氨浓度对氨蒸发法制备Pd-Cu/凹凸棒土催化剂常温CO氧化性能的影响

引用本文: 王永钊, 范莉渊, 武瑞芳, 石晶, 李潇, 赵永祥. 氨浓度对氨蒸发法制备Pd-Cu/凹凸棒土催化剂常温CO氧化性能的影响[J]. 燃料化学学报, 2015, 43(9): 1076-1082. shu

Citation: WANG Yong-zhao, FAN Li-yuan, WU Rui-fang, SHI Jing, LI Xiao, ZHAO Yong-xiang. Effect of ammonia concentration on the catalytic activity of Pd-Cu supported on attapulgite clay prepared by ammonia evaporation in CO oxidation at room temperature[J]. Journal of Fuel Chemistry and Technology, 2015, 43(9): 1076-1082. shu

氨浓度对氨蒸发法制备Pd-Cu/凹凸棒土催化剂常温CO氧化性能的影响

通讯作者: 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。; 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。

基金项目:
国家自然科学基金(21073114) (21073114)

国际合作项目(2013DFA40460) (2013DFA40460)

山西省科技创新重点团队项目(2012021007)。 (2012021007)

摘要: 以凹凸棒土(APT)作载体,采用氨蒸发法制备了Pd-Cu/APT催化剂,以CO氧化为探针反应,在连续流动微反应装置上,考察了初始氨浓度对催化剂CO常温催化氧化性能的影响。通过N₂-physisorption、XRD、FT-IR、TEM和H₂-TPR等手段对催化剂的结构和性质进行了表征。结果表明,在较低或过高氨浓度条件下,制备的Pd-Cu/APT中Cu物种均主要以CuO为主,仅有少量Cu₂(OH)₃Cl;适宜的氨浓度有利于稳定Cu₂(OH)₃Cl物相的形成,其薄片状的形貌特征、良好的分散状态以及与Pd物种间较强的相互作用,显著提高了CO催化氧化性能。在空速6 000 h^-1、CO体积分数1.5%、水蒸气体积分数3.3%的反应条件下,Pd-Cu/APT催化剂表现出优异的CO室温催化氧化活性和稳定性。

关键词:

English

Effect of ammonia concentration on the catalytic activity of Pd-Cu supported on attapulgite clay prepared by ammonia evaporation in CO oxidation at room temperature

1.
School of Chemistry and Chemical Engineering, Engineering Research Center for Fine Chemicals of Ministry of Education, Shanxi University, Taiyuan 030006, China

Corresponding author: 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。; 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。

Received Date: 15 February 2015
Fund Project:
国家自然科学基金(21073114)

国际合作项目(2013DFA40460)

山西省科技创新重点团队项目(2012021007)。

Abstract: With attapulgite clay (APT) as support, the Pd-Cu/APT catalysts were prepared by an ammonia evaporation method and characterized by N₂-physisorption, XRD, FT-IR, TEM and H₂-TPR. The effect of ammonia concentration on the catalytic performance of Pd-Cu/APT in CO oxidation at room temperature was investigated in a fixed-bed continuous flow microreactor. The results showed that CuO appears as the main Cu species in the Pd-Cu/APT catalysts prepared with over low or over high ammonia concentration, whereas the quantity of Cu₂(OH)₃Cl phase is much less. However, a proper concentration of ammonia is of benefits to forming stable Cu₂(OH)₃Cl species in Pd-Cu/APT; owing to its high dispersion, nano-platelet morphology and strong interaction with Pd species, the presence of stable Cu₂(OH)₃Cl can significantly promote the catalytic performance of Pd-Cu/APT in CO oxidation. Under a gas hourly space velocity (GHSV) of 6 000 h^-1 for a feed stream containing 1.5% CO and 3.3% water, the Pd-Cu/APT catalyst exhibits excellent activity and stability in CO oxidation even at room temperature.

Key words:

