三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响

doi:10.1016/S1872-2067(17)62862-6

催化学报 ›› 2017, Vol. 38 ›› Issue (7): 1127-1137.DOI: 10.1016/S1872-2067(17)62862-6

三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响

曹红霞^a,b, 张军^a, 郭成龙^c, 陈经广^d, 任相坤^a

a 中国矿业大学低碳能源研究院, 江苏徐州 221008, 中国;
b 哥伦比亚大学地球与环境工程系, 纽约 10027, 美国;
c 中国矿业大学电气与动力工程学院, 江苏徐州 221116, 中国;
d 哥伦比亚大学化学工程系, 纽约 10027, 美国

出版日期:2017-07-18 发布日期:2017-06-27
通讯作者: 陈经广, 任相坤
基金资助:
中央高校基本科研业务费专项资金资助（2015XKMS061）.

Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation:Effect of promoter species on catalytic performance

HongXia Cao^a,b, Jun Zhang^a, ChengLong Guo^c, Jingguang G. Chen^d, XiangKun Ren^a

a Low Carbon Energy Institute, China University of Mining and Technology, Xuzhou 221008, Jiangsu, China;
b Earth and Environmental Engineering Department, Columbia University, New York 10027, United States;
c School of Electrical and Power Engineering, China University of Mining and Technology, Xuzhou 221116, Jiangsu, China;
d Department of Chemical Engineering, Columbia University, New York 10027, United States

Online:2017-07-18 Published:2017-06-27
Contact: 10.1016/S1872-2067(17)62862-6
Supported by:
This work was supported by the Fundamental Research Funds for the Central Universities (2015XKMS061).

摘要/Abstract

摘要：

作为煤制天然气的核心技术之一，CO甲烷化工艺的开发基础便是高效催化剂的研制.目前，CO甲烷化催化剂主要采用Ni作为活性组分，但如何保持其具有较高的催化活性和优异的高温稳定性，仍为当今不得不面临的棘手问题.本文以乙二醇改性的三维介孔KIT-6为载体，利用其较高的比表面积、可调孔径、独特的双螺旋三维孔道结构等特点，通过湿式浸渍法成功制备了由助剂改性的Ni基催化剂，探讨了V，Ce，La，Mn等不同助剂对Ni基催化剂CO甲烷化催化性能的影响.分别采用X射线衍射、氢气程序升温还原、氢气程序升温脱附、傅里叶变换红外光谱、透射电子显微镜、能量色散X射线光谱、激光拉曼光谱和热重分析等手段对催化剂特性进行了表征.结果显示，Ni-V/KIT-6具有最高的Ni纳米粒子分散性（26.5%）和催化还原性，产生了最多的活性位，同时，Si-O-V的形成增强了金属-载体间相互作用，并因载体的三维介孔限制效应而形成较小Ni纳米粒子，这些均有助于提升Ni基催化剂CO甲烷化的催化性能和稳定性.在常压、250-400 ℃和60000mL/（g·h）空速的实验条件下对催化剂进行了催化活性评价测试.结果表明，助剂提高了CO甲烷化低温催化活性，其中，Ni-V/KIT-6在350 ℃的条件下实现了CO的完全转化，CH₄产率也高达85%；其在常压、500 ℃和60000 mL/（g·h）空速的操作条件下所进行的稳定性测试结果还显示，Ni-V/KIT-6也具有优异的抗烧结和抗积碳能力，展示了良好的高温稳定性.因此，Ni-V/KIT-6是一种具有广阔应用前景的CO甲烷化催化剂.

