OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能

doi:10.3866/PKU.WHXB201704282

物理化学学报 >> 2017, Vol. 33 >> Issue (9): 1855-1864.doi: 10.3866/PKU.WHXB201704282

OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能

傅之丹,臧佳欣,叶青*(),程水源,康天放

北京工业大学区域大气复合污染防治北京市重点实验室,北京100124

收稿日期:2017-03-17 发布日期:2017-07-05
通讯作者: 叶青 E-mail:yeqing@bjut.edu.cn
基金资助:
国家自然科学基金(21277008);国家自然科学基金(20777005);北京市自然科学基金(8082008);和北京市教委教师队伍建设(IDHT20140504)

Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate

Zhi-Dan FU,Jia-Xin ZANG,Qing YE*(),Shui-Yuan CHENG,Tian-Fang KANG

Key Laboratory of Beijing on Regional Air Pollution Control, Beijing University of Technology, Beijing 100124, P. R. China

Received:2017-03-17 Published:2017-07-05
Contact: Qing YE E-mail:yeqing@bjut.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China(21277008);The project was supported by the National Natural Science Foundation of China(20777005);Natural Science Foundation of Beijing, China(8082008);Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality(IDHT20140504)

摘要/Abstract

摘要：

采用氧化还原法合成了层状锰氧化物（OL），并以OL为载体采用离子交换法制备了不同Cu负载量的Cu_x/OL催化剂。利用X射线衍射（XRD）、电子扫描电镜（SEM）、N₂吸附/脱附、H₂-程序升温还原（H₂-TPR）、TG（热重）、X射线光电子能谱（XPS）、O₂-程序升温脱附（O₂-TPD）等技术对所制催化剂进行结构和织构表征，并对其催化氧化CO及乙酸乙酯活性进行了评价。结果表明，OL具有典型的层状锰氧化物结构，适量掺杂Cu对OL的结构和织构影响不大，但Cu的掺杂明显影响Cu_x/OL的还原性、氧移动性及催化剂表面Cu²⁺/CuO、（Mn²⁺+Mn³⁺）/Mn⁴⁺和O_ads/O_latt的比例。Cu_x/OL的催化性能与以上因素密切相关。在Cu_x/OL样品中，Cu₅/OL催化剂具有最佳的催化活性（CO催化氧化，T₅₀=70 ℃和T₉₀=100 ℃；乙酸乙酯催化氧化T₅₀=160 ℃，T₉₀=200 ℃）。同时，Cu₅/OL催化剂具有最佳的还原性能、氧移动性能和最多的Cu²⁺、（Mn²⁺+Mn³⁺）和表面吸附氧浓度。Cu_x/OL催化性能与铜锰之间相互作用、还原性和氧移动性能密切相关。

关键词: 层状锰氧化物, Cu_x/OL, 一氧化碳, 乙酸乙酯, 催化氧化

Abstract:

Octahedral layered birnessite (denoted as OL) was synthesized by the oxidation-reduction method and a series of Cu_x/OL catalysts were prepared by the ion exchange method with various Cu loadings. The materials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), N₂ adsorption-desorption, hydrogen temperature-programmed reduction (H₂-TPR), X-ray photoelectron spectroscopy (XPS), thermogravimetric (TG) and.oxygen temperature-programmed desorption (O₂-TPD) techniques, and their catalytic activities for CO and ethyl acetate oxidation were evaluated. The results show that OL is a typical octahedral layered structure, and the doping of Cu hardly affects the structure of OL. Moreover, Cu_x/OL samples had different reducibility, oxygen mobility, and atomic ratio of Cu²⁺/CuO, (Mn²⁺+Mn³⁺)/Mn⁴⁺, and O_ads/O_latt after the addition of Cu to OL. Among the Cu_x/OL samples, the Cu₅/OL sample showed the best activity for the catalytic oxidation of CO and ethyl acetate (T₅₀=70 and T₉₀=100℃ for CO oxidation; T₅₀=160℃ and T₉₀=200℃ for ethyl acetate oxidation). Cu₅/OL showed the best reducibility, most isolated Cu²⁺ species, highest surface (Mn²⁺+Mn³⁺)/Mn⁴⁺ atomic ratio, highest chemisorbed oxygen species, and lowest O₂ desorption temperature. Hence, factors such as the strong interaction between copper and manganese, good reducibility, and oxygen mobility were responsible for the excellent catalytic activity of Cu₅/OL.