1. [1] 徐慧远, 罗靖洁, 严春蓉, 张燕, 尚书勇. 二氧化硅孔结构对CO氧化用担载型纳米金催化剂的影响[J]. 燃料化学学报, 2012, 40(11): 1397-1402. (XU Hui-yuan, LUO Jing-jie, YAN Chun-rong, ZHANG Yan, SHANG Shu-yong. Impact of silica porosity on the catalytic activity of nanosize gold catalyst for CO oxidation[J]. J Fuel Chem Technol, 2012, 40(11): 1397-1402.)[1] 徐慧远, 罗靖洁, 严春蓉, 张燕, 尚书勇. 二氧化硅孔结构对CO氧化用担载型纳米金催化剂的影响[J]. 燃料化学学报, 2012, 40(11): 1397-1402. (XU Hui-yuan, LUO Jing-jie, YAN Chun-rong, ZHANG Yan, SHANG Shu-yong. Impact of silica porosity on the catalytic activity of nanosize gold catalyst for CO oxidation[J]. J Fuel Chem Technol, 2012, 40(11): 1397-1402.)
2. [2] ZHU H Q, QIN Z F, SHAN W J, SHEN W J, WANG J G. Low-temperature oxidation of CO over Pd/CeO₂-TiO₂ catalysts with different pretreatments[J]. J Catal, 2005, 233(1): 41-50.[2] ZHU H Q, QIN Z F, SHAN W J, SHEN W J, WANG J G. Low-temperature oxidation of CO over Pd/CeO₂-TiO₂ catalysts with different pretreatments[J]. J Catal, 2005, 233(1): 41-50.
3. [3] QI C X, SU H J, GUAN R G, XU X F. An investigation into phosphate-doped Au/alumina for low temperature CO oxidation[J]. J Phys Chem, 2012, 116(33): 17492-17500.[3] QI C X, SU H J, GUAN R G, XU X F. An investigation into phosphate-doped Au/alumina for low temperature CO oxidation[J]. J Phys Chem, 2012, 116(33): 17492-17500.
4. [4] LI L, WANG A Q, QIAO B T, LIN J, HUANG Y Q, WANG X D, ZHANG T. Origin of the high activity of Au/FeO_x for low-temperature CO oxidation: Direct evidence for a redox mechanism[J]. J Catal, 2013, 299: 90-100.[4] LI L, WANG A Q, QIAO B T, LIN J, HUANG Y Q, WANG X D, ZHANG T. Origin of the high activity of Au/FeO_x for low-temperature CO oxidation: Direct evidence for a redox mechanism[J]. J Catal, 2013, 299: 90-100.
5. [5] ATSUSHI S, KAORU O, MASATOSHI Y, JUNYA O, KENICHI S. Activity controlling factors for low-temperature oxidation of CO over supported Pd catalysts[J]. Appl Catal B: Environ, 2013, 132-133: 511-518.[5] ATSUSHI S, KAORU O, MASATOSHI Y, JUNYA O, KENICHI S. Activity controlling factors for low-temperature oxidation of CO over supported Pd catalysts[J]. Appl Catal B: Environ, 2013, 132-133: 511-518.
6. [6] XIE X W, LI Y, LIU Z Q, HARUTA M, SHEN W J. Low-temperature oxidation of CO catalysed by Co₃O₄ nanorods[J]. Nature, 2009, 458: 746-749.[6] XIE X W, LI Y, LIU Z Q, HARUTA M, SHEN W J. Low-temperature oxidation of CO catalysed by Co₃O₄ nanorods[J]. Nature, 2009, 458: 746-749.
7. [7] CHRISTOPHER J, STUART H T, ANDREW B, MANDY J C, CHRISTOPHER J K, GRAHAM J H. Cobalt promoted copper manganese oxide catalysts for ambient temperature carbon monoxide oxidation[J]. Chem Commun, 2008, 14: 1707-1709.[7] CHRISTOPHER J, STUART H T, ANDREW B, MANDY J C, CHRISTOPHER J K, GRAHAM J H. Cobalt promoted copper manganese oxide catalysts for ambient temperature carbon monoxide oxidation[J]. Chem Commun, 2008, 14: 1707-1709.
8. [8] WANG Y Z, ZHAO Y X, GAO C G, LIU D S. Origin of the high activity and stability of Co₃O₄ in low-temperature CO oxidation[J]. Catal Lett, 2008, 125(1/2): 134-138.[8] WANG Y Z, ZHAO Y X, GAO C G, LIU D S. Origin of the high activity and stability of Co₃O₄ in low-temperature CO oxidation[J]. Catal Lett, 2008, 125(1/2): 134-138.
9. [9] LUO M F, MA J M, LU J Q, SONG Y P, WANG Y J. High-surface area CuO-CeO₂ catalysts prepared by a surfactant-templated method for low-temperature CO oxidation[J]. J Catal, 2007, 246(1): 52-59.[9] LUO M F, MA J M, LU J Q, SONG Y P, WANG Y J. High-surface area CuO-CeO₂ catalysts prepared by a surfactant-templated method for low-temperature CO oxidation[J]. J Catal, 2007, 246(1): 52-59.