关键词: 镍基催化剂, 甲烷化, 助剂, 载体, 三维介孔

Abstract:

Promoter-modified Ni-based catalysts were synthesized by an incipient-wetness impregnation method using 3D-mesoporous KIT-6 as a support modified by ethylene glycol, and evaluated for the catalytic production of synthetic natural gas (SNG) from CO methanation. Characterization results suggested that the addition of promoter species could remarkably improve the low-temperature catalytic activity for CO methanation, which was due to a large dispersion of Ni nanoparticles, an enhanced interaction between metal and support as well as a confinement effect of 3D-mesopores. Among all catalysts, Ni-V/KIT-6 possessed the best catalytic performance, which was ascribed to the largest H₂ uptake of 177.6 μmol/g and Ni dispersion of 26.5%, an intimate interaction with the support from the formation of Si-O-V linkage and an enhanced confinement effect of 3D-mesopores to effectively prevent the growth of Ni nanoparticles and carbon filaments. In consequence, Ni-V/KIT-6 displayed excellent catalytic performance as well as high catalytic stability, which can be regarded as a promising candidate for CO methanation.

Key words: Nickel-based catalyst, Methanation, Promoter, Support, 3D-mesopore

曹红霞, 张军, 郭成龙, 陈经广, 任相坤. 三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响[J]. 催化学报, 2017, 38(7): 1127-1137.

HongXia Cao, Jun Zhang, ChengLong Guo, Jingguang G. Chen, XiangKun Ren. Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation:Effect of promoter species on catalytic performance[J]. Chinese Journal of Catalysis, 2017, 38(7): 1127-1137.

