Rh2O3/介孔MOx-Al2O3(M=Mn,Fe,Co,Ni,Cu,Ba)催化剂:合成、表征和催化应用

doi:10.1016/S1872-2067(15)60951-2

摘要/Abstract

摘要：

近年来,研究者们开发了自组装合成介孔氧化铝的方法,并以介孔氧化铝为载体负载金属氧化物,还尝试合成介孔MO_x-Al₂O₃复合氧化物.但以介孔MO_x-Al₂O₃复合氧化物为载体负载金属氧化物,并将这类材料用于催化中的例子相对较少.本工作以非离子型三嵌段共聚物(P123)为模板剂,异丙醇铝为氧化铝前驱物,采用一锅法快速制备了有序介孔Al₂O₃(MA)及一系列MO_x-Al₂O₃(M=Mn,Fe,Co,Ni,Cu,Ba)材料,并以这些材料为载体采用浸渍法制备了Rh/MA和Rh/M-MA催化剂.采用N₂吸附-脱附、X射线粉末衍射、透射电镜、X射线光电子能谱及电感偶合等离子体发射光谱等对催化剂结构和性质进行了表征,考察了催化剂对CO氧化和N₂O分解的催化活性和稳定性.
结果表明,一锅法制备的各催化剂均有大的比表面积、大的孔容和均一的孔径.Rh/Mn-MA和Rh/Fe-MA中掺杂金属氧化物分别为MnO₂和Fe₂O₃,在Rh/Co-MA和Rh/Ni-MA上,Co和Ni分别与介孔氧化铝形成了NiAl₂O₄尖晶石结构;Rh/Cu-MA上还有CuO和少量Cu⁺;对于Rh/Ba-MA催化剂, 其载体的介孔有序性被破坏并有BaCO₃生成.在所有催化剂上,负载的Rh₂O₃颗粒高度分散,其颗粒尺寸分布在1nm左右.对于CO氧化,催化剂的T₅₀(CO转化率到达到50%的温度)活性顺序为:Rh/Mn-MA(122℃)>Rh/Fe-MA(130℃)≈Rh/Cu-MA(131℃)>Rh/Co-MA(136℃)>Rh/Ni-MA(156℃)>Rh/MA(161℃)>Rh/Ba-MA(171℃).大多数载体在200℃以下没有活性.对于N₂O分解,催化剂的T₅₀(N₂O转化率到达到50%的温度)活性顺序为:Rh/Co-MA(283℃)>Rh/Ni-MA(287℃)≈Rh/Fe-MA(290℃)≈Rh/Ba-MA(292℃)>Rh/MA(301℃)>Rh/Cu-MA(314℃)>Rh/Mn-MA(321℃).这些载体在400℃以下都没有活性
实验证明,通过掺杂的方法可以调变介孔Al₂O₃的物理化学性质,负载Rh₂O₃后,催化性能进一步被调变.虽然本文仅选取CO氧化和N₂O分解作为探针反应来比较这一类介孔氧化物材料的催化活性,考虑到Rh₂O₃和Al₂O₃在催化中的广泛使用,我们认为这些催化剂有可能用在其他反应中.

关键词: 一锅法, 介孔氧化铝, 金属氧化物, CO氧化, N₂O分解

Abstract:

Recently, a one-pot self-assembly method was proposed for the synthesis of mesoporous Al₂O₃ and MO_x-Al₂O₃ composite materials. However, few attempts have been made to use mesoporous MO_x-Al₂O₃ composites to support metal oxides for catalysis. In the present work, mesoporous MO_x-Al₂O₃ (M = Mn, Fe, Co, Ni, Cu, Ba) materials were prepared by a one-pot self-assembly method using Pluronic P123 as a structure-directing agent. The obtained mesoporous materials were loaded with Rh₂O₃ nanoparticles via impregnation with Rh(NO₃)₃ followed by calcination in air at 500 ℃. The resulting catalysts were characterized by X-ray diffraction, N₂ adsorption-desorption measurements, transmission electron microscopy, inductively coupled plasma optical emission spectrometry, X-ray photoelectron spectroscopy, and their catalytic activity and stability for CO oxidation and N₂O decomposition were tested. The Rh₂O₃ nanoparticles were found to be on the order of 1 nm in size and were highly dispersed on the high surface area mesoporous MO_x-Al₂O₃ supports. A number of the Rh₂O₃/mesoporous MO_x-Al₂O₃ catalysts exhibited higher catalytic activity than the Rh₂O₃/mesoporous Al₂O₃ prepared for comparison.