10. [10] 邵建军, 朱锡, 张永坤, 王明贵. Co₃O₄/CeO₂ CO氧化的原位红外光谱研究[J]. 燃料化学学报, 2012, 40(2): 229-234. (SHAO Jian-jun, ZHU Xi, ZHANG Yong-kun, WANG Ming-gui. In situ FT-IR study on CO oxidation over Co₃O₄/CeO₂ catalyst[J]. J Fuel Chem Technol, 2012, 40(2): 229-234.)[10] 邵建军, 朱锡, 张永坤, 王明贵. Co₃O₄/CeO₂ CO氧化的原位红外光谱研究[J]. 燃料化学学报, 2012, 40(2): 229-234. (SHAO Jian-jun, ZHU Xi, ZHANG Yong-kun, WANG Ming-gui. In situ FT-IR study on CO oxidation over Co₃O₄/CeO₂ catalyst[J]. J Fuel Chem Technol, 2012, 40(2): 229-234.)
11. [11] PARK E D, LEE J S. Effect of surface treatment of the support on CO oxidation over carbon-supported wacker-type catalysts[J]. J Catal, 2000, 193: 5-15.[11] PARK E D, LEE J S. Effect of surface treatment of the support on CO oxidation over carbon-supported wacker-type catalysts[J]. J Catal, 2000, 193: 5-15.
12. [12] WANG F G, ZHANG H J, HE D N. Catalytic oxidation of low-concentration CO at ambient temperature over supported Pd-Cu catalysts[J]. Environ Technol, 2014, 35(3): 347-354.[12] WANG F G, ZHANG H J, HE D N. Catalytic oxidation of low-concentration CO at ambient temperature over supported Pd-Cu catalysts[J]. Environ Technol, 2014, 35(3): 347-354.
13. [13] SHEN Y X, LU G Z, GUO Y, WANG Y Q. A synthesis of high-efficiency Pd-Cu-Cl_x/Al₂O₃ catalyst for low temperature CO oxidation[J]. Chem Commun, 2010, 46: 8433-8435.[13] SHEN Y X, LU G Z, GUO Y, WANG Y Q. A synthesis of high-efficiency Pd-Cu-Cl_x/Al₂O₃ catalyst for low temperature CO oxidation[J]. Chem Commun, 2010, 46: 8433-8435.
14. [14] SHEN Y X, LU G Z, GUO Y, WANG Y Q, GUO Y L, GONG X Q. Study on the catalytic reaction mechanism of low temperature oxidation of CO over Pd-Cu-Cl_x/Al₂O₃ catalyst[J]. Catal Today, 2011, 175: 558-567.[14] SHEN Y X, LU G Z, GUO Y, WANG Y Q, GUO Y L, GONG X Q. Study on the catalytic reaction mechanism of low temperature oxidation of CO over Pd-Cu-Cl_x/Al₂O₃ catalyst[J]. Catal Today, 2011, 175: 558-567.
15. [15] JAE S L, EUN D P, BYUNG J S. Process development for low temperature CO oxidation in the presence of water and halogen compounds[J]. Catal Today, 1999, 54: 57-64.[15] JAE S L, EUN D P, BYUNG J S. Process development for low temperature CO oxidation in the presence of water and halogen compounds[J]. Catal Today, 1999, 54: 57-64.
16. [16] CHUL W L, SEOK J P, YOUNG S K, PAUL J C. Catalytic oxidation of carbon monoxide at low temperature over Pd-Cu loaded porous supports[J]. B Kor Chem Soc, 1995, 16(3): 296-298.[16] CHUL W L, SEOK J P, YOUNG S K, PAUL J C. Catalytic oxidation of carbon monoxide at low temperature over Pd-Cu loaded porous supports[J]. B Kor Chem Soc, 1995, 16(3): 296-298.
17. [17] 王永钊, 程慧敏, 范莉渊, 石晶, 赵永祥. 焙烧温度对Pd-Cu/凹凸棒土CO常温催化氧化性能的影响[J]. 燃料化学学报, 2014, 42(5): 597-602. (WANG Yong-zhao, CHEN Hui-min, FAN LI-yuan, SHI Jing, ZHAO Yong-xiang. Effect of calcination temperature on catalytic performance of Pd-Cu/attapulgite clay catalyst for CO oxidation at room temperature[J]. J Fuel Chem Technol, 2014, 42(5): 597-602.)[17] 王永钊, 程慧敏, 范莉渊, 石晶, 赵永祥. 焙烧温度对Pd-Cu/凹凸棒土CO常温催化氧化性能的影响[J]. 燃料化学学报, 2014, 42(5): 597-602. (WANG Yong-zhao, CHEN Hui-min, FAN LI-yuan, SHI Jing, ZHAO Yong-xiang. Effect of calcination temperature on catalytic performance of Pd-Cu/attapulgite clay catalyst for CO oxidation at room temperature[J]. J Fuel Chem Technol, 2014, 42(5): 597-602.)
18. [18] 王永钊, 张卓, 李凤梅, 赵永祥. Pd-Cu/凹凸棒石黏土催化剂催化CO氧化性能[J]. 工业催化, 2011, 11(19): 75-79. (WANG Yong-zhao, ZHANG Zhuo, LI Feng-mei, ZHAO Yong-xiang. Catalytic performance of Pd-Cu/attapulgite clay catalyst for CO oxidation[J]. Ind Catal, 2011, 11(19): 75-79.)[18] 王永钊, 张卓, 李凤梅, 赵永祥. Pd-Cu/凹凸棒石黏土催化剂催化CO氧化性能[J]. 工业催化, 2011, 11(19): 75-79. (WANG Yong-zhao, ZHANG Zhuo, LI Feng-mei, ZHAO Yong-xiang. Catalytic performance of Pd-Cu/attapulgite clay catalyst for CO oxidation[J]. Ind Catal, 2011, 11(19): 75-79.)