×
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(17)62862-6

https://www.cjcatal.com/CN/Y2017/V38/I7/1127

参考文献

[1] M. Götz, J. Lefebvre, F. Mörs, A. M. D. Koch, F. Graf, S. Bajohr, R. Reimert, T. Kolb, Renew. Energy, 2016, 85, 1371-1390.
[2] L. Pandian, S. K. Min, D. P. Eun, Appl. Catal., 2016, 513, 98-105.
[3] X. J. Hu, W. J. Yan, W. H. Ding, J. Yu, Y. Huang, Chin. J. Catal., 2013, 34, 1720-1729.
[4] L. Bian, W. H. Wang, R. Xia, Z. H. Li, RSC Adv., 2016, 6, 677-686.
[5] J. Sehested, S. Dahl, J. Jacobsen, J. R. Rostrup-Nielsen, J. Phys. Chem. B, 2005, 109, 2432-2438.
[6] L. K. Zhou, Z. L. Li, J. F. Pang, M. Y. Zheng, A. Q. Wang, T. Zhang, Chin. J. Catal., 2015, 36, 1694-1700.
[7] S. Carenco, C. Sassoye, M. Faustini, P. Eloy, D. P. Debecker, H. Bluhm, M. Salmeron, J. Phys. Chem. C, 2016, 120, 15354-15361.
[8] W. B. Shi, X. L. Liu, J. L. Zeng, J. Wang, Y. D. Wei, T. Y. Zhu, Chin. J. Catal., 2016, 37, 1181-1192.
[9] W. Kim, K. Y. Koo, H. J. Lee, Y. G. Shul, W. L. Yoon, Int. J. Hydrogen Energy, 2015, 40, 10033-10040.
[10] H. Liu, Y. Lin, Z. Ma, Chin. J. Catal., 2016, 37, 73-82.
[11] C. Galletti, S. Specchia, V. Specchia, Chem. Eng. J., 2011, 167, 616-621.
[12] M. A. Lucchini, A. Testino, A. Kambolis, C. Proff, C. Ludwig, Appl. Catal. B, 2016, 182, 94-101.
[13] S. Abate, K. Barbera, E. Giglio, F. Deorsola, S. Bensaid, S. Perathon-er, R. Pirone, G. Centi, Ind. Eng. Chem. Res., 2016, 55, 8299-8308.
[14] H. Zhang, Y. Y. Dong, W. P. Fang, Y. X. Lian, Chin. J. Catal., 2013, 34, 330-335.
[15] T. Miyao, S. Sakurabayashi, W. H. Shen, K. Higashiyama, M. Watanabe. Catal. Commun., 2015, 58, 93-96.
[16] X. Li, X. Z. Yang, H. D. Tang, H. Z. Liu, Chin. J. Catal., 2011, 32, 1400-1404.
[17] J. J. Gao, C. M. Jia, J. Li, M. J. Zhang, F. N. Gu, G. W. Xu, Z. Y. Zhong, F. B. Su, J. Energy Chem., 2013, 22, 919-927.
[18] A. M. Zhao, W. Y. Ying, H. T. Zhang, H. F. Ma, D. Y. Fang, Catal. Commun., 2012, 17, 34-38.
[19] M. Tao, X. Meng, Y. H. Lv, Z. C. Bian, Z. Xin, Fuel, 2016, 165, 289-297.
[20] M. Tao, Z. Xin, X. Meng, Z. C. Bian, Y. H. Lv, Fuel, 2017, 188, 267-276.
[21] B. W. Lu, Y. W. Ju, T. Abe, K. Kawamoto, RSC Adv., 2015, 5, 56444-56454.
[22] J. Y. Zhang, Z. Xin, X. Meng, M. Tao, Fuel, 2013, 109, 693-701.
[23] B. Dai, B. Wen, M. Y. Zhu, L. H. Kang, F. Yu, RSC Adv., 2016, 6, 66957-66962.
[24] M. A. A. Aziz, A. A. Jalil, S. Triwahyono, R. R. Mukti, Y. H. Taufiq-Yap, M. R. Sazegar, Appl. Catal. B, 2014, 147, 359-368.
[25] Q. Liu, F. N. Gu, X. P. Lu, Y. J. Liu, H. F. Li, Z. Y. Zhong, G. W. Xu, F. B. Su, Appl. Catal. A, 2014, 488, 37-47.
[26] Y. Zeng, H. F. Ma, H. T. Zhang, W. Y. Ying, D. Y. Fang, Fuel, 2015, 162, 16-22.
[27] G. J. Zhi, X. N. Guo, Y. Y. Wang, G. Q. Jin, X. Y. Guo, Catal. Commun., 2011, 16, 56-59.
[28] K. H. Song, X. Yan, D. J. Koh, T. Kim, J. S. Chung. Appl. Catal. A, 2017, 530, 184-192.