Key words: One-pot synthesis, Mesoporous alumina, Metal oxide, CO oxidation, N₂O decomposition

刘欢, 林毅, 马臻. Rh₂O₃/介孔MO_x-Al₂O₃(M=Mn,Fe,Co,Ni,Cu,Ba)催化剂:合成、表征和催化应用[J]. 催化学报, 2016, 37(1): 73-82.

Huan Liu, Yi Lin, Zhen Ma. Rh₂O₃/mesoporous MO_x-Al₂O₃ (M = Mn, Fe, Co, Ni, Cu, Ba) catalysts: Synthesis, characterization, and catalytic applications[J]. Chinese Journal of Catalysis, 2016, 37(1): 73-82.

×
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(15)60951-2

https://www.cjcatal.com/CN/Y2016/V37/I1/73

参考文献

[1] J. S. Beck, J. C. Vartuli, W. J. Roth, M. E. Leonowicz, C. T. Kresge, K. D. Schmitt, C. T. W. Chu, D. H. Olson, E. W. Sheppard, S. B. Mccullen, J. B. Higgins, J. L. Schlenker, J. Am. Chem. Soc., 1992, 114, 10834.
[2] D. Y. Zhao, Q. S. Huo, J. L. Feng, B. F. Chmelka, G. D. Stucky, J. Am. Chem. Soc., 1998, 120, 6024.
[3] A. Corma, Chem. Rev., 1997, 97, 2373.
[4] J. Y. Ying, C. P. Mehnert, M. S. Wong, Angew. Chem. Int. Ed., 1999, 38, 56.
[5] D. T. On, D. Desplantier-Giscard, C. Danumah, S. Kaliaguine, Appl. Catal. A., 2003, 253, 545.
[6] Y. Wan, D. Y. Zhao, Chem. Rev., 2007, 107, 2821.
[7] H. Tüysüz, F. Schüth, Adv. Catal., 2012, 55, 127.
[8] F. Schüth, Chem. Mater., 2001, 13, 3184.
[9] Y. Ren, Z. Ma, P. G. Bruce, Chem. Soc. Rev., 2012, 41, 4909.
[10] D. Gu, F. Schüth, Chem. Soc. Rev., 2014, 43, 313.
[11] C. N. Satterfield, Heterogeneous Catalysis in Industrial Practice, 2nd ed., Krieger Publishing, Malabar, Florida, 1991.
[12] S. A. Bagshaw, E. Prouzet, T. J. Pinnavaia, Science, 1995, 269, 1242.
[13] F. Vaudry, S. Khodabandeh, M. E. Davis, Chem. Mater., 1996, 8, 1451.
[14] Z. R. Zhang, T. J. Pinnavaia, J. Am. Chem. Soc., 2002, 124, 12294.
[15] B. Z. Tian, H. F. Yang, X. Y. Liu, S. H. Xie, C. Z. Yu, J. Fan, B. Tu, D. Y. Zhao, Chem. Commun., 2002, 1824.
[16] B. Z. Tian, X. Y. Liu, B. Tu, C. Z. Yu, J. Fan, L. M. Wang, S. H. Xie, G. D. Stucky, D. Y. Zhao, Nat. Mater., 2003, 2, 159.
[17] K. Niesz, P. D. Yang, G. A. Somorjai, Chem. Commun., 2005, 1986.
[18] Q. Yuan, A. X. Yin, C. Luo, L. D. Sun, Y. W. Zhang, W. T. Duan, H. C. Liu, C. H. Yan, J. Am. Chem. Soc., 2008, 130, 3465.
[19] S. M. Morris, P. F. Fulvio, M. Jaroniec, J. Am. Chem. Soc., 2008, 130, 15210.
[20] L. B. Sun, W. H. Tian, X. Q. Liu, J. Phys. Chem. C, 2009, 113, 19172.
[21] W. Li, C. Y. Cao, L. Y. Wu, M. F. Ge, W. G. Song, J. Hazard Mater., 2011, 198, 143.
[22] H. Oveisi, A. Beitollahi, M. Imura, C. W. Wu, Y. Yamauchi, Microporous Mesoporous Mater., 2010, 134, 150.
[23] S. M. Morris, J. A. Horton, M. Jaroniec, Microporous Mesoporous Mater., 2010, 128, 180.
[24] D. H. Pan, M. Guo, M. He, S. W. Chen, X. Wang, F. Yu, R. F. Li, J. Mater. Res., 2014, 29, 811.
[25] W. Q. Cai, J. G. Yu, C. Anand, A. Vinu, M. Jaroniec, Chem. Mater., 2011, 23, 1147.