Key words: Octahedral layered birnessite, Cu_x/OL, Carbon monoxide, Ethyl acetate, Catalytic oxidation

傅之丹,臧佳欣,叶青,程水源,康天放. OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能[J]. 物理化学学报, 2017, 33(9), 1855-1864. doi: 10.3866/PKU.WHXB201704282

Zhi-Dan FU,Jia-Xin ZANG,Qing YE,Shui-Yuan CHENG,Tian-Fang KANG. Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate[J]. Acta Phys. -Chim. Sin. 2017, 33(9), 1855-1864. doi: 10.3866/PKU.WHXB201704282

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201704282

https://www.whxb.pku.edu.cn/CN/Y2017/V33/I9/1855

参考文献

1	Wang Y. Z. ; Zhao Y. X. ; Liu S. S. Chin. J. Process. Eng. 2003, 4 (8), 8.
1	王永钊; 赵永祥; 刘滇生. 环境工程学报, 2003, 4 (8), 8.
2	Zhang X. D. ; Wang Y. ; Yang Y. Q. ; Chen D. Acta Phys. -Chim. Sin. 2015, 31 (9), 1633.
2	张晓东; 王吟; 杨一琼; 陈丹. 物理化学学报, 2015, 31 (9), 1633.
3	Gardner S. D. ; Hoflund G. B. ; Schryer D. R. ; Schryer J. ; Upchurch B. T. ; Kielin E. J. Langmuir 1991, 7 (10), 2135.
4	Chen J. ; Li J. ; Li H. ; Huang X. ; Shen W. Microporous Mesoporous Mater. 2008, 116 (1–3), 586.
5	Duan M. H. ; Li J. J. ; Chu X. ; Wang J. M. Ind. Catal. 2010, 18 (3), 46.
5	段明华; 李进军; 褚霞; 王家明. 工业催化, 2010, 18 (3), 46.
6	Li W. B. ; Gong H. Acta Phys. -Chim. Sin. 2010, 26 (4), 885.
6	黎维彬; 龚浩. 物理化学学报, 2010, 26 (4), 885.
7	Gandhe A. R. ; Rebello J. S. ; Figueiredo J. L. ; Fernandes J. B. Appl. Catal. B 2007, 72 (1–2), 129.
8	Zhou H. ; Wang J. Y. ; Chen X. ; O'Young C. L. ; Suib S. L. Microporous Mesoporous Mater. 1998, 21, 315.
9	Deng Y. Q. ; Zhang T. ; Au C. T. ; Yin S. F. Appl. Catal. A 2013, 467, 117.
10	Deguzman N.R. ; Shen Y. F. ; Neth E. J. ; Suib S. L. ; Levine S. ; Newsam J. M. Chem. Mater. 1994, 6 (6), 815.
11	Luo J. ; Zhang Q. H. ; Huang A. M. ; Suib S. L. Microporous Mesoporous Mater. 2000, 35 (6), 209.
12	Ge J. ; Zhuo L. ; Yang F. ; Tang B. ; Wu L. ; Tung C. J. Phys. Chem. B 2006, 110 (36), 17854.
13	Carno J. ; Ferrandon M. ; Bjornbom E. ; Jaras S. Appl. Catal. A 1997, 155 (2), 265.
14	Post J. E. ; Veblen D. R. Am. Mineral. 1990, 75, 477.
15	Hu H. M. ; Deng C. H. ; Sun F. X. ; Zhang K. H. ; Sun M. ; Xuan H. Chin. Inorg. Chem. 2012, 28 (2), 405.
15	胡寒梅; 邓崇海; 孙凤霞; 张克华; 孙梅; 宣寒. 无机化学学报, 2012, 28 (2), 405.