[29] D. E. Rivero-Mendoza, J. N. G. Stanley, J. Scott, K. F. Aguey-Zinsou. Catalysts, 2016, 6, 170-185.
[30] K. C. Zhao, Z. H. Li, L. Bian. Front. Chem. Sci. Eng., 2016, 10, 273-280.
[31] J. Happel, I. Suzuki, P. Kokayeff, V. Fthenakis, J. Catal., 1980, 65, 59-77.
[32] J. Liu, C. M. Li, F. Wang, S. He, H. Chen, Y. F. Zhao, M. Wei, D. G. Evansa, X. Duan, Catal. Sci. Technol., 2013, 3, 2627-2633.
[33] P. Xu, Z. X. Wu, J. G. Deng, Y. X. Liu, S. H. Xie, G. S. Guo, H. X. Dai, Chin. J. Catal., 2017, 38, 92-105.
[34] B. T. Li, X. Luo, J. Huang, X. J. Wang, Z. X. Liang, Chin. J. Catal., 2017, 38, 518-528.
[35] F. Kleitz, S. H. Choi, R. Ryoo, Chem. Commun., 2003, 2136-2137.
[36] Q. Liu, J. J. Gao, M. J. Zhang, H. F. Li, F. N. Gu, G. W. Xu, Z. Y. Zhong, F. B. Su, RSC Adv., 2014, 4, 16094-16103.
[37] X. Z. Yang, Wendurima, G. J. Gao, Q. Q. Shi, X. Wang, J. N. Zhang, C. H. Han, J. Wang, H. L. Lu, J. Liu, M. Tong, Int. J. Hydrogen Energy, 2014, 39, 3231-3242.
[38] F. Kleitz, F. Berube, R. Guillet-Nicolas, C. M. Yang, M. Thommes, J. Phys. Chem. C, 2010, 114, 9344-9355.
[39] J. Sun, Q. B. Kan, Z. F. Li, G. L. Yu, H. Liu, X. Y. Yang, Q. S. Huo, J. Q. Guan, RSC Adv., 2014, 4, 2310-2317.
[40] H. D. Li, J. Ren, X. Qin, Z. F. Qin, J. Y. Lin, Z. Li, RSC Adv., 2015, 5, 96504-96517.
[41] X. Y. Liu, B. Z. Tian, C. Z. Yu, F. Gao, S. H. Xie, B. Tu, R. C. Che, L. M. Peng, D. Y. Zhao, Angew. Chem. Int. Ed., 2002, 41, 3876-3878.
[42] Q. Zhang, T. J. Wang, B. Li, T. Jiang, L. L. Ma, X. H. Zhang, Q. Y. Liu, Appl. Energy, 2012, 97, 509-513.
[43] C. F. Wu, L. Z. Wang, P. T. Williams, J. Shi, J. Huang, Appl. Catal. B, 2011, 108, 6-13.
[44] S. Velu, S. K. Gangwal, Solid State Ionics, 2006, 177, 803-811.
[45] Z. C. Liu, J. Zhou, K. Cao, W. M. Yang, H. X. Gao, Y. D. Wang, H. X. Li, Appl. Catal. B, 2012, 125, 324-330.
[46] M. Piumetti, B. Bonelli, P. Massiani, S. Dzwigaj, I. Rossetti, S. Casale, M. Armandi, C. Thomas, E. Garrone, Catal. Today, 2012, 179, 140-148.
[47] Y. Y. Fu, Y. N. Wu, W. J. Cai, B. Yue, H. Y. He, Sci. China Chem., 2015, 58, 148-155.
[48] W. C. Zhang, Y. L. Guo, Y. Q. Wang, Y. Guo, G. Z. Lu, J. Rare Earths, 2010, 28, 369-375.
[49] V. K. Tomer, S. Duhan, P. V. Adhyapak, I. S. Mulla, J. Am. Ceram. Soc., 2015, 98, 741-747.
[50] G. Ricchiardi, A. Damin, S. Bordiga, C. Lamberti, G. Spano, F. Rivetti, A. Zecchina, J. Am. Chem. Soc., 2001, 123, 11409-11419.
[51] X. T. Gao, S. R. Bare, B. M. Weckhuysen, I. E. Wachs, J. Phys. Chem. B, 1998, 102, 10842-10852.
[52] Q. L. Liu, J. M. Li, Z. Zhao, M. L. Gao, L. Kong, J. Liu, Y. C. Wei. Catal. Sci. Technol., 2016, 6, 5927-5941
[53] G. Xiong, C. Li, H. Y. Li, Q. Xin, Z. C. Feng, Chem. Commun., 2000, 8, 677-678.
[54] G. Du, S. Lim, M. Pinault, C. Wang, F. Fang, L. Pfefferle, G. L. Haller, J. Catal., 2008, 253, 74-90.