[26] X. Y. Wang, D. H. Pan, M. Guo, M. He, P. Y. Niu, R. F. Li, Mater. Lett., 2013, 97, 27.
[27] Q. P. Sun, Y. Zheng, Z. H. Li, Y. Zheng, Y. H. Xiao, G. H. Cai, K. M. Wei, Phys. Chem. Chem. Phys., 2013, 15, 5670.
[28] Q. P. Sun, Y. Zheng, Y. Zheng, Y. H. Xiao, G. H. Cai, K. M. Wei, Scrip. Mater., 2011, 65, 1026.
[29] Q. Yuan, H. H. Duan, L. L. Li, Z. X. Li, W. T. Duan, L. S. Zhang, W. G. Song, C. H. Yan, Adv. Mater., 2010, 22, 1475.
[30] D. Shee, A. Sayari, Appl. Catal. A, 2010, 389, 155.
[31] R. Y. Liu, M. H. Yang, C. J. Huang, W. Z. Weng, H. L. Wan, Chin. J. Catal., 2013, 34, 146.
[32] H. Q. Jiang, H. Bongard, W. Schmidt, F. Schüth, Microporous Mesoporous Mater., 2012, 164, 3.
[33] Y. F. Zhu, X. Kong, X. Q. Li, G. Q. Ding, Y. L. Zhu, Y. W. Li, ACS Catal., 2014, 4, 3612.
[34] L. L. Xu, H. L. Song, L. J. Chou, Catal. Sci. Technol., 2011, 1, 1032.
[35] K. Tao, L. Shi, Q. X. Ma, D. Wang, C. Y. Zeng, C. L. Kong, M. B. Wu, L. Chen, S. H. Zhou, Y. B. Hu, N. Tsubaki, Chem. Eng. J., 2013, 221, 25.
[36] X. Huang, N. N. Sun, G. X. Xue, C. Z. Wang, H. J. Zhan, N. Zhao, F. K. Xiao, W. Wei, Y. H. Sun, RSC Adv., 2015, 5, 21090.
[37] L. L. Xu, H. L. Song, L. J. Chou, Appl. Catal. B, 2011, 108-109, 177.
[38] W. H. Shen, H. Momoi, K. Komatsubara, T. Saito, A. Yoshida, S. Naito, Catal. Today, 2011, 171, 150.
[39] L. L. Xu, H. L. Song, L. J. Chou, ACS Catal., 2012, 2, 1331.
[40] L. L. Xu, Z. C. Miao, H. L. Song, L. J. Chou, Int. J. Hydrogen Energy, 2014, 39, 3253.
[41] N. Wang, K. Shen, L. H. Huang, X. P. Yu, W. Z. Qian, W. Chu, ACS Catal., 2013, 3, 1638.
[42] N. Wang, Z. X. Xu, J. Deng, K. Shen, X. P. Yu, W. Z. Qian, W. Chu, F. Wei, ChemCatChem, 2014, 6, 1470.
[43] S. B. Cao, A. H. Chen, Y. B. Zhao, Y. L. Lu, Nanoscale, 2015, 7, 5612.
[44] J. Horiguchi, Y. Kobayashi, S. Kobayashi, Y. Yamazaki, K. Omata, D. Nagao, M Konno, M. Yamada, Appl. Catal. A, 2011, 392, 86.
[45] Y. J. Bang, S. J. Han, J. G. Seo, M. H. Youn, J. H. Song, I. K. Song, Int. J. Hydrogen Energy, 2012, 37, 17967.
[46] S. J. Han, Y. Bang, J. Yoo, S. Park, K. H. Kang, J. H .Choi, J. W. Song, I. K. Song, Int. J. Hydrogen Energy, 2014, 39, 10445.
[47] W. H. Shen, K. Komatsubara, T. Hagiyama, A. Yoshida, S. Naito, Chem. Commun., 2009, 6490.
[48] Y. Wang, S. H. Xie, B. Yue, S. J. Feng, H. Y. He, Chin. J. Catal., 2010, 31, 1054.
[49] Y. J. Wang, M. N. Guo, J. Q. Lu, M. F. Luo, Chin. J. Catal., 2011, 32, 1496.
[50] L. L. Xu, H. H. Zhao, H. L. Song, L. J. Chou, Int. J. Hydrogen Energy, 2012, 37, 7497.
[51] C. M. A. Parlett, L. J. Durndell, K. Wilson, D. W. Bruce, N. S. Hondow, A. F. Lee, Catal. Commun., 2014, 44, 40.
[52] L. L. Pérez, C. Alvarez-Galván, V. Zarubina, B. O. Figueiredo Fernandes, I. Melián-Cabrera, CrystEngComm, 2014, 16, 6775.
