 1320-1322.
[22] F. Studt, F. Abild-Pedersen, T. Bligaard, R. Z. Sørensen, C. H. Christensen, J. K. Nørskov, Angew. Chem., 2008, 120, 9439-9442.
[23] B. Blaise, P. R. Javier, J. Am. Chem. Soc., 2010, 132, 4321-4327.
[24] B. Yang, R. Burch, C. Hardacre, P. Hu, P. Hughes, Catal. Sci. Technol., 2017, 7, 1508-1514.
[25] B. Yang, R. Burch, C. Hardacre, G. Headdock, P. Hu, R. Burch, ACS Catal., 2012, 2, 1027-1032.
[26] H. Wei, X. Wei, X. Yang, G. Yin, A. Wang, X. Liu, T. Zhang, Chin. J. Catal., 2015, 36, 160-167.
[27] Q. Zheng, M. D. Wales, M. G. Heidlage, M. Rezac, H. Wang, S. H. Bossmann, J. Catal., 2015, 330, 222-237.
[28] M. T. Tsay, F. W. Chang, Appl. Catal. A, 2000, 203, 15-22.
[29] S. D. Robertson, B. D. Mcnicol, J. H. D. Baas, S. C. Kloet, J. W. Jenkins, J. Catal., 1975, 37, 424-431.
[30] P. P. Upare, M.-G. Jeong, Y. K. Hwang, D. H. Kim, Y. D. Kim, D. W. Hwang, Appl. Catal. A, 2015, 491, 127-135.
[31] C. Fang, S. Kuboon, P. Khemthong, T. Butburee, P. Chakthranont, V. Itthibenchapong, Int. J. Hydrogen Energy, 2019, DOI:/10.1016/j.ijhydene.2019.03.272.
[32] J. Zelin, S. A. Regenhardt, C. I. Meyer, H. A. Duarte, V. Sebastian, A. J. Marchi, Chem. Eng. Sci., 2019, 206, 315-326.
[33] R. Arnaldo, R. Giulia, F. Riccardo, F. Alessandro, B. C. Curley, L. D. Lloyd, J. Chem. Phys., 2005, 122, 277-308.
[34] G. Treglia, B. Legrand, Phys. Rev. B, 1987, 35, 4338-4344.
[35] S. Mukherjee, J. L. Morán-López, Surf. Sci. Lett., 1987, 188, L742-L748.
[36] Q. Fu, T. Wagner, Surf. Sci. Rep., 2007, 62, 431-498.
[37] A. V. Ruban, H. L. Skriver, J. K. Nørskov, Phys. Rev. B, 1999, 59, 15990-16000.

IB金属对Ni/SiO₂催化剂乙炔选择性加氢反应性能的影响

Effect of IB-metal on Ni/SiO₂ catalyst for selective hydrogenation of acetylene

PDF

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	刘诗瑶, 巩玉同, 杨晓, 张楠楠, 刘会斌, 梁长海, 陈霄. 具有富电子镍位点的耐酸金属间化合物CaNi₂Si₂催化剂用于不饱和有机酸酐/酸的水相加氢[J]. 催化学报, 2023, 50(7): 260-272.
[2]	李倩, 刘䶮, 李灿. 钯催化不对称烯丙基化/去对称化反应合成无保护基的2-喹啉酮骨架环状氨基酸[J]. 催化学报, 2023, 47(4): 222-228.
[3]	曾严, 王慧, 杨惠茹, 隽超, 李丹, 温晓东, 张帆, 邹吉军, 彭冲, 胡常伟. 镍纳米粒子耦合氧空位高效催化转化棕榈酸制备烷烃[J]. 催化学报, 2023, 47(4): 229-242.
[4]	董兴宗, 刘广业, 陈兆安, 张权, 徐云鹏, 刘中民. 性能优异的Pd-[DBU][Cl]/AC无汞催化剂在乙炔氢氯化中的应用[J]. 催化学报, 2023, 46(3): 137-147.
[5]	张平, 陈浩, 陈林, 熊鹰, 孙子其, 杨浩宇, 付莹珂, 张亚萍, 廖婷, 李斐. 基于NiZn层状双金属氢氧化物制备高效电催化CO₂还原的原子分散Ni-N-C催化剂[J]. 催化学报, 2023, 45(2): 152-161.
[6]	夏苏为, 周其兴, 孙若栩, 陈立章, 张明义, 庞欢, 徐林, 杨军, 唐亚文. 在N掺杂碳纳米管/纳米线耦合超结构中原位固载CoNi纳米颗粒制备莫特-肖特基催化剂并用于高效电催化氧还原反应[J]. 催化学报, 2023, 54(11): 278-289.
[7]	卞磊, 张紫阳, 田昊, 田娜娜, 马智, 王中利. 具有丰富晶界的铜催化剂在气-液平衡扩散电极上高效电还原CO₂制C₂H₄[J]. 催化学报, 2023, 54(11): 199-211.
[8]	张纹, 田梦, 焦海淼, 蒋海英, 唐军旺. 高匹配的BiVO₄/WO₃纳米碗异质结光阳极用于高效光电化学分解水[J]. 催化学报, 2022, 43(9): 2321-2331.
[9]	崔彤, 翟雪君, 郭莉莉, 迟京起, 张昱, 朱家伟, 孙雪梅, 王磊. 自组装百合花状超低Ru, Ni掺杂的Fe₂O₃用于大电流碱性海水电解双功能电催化[J]. 催化学报, 2022, 43(8): 2202-2211.
[10]	陈晨欣, 何苏祺, Kamran Dastafkan, 邹泽华, 汪庆祥, 赵川. 海胆状NiMoO₄纳米棒阵列作为高效双功能催化剂用于电催化及光伏驱动尿素电解[J]. 催化学报, 2022, 43(5): 1267-1276.
[11]	茆卉, 杨浩然, 柳金池, 张帅, 刘大亮, 吴琼, 孙文平, 宋溪明, 马天翼. 基于聚(两性离子液体)功能化聚吡咯/氧化石墨烯的独特MoS₂-SnS₂异质纳米片及其改善的氮还原电活性[J]. 催化学报, 2022, 43(5): 1341-1350.
[12]	李婧宇, 祁明雨, 徐艺军. 超薄Ni掺杂ZnIn₂S₄纳米片用于光催化醇裂解同时制备C-C耦合产物及氢气[J]. 催化学报, 2022, 43(4): 1084-1091.
[13]	王兰, 公宁, 周洲, 张启成, 彭文朝, 李阳, 张凤宝, 范晓彬. MOF衍生的分层多孔三维N-CoP_x/Ni₂P大电流密度下加速析氢[J]. 催化学报, 2022, 43(4): 1176-1183.
[14]	王琳琳, 李欣, 郝磊端, 洪崧, Alex W. Robertson, 孙振宇. 超细氧化铜纳米颗粒修饰二维金属有机框架协同增强二氧化碳电化学还原生成乙烯[J]. 催化学报, 2022, 43(4): 1049-1057.
[15]	于晴, 王诗怡, 王梦茹, 牟效玲, 林荣和, 丁云杰. M/C₃N₄/AC (M = Au, Pt, Ru)催化乙炔与二氯乙烷耦合反应: 双功能催化剂性能如何?[J]. 催化学报, 2022, 43(3): 820-831.