三维介孔KIT-6上高分散Ni纳米粒子用于CO甲烷化:助剂对催化性能的影响

Highly dispersed Ni nanoparticles on 3D-mesoporous KIT-6 for CO methanation:Effect of promoter species on catalytic performance

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]	刘赵春, 宗雪, Dionisios G. Vlachos, Ivo A. W. Filot, Emiel J. M. Hensen. 金属掺杂SnO₂电化学还原CO₂制甲酸的计算研究[J]. 催化学报, 2023, 50(7): 249-259.
[2]	张锋伟, 郭河芳, 刘萌萌, 赵阳, 洪峰, 李静静, 董正平, 乔波涛. 表面应力介导的碳基Pt纳米催化剂用于硝基芳烃的高选择性加氢[J]. 催化学报, 2023, 48(5): 195-204.
[3]	李航杰, 肖月华, 肖佳乐, 范凯, 李炳宽, 李晓龙, 王亮, 肖丰收. 镓改性的铜基疏水催化剂用于CO₂选择性加氢制二甲醚的研究[J]. 催化学报, 2023, 54(11): 178-187.
[4]	张华阳, 田文婕, 段晓光, 孙红旗, 黄应平, 方艳芬, 王少彬. 金属基载体支撑的单原子催化剂用于光催化还原反应[J]. 催化学报, 2022, 43(9): 2301-2315.
[5]	高广, 赵泽伦, 王嘉, 席永杰, 孙鹏, 李福伟. PtReO_x/TiO₂金属-氧化物-载体相互作用增强手性羧酸选择性加氢[J]. 催化学报, 2022, 43(8): 2034-2044.
[6]	李鹏, 赵国强, 程宁燕, 夏力学, 李晓宁, 陈亚平, 劳梦梦, 程振祥, 赵焱, 徐迅, 姜银珠, 潘洪革, 窦士学, 孙文平. 过渡金属单原子功能化碳载体促进碱性氢电催化反应动力学[J]. 催化学报, 2022, 43(5): 1351-1359.
[7]	钟威, 许家超, 王苹, 朱必成, 范佳杰, 余火根. 新型核壳Ag@AgSe_x纳米粒子析氢助剂: 原位表面硒化以提升TiO₂的光催化产氢活性[J]. 催化学报, 2022, 43(4): 1074-1083.
[8]	刘军辉, 宋亚坤, 郭旭明, 宋春山, 郭新闻. 铁基催化剂在CO_x加氢制高附加值烃反应中的应用[J]. 催化学报, 2022, 43(3): 731-754.
[9]	王可, 何仕辉, 林云志, 陈旬, 戴文新, 付贤智. 氧空位修饰的暴露TiO₂{001}的Ru/TiO₂增强光热协同CO₂甲烷化活性和稳定性[J]. 催化学报, 2022, 43(2): 391-402.
[10]	洪峰, 王升扬, 张军营, 付俊红, 蒋齐可, 孙科举, 黄家辉. 金属载体强相互作用增强Au/TiO₂催化剂在3-硝基苯乙烯选择性加氢反应的活性[J]. 催化学报, 2021, 42(9): 1530-1537.
[11]	陈军伟, 欧祖翘, 陈海鑫, 宋树芹, 王昆, 王毅. 电催化剂纳米碳基载体的研究进展[J]. 催化学报, 2021, 42(8): 1297-1326.
[12]	罗靖洁, 董亚南, Corinne Petit, 梁长海. 不可还原材料负载的纳米金催化剂: 理性设计与优化[J]. 催化学报, 2021, 42(5): 670-693.
[13]	赵东越, 杨岳溪, 高中楠, 尹萌欣, 田野, 张静, 姜政, 于晓波, 李新刚. 贫燃/富燃循环气氛下原位活化Pd负载钙钛矿催化剂促进NO_x还原消除[J]. 催化学报, 2021, 42(5): 795-807.
[14]	冯小辉, 刘瑞, 徐香兰, 佟云艳, 张诗婧, 何佳城, 徐骏伟, 方修忠, 王翔. 构建稳定的CuO/La₂Sn₂O₇催化剂用于碳烟颗粒燃烧: CuO在La₂Sn₂O₇烧绿石复合氧化物载体上的单层分散行为[J]. 催化学报, 2021, 42(3): 396-408.
[15]	谭媛, 刘晓艳, 张磊磊, 刘菲, 王爱琴, 张涛. 纳米金催化肉桂醛选择加氢制肉桂醇[J]. 催化学报, 2021, 42(3): 470-481.