[53] A. H. Chen, T. Miyao, K. Higashiyama, H. Yamashita, M. Watanabe, Angew. Chem. Int. Ed., 2010, 49, 9895.
[54] H. Tan, K. Li, S. Sioud, D. Cha, M. H. Amad, M. N. Hedhili, Z. A. Al-Talla, Catal. Commun., 2012, 26, 248.
[55] R. D. Zhang, P. X. Li, N. Liu, W. Yang, X. D. Wang, R. Cui, B. H. Chen, Catal. Today, 2013, 216, 169.
[56] L. L. Xu, H. L. Song, L. J. Chou, Int. J. Hydrogen Energy, 2013, 38, 7307.
[57] L. L. Xu, Z. C. Miao, H. L. Song, W. Chen, L. J. Chou, Catal. Sci. Technol., 2014, 4, 1759.
[58] S. J. Zhou, Y. M. Zhou, J. J. Shi, Y. W. Zhang, X. L. Sheng, Z. W. Zhang, J. Mater. Sci., 2015, 50, 3984.
[59] Q. Liu, J. J. Gao, F. N. Gu, X. P. Lu, Y. J. Liu, H. F. Li, Z. Y. Zhong, B. Liu, G. W. Xu, F. B. Su, J. Catal., 2015, 326, 127.
[60] A. Bueno-López, I. Such-Basáñez, C. S. M. de Lecea, J. Catal., 2006, 244, 102.
[61] J. Oi, A. Obuchi, G. R. Bamwenda, A. Ogata, H. Yagita, S. Kushiyama, K. Mizuno, Appl. Catal. B, 1997, 12, 277.
[62] Y. F. Han, F. X. Chen, Z. Y. Zhong, K. Ramesh, L. W. Chen, E. Widjaja, J. Phys. Chem. B, 2006, 110, 24450.
[63] Y. P. Huang, Z. Y. Liang, Y. E. Miao, T. X. Liu, ChemNanoMat, 2015, 1, 159.
[64] H. D. Liu, J. L. Zhang, D. D. Xu, L. H. Huang, S. Z. Tan, W. J. Mai, J. Solid State Electrochem., 2015, 19, 135.
[65] M. Salavati-Niasari, M. Farhadi-Khouzani, F. Davar, J. Sol-Gel Sci. Technol., 2009, 52, 321.
[66] N. Srisawad, W. Chaitree, O. Mekasuwandumrong, P. Praserthdam, J. Panpranot, J. Nanomater., 2012, 108369.
[67] F. Tielens, M Calatayud, R Franco, J M Recio, J Perez-Ramirez, C. Minot, J. Phys. Chem. B, 2006, 110, 988.
[68] Y. Xiong, X. J. Yao, C. J. Tang, L. Zhang, Y. Cao, Y. Deng, F. Gao, L.Dong, Catal. Sci. Technol., 2014, 4, 4416.
[69] C. He, Y. K. Yu, L. Yue, N. L. Qiao, J. J. Li, Q. Shen, W. J. Yu, J. S. Chen, Z. P. Hao, Appl. Catal. B, 2014, 147, 156.
[70] P Nachimuthu, Y J Kim, S V N T Kuchibhatla, Z Q Yu, W Jiang, M H Engelhard, V. Shutthanandan, J. Szanyi, S. Thevuthasan, J. Phys. Chem. C, 2009, 113, 14324.
[71] Y. Ren, Z. Ma, S. Dai, Materials, 2014, 7, 3547.
[72] Y. P. Cai, H G Stenger Jr, C. E. Lyman, J. Catal., 1996, 161, 123.
[73] V. R. Pérez, M. Á. V. Beltrán, Q. G. He, Q. Wang, C. S. M. de Lecea, A. B. López, Catal. Commun., 2013, 33, 47.
[74] S. Parres-Esclapez, M. J. Illán-Gómez, C. S. M. de Lecea, A. Bueno-López, Appl. Catal. B, 2010, 96, 370.
[75] L. Chmielarz, P. Ku?trowski, M. Drozdek, M. Rutkowska, R. Dziembaj, M. Michalik, P. Cool, E. F. Vansant, J. Porous Mater., 2011, 18, 483.
[76] M. Hussain, P. Akhter, D. Fino, N. Russo, J. Environ. Chem. Eng., 2013, 1, 164.
[77] A. Bueno-López, I. Such-Basáñez, C. S. M. de Lecea, J. Catal., 2006, 244, 102.
[78] Y. Lin, T. Meng, Z. Ma, J. Ind. Eng. Chem., 2015, 28, 138.