16	Kapteijn F. ; Singoredjo L. ; Andreini A. ; Moulijn J. A. Appl. Catal. B 1994, 3 (2-3), 173.
17	Ma Z. Y. ; Yang C. ; Wei W. ; Li W. H. ; Sun Y. H. J. Mol. Catal. A 2005, 231 (1–2), 75.
18	Tsuji, Y.; Imamura, S. New Aspects of Spillover Effect in Catalysis; Elsevier Press: Amsterdam, The Netherlands, 1993.
19	Xu R. ; Wang X. ; Wang D. S. ; Zhou K. B. ; Li Y. D. J. Catal. 2006, 237 (2), 426.
20	Ferrandon M. ; Carno J. ; Jaras S. D. Appl. Catal. A 1999, 180 (1–2), 141.
21	Muilenbergy, G. E. Handbook of X-ray Photoelectron Spectroscopy; Perkin Elmer Corporation: MA, USA, 1979.
22	Wang J. ; Liu Z. ; Feng G. ; Chang L. ; Bao W. Fuel 2013, 109, 101.
23	Haneda M. ; Kintaichi Y. ; Bion N. ; Hamada H. Appl. Catal. B 2003, 46, 473.
24	Dong Y. ; Niu X. ; Zhu Y. ; Yuan F. ; Fu H. Catal. Lett. 2011, 141 (2), 242.
25	Xia Y. ; Dai H. ; Jiang H. ; Zhang L. Catal. Commun. 2010, 11 (15), 1171.
26	Gaillot A. C. ; Lanson B. ; Drits V. A. Chem. Mater. 2005, 17 (11), 2959.
27	Ma R. ; Bando Y. ; Zhang ; L. Sasaki T. Adv. Mater. 2004, 16, 918.
28	Yin Y. G. ; Xu W. Q. ; Suib S. L. ; Oyoung C. L. Inorg. Chem. 1995, 34 (16), 4187.
29	Jiratova K. ; Mikulova J. ; Klempa J. ; Grygar T. ; Bastl Z. ; Kovanda F. Appl. Catal. A 2009, 361 (1–2), 106.
30	Ye Q. ; Zhao J. S. ; Huo F. F. Microporous Mesoporous Mater. 2013, 172, 20.
31	Carabineiro S. A. C. ; Bastos S. S. T. ; Orfao J. J. M. ; Pereira M. F. R. ; Delgado J. J. ; Figueiredo J. L. Catal. Lett. 2010, 134 (3–4), 217.
32	Wang L. C. ; Liu Q. ; Huang X. S. ; Liu Y. M. ; Cao Y. ; Fan K. N. Appl. Catal. B 2009, 88 (1–2), 204.
33	Huang Q. ; Yan X. ; Li B. ; Xu X. ; Cheng Y. ; Zhu S. ; Shen S. J Ind. Eng. Chem 2013, 19 (2), 438.
34	Larsson P, O ; Andersson A. Appl. Catal. B 2000, 24 (3–4), 175.
35	Sun H. ; Liu Z. ; Chen S. ; Quan X. Chem. Eng. J. 2015, 270, 58.
36	Liu X. S. ; Jin Z. N. ; Lu J. Q. ; Wang X. X. ; Luo M. F. Chem. Eng. J. 2010, 162 (1), 151.

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OL负载Cu催化剂及其催化氧化CO及乙酸乙酯性能

Cu-Doped Octahedral Layered Birnessites Catalysts for the Catalytic Oxidation of CO and Ethyl Acetate

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