19. [19] DYAKONOV A J. Abatement of CO from relatively simple and complex mixtures - II. Oxidation on Pd-Cu/C catalysts[J]. Appl Catal B: Environ, 2003, 45(4): 257-267.[19] DYAKONOV A J. Abatement of CO from relatively simple and complex mixtures - II. Oxidation on Pd-Cu/C catalysts[J]. Appl Catal B: Environ, 2003, 45(4): 257-267.
20. [20] PARK E D, LEE J S. Effects of copper phase on CO oxidation over supported Wacker-type catalysts[J]. J Catal, 1998, 180(2): 123-131.[20] PARK E D, LEE J S. Effects of copper phase on CO oxidation over supported Wacker-type catalysts[J]. J Catal, 1998, 180(2): 123-131.
21. [21] YOU J, CHEN F, ZHAO X B, CHEN Z G. Preparation, characterization and catalytic oxidation property of CeO₂/Cu²⁺-attapulgite (ATP) nanocomposites[J]. J Rare Earth, 2010, 28(9): 347-352.[21] YOU J, CHEN F, ZHAO X B, CHEN Z G. Preparation, characterization and catalytic oxidation property of CeO₂/Cu²⁺-attapulgite (ATP) nanocomposites[J]. J Rare Earth, 2010, 28(9): 347-352.
22. [22] CAO J L, SHAO G S, WANG Y, LIU Y P, YUAN Z Y. CuO catalysts supported on attapulgite clay for low-temperature CO oxidation[J]. Catal Commun, 2008, 9: 2555-2559.[22] CAO J L, SHAO G S, WANG Y, LIU Y P, YUAN Z Y. CuO catalysts supported on attapulgite clay for low-temperature CO oxidation[J]. Catal Commun, 2008, 9: 2555-2559.
23. [23] YANG H M, TANG A D, OUYANG J, LI M, MANN S. From natural attapulgite to mesoporous materials: methodology, characterization and structural evolution[J]. J Phys Chem B, 2010, 114: 2390-2398.[23] YANG H M, TANG A D, OUYANG J, LI M, MANN S. From natural attapulgite to mesoporous materials: methodology, characterization and structural evolution[J]. J Phys Chem B, 2010, 114: 2390-2398.
24. [24] WEI W, GAO P, XIE J M, ZONG S K, CUI H L, YUE X J. Uniform Cu₂Cl(OH)₃ hierarchical microspheres: A novel adsorbent for methylene blue adsorptive removal from aqueous solution[J]. J Solid State Chem, 2013, 204: 305-313.[24] WEI W, GAO P, XIE J M, ZONG S K, CUI H L, YUE X J. Uniform Cu₂Cl(OH)₃ hierarchical microspheres: A novel adsorbent for methylene blue adsorptive removal from aqueous solution[J]. J Solid State Chem, 2013, 204: 305-313.

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 653
HTML全文浏览量: 39

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

氨浓度对氨蒸发法制备Pd-Cu/凹凸棒土催化剂常温CO氧化性能的影响

通讯作者: 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。; 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。

English

Effect of ammonia concentration on the catalytic activity of Pd-Cu supported on attapulgite clay prepared by ammonia evaporation in CO oxidation at room temperature

Corresponding author: 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。; 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。

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

氨浓度对氨蒸发法制备Pd-Cu/凹凸棒土催化剂常温CO氧化性能的影响

通讯作者: 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。; 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。

English

Effect of ammonia concentration on the catalytic activity of Pd-Cu supported on attapulgite clay prepared by ammonia evaporation in CO oxidation at room temperature

Corresponding author: 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。; 王永钊,Fax:+86-351-7011688,E-mail:catalyst@sxu.edu.cn;赵永祥,E-mail:yxzhao@sxu.edu.cn。

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