Rh₂O₃/介孔MO_x-Al₂O₃(M=Mn,Fe,Co,Ni,Cu,Ba)催化剂:合成、表征和催化应用

Rh₂O₃/mesoporous MO_x-Al₂O₃ (M = Mn, Fe, Co, Ni, Cu, Ba) catalysts: Synthesis, characterization, and catalytic applications

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]	吴尧, 杨杰夫, 郑媚, 胡点轶, Teddy Salim, 汤碧珺, 刘政, 李述周. 直接化学气相沉积法制备二维钴铁氧体用于高效析氧反应[J]. 催化学报, 2023, 55(12): 265-277.
[2]	吴沛文, 邓畅, 刘锋, 朱昊男, 陈琳琳, 刘若禹, 朱文帅, 徐春明. 磁性可循环高熵金属氧化物催化剂用于活化氧气催化氧化脱硫[J]. 催化学报, 2023, 54(11): 238-249.
[3]	翁雪霏, 杨双莉, 丁丁, 陈明树, 万惠霖. 宽波段原位红外吸收光谱在Pd/SiO₂和Cu/SiO₂催化剂上CO氧化中的应用[J]. 催化学报, 2022, 43(8): 2001-2009.
[4]	欧阳, 李松达, 王飞, 段心怡, 袁文涛, 杨杭生, 张泽, 王勇. 二氧化钛负载的铂纳米颗粒在CO和O₂环境下表面平台位点和台阶位点的可逆转变[J]. 催化学报, 2022, 43(8): 2026-2033.
[5]	朱纯, 梁锦霞, 王阳刚, 李隽. MXene负载的非贵金属单原子催化剂催化CO氧化反应[J]. 催化学报, 2022, 43(7): 1830-1841.
[6]	卢海娇, 李显龙, Sabiha Akter Monny, 王志亮, 王连洲. 基于过渡金属氧化物半导体上光电催化生产过氧化氢[J]. 催化学报, 2022, 43(5): 1204-1215.
[7]	董春燕, 周燕, 塔娜, 刘雯璐, 李名润, 申文杰. 氧化铈形貌对Pd纳米粒子分散的影响[J]. 催化学报, 2021, 42(12): 2234-2241.
[8]	郑珠媛, 王栋, 张毅, 杨帆, 龚学庆. CeO₂/Pt(111)反向催化剂结构和活性的密度泛函理论研究[J]. 催化学报, 2020, 41(9): 1360-1368.
[9]	Linxi Wang, Shyam Deo, Kerry Dooley, Michael J. Janik, Robert M. Rioux. 金属核及氧化铈的物理化学性质对一氧化碳氧化的影响[J]. 催化学报, 2020, 41(6): 951-962.
[10]	高玉仙, 张振华, 李兆瑞, 黄伟新. 从头开始理解形貌依赖的CuO_x-CeO₂相互作用[J]. 催化学报, 2020, 41(6): 1006-1016.
[11]	Valentín Briega-Martos, Enrique Herrero, Juan M. Feliu. Pt单晶电极上氧和过氧化氢还原反应研究进展[J]. 催化学报, 2020, 41(5): 732-738.
[12]	李双德, 王东东, 武晓峰, 陈运法. 水滑石衍生的复合氧化物催化氧化挥发性有机气体的研究进展[J]. 催化学报, 2020, 41(4): 550-560.
[13]	邓天宇, 许光月, 傅尧. Cu/SBA-15-SO₃H催化木糖一锅转化制备糠醇[J]. 催化学报, 2020, 41(3): 404-414.
[14]	鲍佳锋, 陈皓, 杨是赜, 张鹏飞. 基于机械化学的高比表面积Co_xMn_1-xO_y催化剂合成及其VOCs燃烧研究[J]. 催化学报, 2020, 41(12): 1846-1854.
[15]	张健, 阎婷婷, 杨宇森, 孙嘉略, 林彦军, 卫敏. Zn-Zr-Al氧化物催化乙醇合成碳酸二乙酯[J]. 催化学报, 2019, 40(4): 515-522.