浸渍顺序对CuCe/AC催化剂结构和性能的影响

引用本文: 郑华艳, 郭天玉, 李忠, 孟凡会, 秦瑶. 浸渍顺序对CuCe/AC催化剂结构和性能的影响[J]. 无机化学学报, 2013, 29(12): 2575-2581. doi: 10.3969/j.issn.1001-4861.2013.00.388 shu

Citation: ZHENG Hua-Yan, GUO Tian-Yu, LI Zhong, MENG Fan-Hui, QIN Yao. Effect of Impregnation Strategy on Structure and Catalytic Performance of CuCe/AC Catalyst[J]. Chinese Journal of Inorganic Chemistry, 2013, 29(12): 2575-2581. doi: 10.3969/j.issn.1001-4861.2013.00.388 shu

浸渍顺序对CuCe/AC催化剂结构和性能的影响

基金项目:
国家自然科学基金(No.20976113，21276169) (No.20976113，21276169)

山西省科技攻关项目(20120321003-03) (20120321003-03)

山西省归国留学基金(No.20100038)资助项目。 (No.20100038)

摘要: 通过在Cu/AC催化剂中添加稀土助剂Ce，考察不同的浸渍顺序对CuCe/AC(活性炭)催化剂表面结构及其催化甲醇气相氧化羰基化合成碳酸二甲酯性能的影响，并采用XRD、XPS、H₂-TPR、AAS和HR-TEM等表征了催化剂活性组分含量、分散状态和价态等性质。发现共浸渍法制备的催化剂，Ce对活性组分Cu在活性炭表面的分散起到一定的促进作用；先浸渍Cu后浸渍Ce制备的催化剂，后浸渍的Ce覆盖部分Cu组分，使这些Cu组分难以还原并无法与反应物分子接触，导致其催化性能有所降低；而先浸渍Ce后浸渍Cu制备的催化剂，Ce组分和Cu组分产生相互作用，使表面存在较多分散均匀的Cu(0)和Cu(Ⅰ)物种，其催化性能最佳，碳酸二甲酯的时空收率及选择性分别达到了142 mg·g^-1·h^-1和85%。

关键词:

助剂Ce;浸渍顺序;Cu/AC催化剂;氧化羰基化

English

Effect of Impregnation Strategy on Structure and Catalytic Performance of CuCe/AC Catalyst

1.
Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
Received Date: 18 March 2013
Fund Project:
国家自然科学基金(No.20976113，21276169)

山西省科技攻关项目(20120321003-03)

山西省归国留学基金(No.20100038)资助项目。

Abstract: The effect of impregnation sequence on the surface structure and catalytic performance of CuCe/AC (Activated carbon) (by adding rare earth Ce promoter to Cu/AC) catalyst was studied for gas-phase oxidative carbonylation of methanol to dimethyl carbonate. The active component content, surface dispersion and valence state of as-prepared catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H₂-temperature programmed reduction(H₂-TPR), High resolution transmission electron microscope (HR-TEM). The results show that Ce promoter plays a key role for active component Cu to disperse on the surface of activated carbon in CuCe/AC catalyst prepared by co-impregnation. The Cu components are difficult to be reduced and difficult to contact with reactant molecules for CuCe/AC catalyst prepared by first impregnation with Cu and then with Ce because part of Cu components are covered by Ce impregnation leading to the decrease of catalytic activity. For CuCe/AC catalyst prepared by first impregnation with Ce and then with Cu, the Ce and Cu components interact with each other, resulting in an optimal catalytic performance because of a more uniform dispersion of Cu (0) and Cu(Ⅰ) species on the surface of the catalyst. The space time yield and selectivity of dimethyl carbonate are 142 mg·g^-1·h^-1 and 85%, respectively.

Key words:

Ce promoter;impregnation sequence;Cu/AC catalyst;oxidative carbonylation

1. [1] Keller N, Rebmann G, Keller V. J. Mol. Catal. A Chem., 2010, 317 (1/2):1-18[1] Keller N, Rebmann G, Keller V. J. Mol. Catal. A Chem., 2010, 317 (1/2):1-18
2. [2] Jiang R, Wang Y, Zhao X, et al. J. Mol. Catal. A Chem., 2002, 185 (1/2):/159-166[2] Jiang R, Wang Y, Zhao X, et al. J. Mol. Catal. A Chem., 2002, 185 (1/2):/159-166
3. [3] King S T. Catal. Today, 1997, 33 (1/2/3):173-182[3] King S T. Catal. Today, 1997, 33 (1/2/3):173-182
4. [4] Richter M, Fait M J G, Eckelt R, et al. J. Catal., 2007, 245 (1):11-24[4] Richter M, Fait M J G, Eckelt R, et al. J. Catal., 2007, 245 (1):11-24
5. [5] Wang Y J, Jiang R X, Zhao X Q, et al. J. Nat. Gas Chem., 2000, 9 (3):205-211[5] Wang Y J, Jiang R X, Zhao X Q, et al. J. Nat. Gas Chem., 2000, 9 (3):205-211
6. [6] LI Zhong (李忠), ZHU Qiong-Fang (朱琼芳), WANG Rui-Yu (王瑞玉), et al. Chinese J. Inorg. Chem. (Wuji Huaxue Xuebao), 2011, 27 (4):718-724[6] LI Zhong (李忠), ZHU Qiong-Fang (朱琼芳), WANG Rui-Yu (王瑞玉), et al. Chinese J. Inorg. Chem. (Wuji Huaxue Xuebao), 2011, 27 (4):718-724
7. [7] LI Zhong (李忠), NIU Yan-Yan (牛燕燕), ZHENG Hua-Yan (郑华艳), et al. Chinese J. Inorg. Chem. (Wuji Huaxue Xuebao), 2011, 27 (7):1277-1284[7] LI Zhong (李忠), NIU Yan-Yan (牛燕燕), ZHENG Hua-Yan (郑华艳), et al. Chinese J. Inorg. Chem. (Wuji Huaxue Xuebao), 2011, 27 (7):1277-1284
8. [8] LI Zhong (李忠), WEN Chun-Mei (文春梅), ZHENG Hua-Yan (郑华艳), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 2010, 31 (1):145-152[8] LI Zhong (李忠), WEN Chun-Mei (文春梅), ZHENG Hua-Yan (郑华艳), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 2010, 31 (1):145-152
9. [9] LI Zhong (李忠), WEN Chun-Mei (文春梅), WANG Rui-Yu (王瑞玉), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 2009, 30 (10):2024-2031[9] LI Zhong (李忠), WEN Chun-Mei (文春梅), WANG Rui-Yu (王瑞玉), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 2009, 30 (10):2024-2031
10. [10] Zou H, Dong X, Lin W. Appl. Surf. Sci., 2006, 253 (5):2893-2898[10] Zou H, Dong X, Lin W. Appl. Surf. Sci., 2006, 253 (5):2893-2898
11. [11] Qi L, Yu Q, Dai Y, et al. Appl. Catal. B: Environ., 2012, 119-120:308-320[11] Qi L, Yu Q, Dai Y, et al. Appl. Catal. B: Environ., 2012, 119-120:308-320
12. [12] Liu Z G, Zhou R X, Zheng X M. J. Nat. Gas Chem., 2008, 17 (2):125-129[12] Liu Z G, Zhou R X, Zheng X M. J. Nat. Gas Chem., 2008, 17 (2):125-129
13. [13] Jiang X Y, Lou L P, Chen Y X, et al. J. Mol. Catal. A Chem., 2003, 197 (1/2):193-205[13] Jiang X Y, Lou L P, Chen Y X, et al. J. Mol. Catal. A Chem., 2003, 197 (1/2):193-205
14. [14] LI Zhong (李忠), ZHENG Hua-Yan (郑华艳), XIE Ke-Chang (谢克昌). Chin. J. Catal. (Cuihua Xuebao), 2008, 29 (5): 431-435[14] LI Zhong (李忠), ZHENG Hua-Yan (郑华艳), XIE Ke-Chang (谢克昌). Chin. J. Catal. (Cuihua Xuebao), 2008, 29 (5): 431-435
15. [15] Shishido T, Yamamoto M, Li D, et al. Appl. Catal. A: Gen., 2006, 303 (1):62-71[15] Shishido T, Yamamoto M, Li D, et al. Appl. Catal. A: Gen., 2006, 303 (1):62-71
16. [16] Beck D D, Capehart T W, Hoffman R W. Chem. Phys. Lett., 1989, 159 (2/3):205-213[16] Beck D D, Capehart T W, Hoffman R W. Chem. Phys. Lett., 1989, 159 (2/3):205-213
17. [17] Luo M F, Fang P, He M, et al. J. Mol. Catal. A: Chem., 2005, 239 (1/2):243-248[17] Luo M F, Fang P, He M, et al. J. Mol. Catal. A: Chem., 2005, 239 (1/2):243-248
18. [18] Jung C R, Kundu A, Nam S W, et al. Appl. Catal. B: Environ., 2008, 84 (3/4):426-432[18] Jung C R, Kundu A, Nam S W, et al. Appl. Catal. B: Environ., 2008, 84 (3/4):426-432
19. [19] XIE You-Chang (谢有畅), ZHANG Jia-Ping (张佳平), ZHANG Xian-Zhong (童显忠), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 1997, 18 (7): 1159-1165[19] XIE You-Chang (谢有畅), ZHANG Jia-Ping (张佳平), ZHANG Xian-Zhong (童显忠), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 1997, 18 (7): 1159-1165
20. [20] Idem R O, Bakhshi N N. Chem. Eng. Sci., 1996, 51 (14): 3697-3708[20] Idem R O, Bakhshi N N. Chem. Eng. Sci., 1996, 51 (14): 3697-3708
21. [21] ZHANG Ri-Guang (章日光), ZHENG Hua-Yan (郑华艳), WANG Bao-Jun (王宝俊), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 2010, 31 (6):1246-1251[21] ZHANG Ri-Guang (章日光), ZHENG Hua-Yan (郑华艳), WANG Bao-Jun (王宝俊), et al. Chem. J. Chinese Universities (Gaodeng Xuexiao Huaxue Xuebao), 2010, 31 (6):1246-1251

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 790
HTML全文浏览量: 146

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

浸渍顺序对CuCe/AC催化剂结构和性能的影响

English

Effect of Impregnation Strategy on Structure and Catalytic Performance of CuCe/AC Catalyst

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

浸渍顺序对CuCe/AC催化剂结构和性能的影响

English

Effect of Impregnation Strategy on Structure and Catalytic Performance of CuCe/AC Catalyst

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs