Synthesis of Bimetallic MOF-74-CoMn Catalyst and Its Application in Selective Catalytic Reduction of NO with CO

doi:10.6023/A19040129

Acta Chim. Sinica ›› 2019, Vol. 77 ›› Issue (8): 758-764.DOI: 10.6023/A19040129 Previous Articles

Special Issue: 多孔材料：金属有机框架(MOF)

Article

双金属MOF-74-CoMn催化剂的制备及其CO选择性催化还原技术应用

武卓敏^a, 石勇^a, 李春艳^b, 牛丹阳^a, 楚奇^a, 熊巍^a, 李新勇^a

a 大连理工大学环境学院工业生态与环境工程教育部重点实验室和精细化工国家重点实验室大连 116024;
b 大连理工大学材料学院大连 116024

投稿日期:2019-04-11 发布日期:2019-07-08
通讯作者: 石勇 E-mail:sys-99@163.com
基金资助:
国家自然科学基金面上资助项目（No.21677022）.

Synthesis of Bimetallic MOF-74-CoMn Catalyst and Its Application in Selective Catalytic Reduction of NO with CO

Wu Zhuomin^a, Shi Yong^a, Li Chunyan^b, Niu Danyang^a, Chu Qi^a, Xiong Wei^a, Li Xinyong^a

a Key Laboratory of Industrial Ecology and Environmental Engineering and State Key Laboratory of Fine Chemicals, School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China;
b School of Materials, Dalian University of Technology, Dalian 116024, China

Received:2019-04-11 Published:2019-07-08
Contact: 10.6023/A19040129 E-mail:sys-99@163.com
Supported by:
Project supported by the National Natural Science Foundation of China (No. 21677022).

A series of bimetallic MOF-74-CoMn catalysts with different metal ratios have been successfully synthesized by hydrothermal method and applied in selective catalytic reduction of NO with CO (CO-SCR). The experimental procedure for the preparation of MOF-74-CoMn catalyst is as follows:The reaction solution was a 3.28 mmol mixture of Co(NO₃)₂·6H₂O and Mn(NO₃)₂·6H₂O, 1.09 mmol 2,5-dihydroxyterephthalic acid (H₄DOBDC) and 90 mL ethanol-DMF-water. The molar ratio of mixture (Co/Mn) was 1:0, 1:1, 1:2, 1:4, 1:6, respectively. The reactant solution was ultrasonically stired for 30 min until homogeneous. Then, the mixture was transferred into a 100 mL Teflon autoclave then kept in an oven at 100℃ for 24 h. Finally, after purified with DMF and methanol, the products were dried in a vacuum oven at 80℃ for 24 h to obtain a purple MOF-74-CoMn catalyst, which were stored in vacuum or an inert atmosphere. The prepared sample is referred to as MOF-74-Co1Mnx, where x represents a molar ratio of Co to Mn is 1:x (x=0, 1, 2, 4, 6). The SCR catalytic activities were carried out in a fixed-bed flow reactor in gas stream. The experimental results show that the NO_x conversion rate of bimetallic MOF-74-CoMn catalyst is generally higher than that of single metal MOF-74-Co catalyst, and their reaction temperature window is wider. Especially, MOF-74-Co1Mn2 exhibited the highest selective catalytic reduction of NO with CO (CO-SCR) performance which is close to 100% with a temperature range from 175 to 275℃. Further, the bimetallic MOFs catalysts were characterized by X-ray powder diffraction (XRD), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), N₂ adsorption/desorption, X-ray photoelectron spectroscopy (XPS), Hydrogen-temperature programed reduction (H₂-TPR) and Infrared spectroscopy (FTIR) techniques. The results showed that the synergistic effect between Co and Mn metals could obviously promote the formation of unsaturated metal sites and oxygen vacancies, thereby promoting their catalytic reduction efficiency of selective catalytic reduction of NO with CO (CO-SCR).

Key words: bimetallic organic framework material, MOF-74-CoMn, selective catalytic reduction, carbon monoxide, nitrogen oxide, hydrothermal method

Cite this article

Wu Zhuomin, Shi Yong, Li Chunyan, Niu Danyang, Chu Qi, Xiong Wei, Li Xinyong. Synthesis of Bimetallic MOF-74-CoMn Catalyst and Its Application in Selective Catalytic Reduction of NO with CO[J]. Acta Chim. Sinica, 2019, 77(8): 758-764.

Export EndNote|Reference Manager|ProCite|BibTeX|RefWorks

share this article

References

[1] Qu, Y.; An, J. L.; He, Y. J.; Zheng, J. J. Environ. Sci. 2016, 44, 13.
[2] Saikawa, E.; Kim, H.; Zhong, M.; Avramov, A.; Zhao, Y.; Janssens-Maenhout, G.; Kurokawa, J.; Klimont, Z.; Wagner, F.; Naik, V.; Horowitz, L. W.; Zhang, Q. Atmos. Chem. Phys. 2017, 17, 6393.
[3] Hamada, H.; Hanedab, M. Appl. Catal. A 2012, 421, 1.
[4] Skalska, K.; Miller, J. S.; Ledakowicz, S. Sci. Total Environ. 2010, 408, 3976.
[5] Liu, T. K.; Qian, J. N.; Yao, Y. Y.; Shi, Z. F.; Han, L. Y.; Liang, C. Y.; Li, B.; Dong, L. H.; Fan, M. G.; Zhang, L. L. J. Mol. Catal. A:Chem. 2017, 430, 43.
[6] Li, S. S; Wang, F. Z. R.; Liu, Y. M.; Cao, Y. Chin. J. Chem. 2017, 35, 591.
[7] Shin, H. U.; Lolla, D.; Nikolov, Z.; Chase, G. G. J. Ind. Eng. Chem. 2016, 33, 91.
[8] Liu, J.; Li, X. Y.; Zhao, Q. D.; Ke, J.; Xiao, H. N.; Lv, X. J.; Liu, S. M.; Tadéc, M.; Wang, S. B. Appl. Catal. B 2017, 200, 297.
[9] Lee, Y. R.; Kim, J.; Ahn, W. S. Korean J. Chem. Eng. 2013, 30, 1667.
[10] Wang, J. H.; Zhao, H. W.; Haller, G.; Li, Y. D. Appl. Catal. B 2017, 202, 346.
[11] Cai, S. X.; Liu, J.; Zha, K. W.; Li, H. R.; Shi, L. Y.; Zhang, D. S. Nanoscale 2017, 9, 5648.
[12] Shi, Y.; Tang, X. L.; Yi, H. L.; Gao, F. Y.; Zhao, S. Z.; Wang, J. G.; Yang, K.; Zhang, R. C. Ind. Eng. Chem. Res. 2019, 58, 3606.
[13] Shen, Q.; Zhang, L. Y.; Sun, N. N.; Wang, H.; Zhong, L. S.; He, C.; Wei, W.; Sun, Y. H. Chem. Eng. J. 2017, 322, 46.
[14] Cheng, X. X.; Bi, X. T. Particuology 2014, 16, 1.
[15] Dai, X. X.; Jiang, W. Y.; Wang, W. L.; Weng, X, L.; Shang, Y.; Xue, Y. H.; Wu, Z. B. Chin. J. Catal. 2018, 39, 728.
[16] Zhang, L.; Shi L. Y.; Huang L.; Zhang, J. P.; Gao, R. H.; Zhang, D. S. ACS Catal. 2014, 4, 1753.
[17] Liu, Z. Z.; Shi, Y.; Li, C. Y.; Zhao, Q. D.; Li, X. Y. Acta Phys.-Chim. Sin. 2015, 31, 9. (刘震震, 石勇, 李春艳, 肇启东, 李新勇, 物理化学学报, 2015, 31, 9.)
[18] Huang, G.; Chen, Y. Z.; Jiang, H. L. Acta Chim. Sinica 2016, 74, 113. (黄刚, 陈玉贞, 江海龙, 化学学报, 2016, 74, 113.)
[19] Xiao, J. D.; Jiang, H. L. Acc. Chem. Res. 2019, 52, 356.
[20] Jiao, L.; Wang, Y.; Jiang, H. L.; Xu, Q. Adv. Mater. 2018, 30, 1703663.
[21] Adhikari, A. K.; Lin, K. S. Chem. Eng. J. 2016, 284, 1348.
[22] Yan, L. T.; Dai, P. C.; Wang, Y.; Gu, X.; Li, L. J.; Cao, L.; Zhao, X. B. ACS Appl. Mater. Interfaces 2017, 9, 11642.
[23] Sun, D. R.; Ye, L.; Sun, F. X.; García, H.; Li, Z. H. Inorg. Chem. 2017, 56, 5203.
[24] Pliekhov, O.; Pliekhova, O.; Lavrencic štangar, U.; Logar, N. Z. Catal. Commun. 2018, 110, 88.
[25] Jiang, H. X.; Niu, Y.; Wang, Q. Y.; Chen, Y. F.; Zhang, M. H. Catal. Commun. 2018, 113, 46.
[26] Chen, S.; Xue, M.; Li, Y. Q.; Pan, Y.; Zhu, L. K.; Qiu, S. L. J. Mater. Chem. 2015, 3, 20145.
[27] Liu, T. K.; Yao, Y. Y.; Wei, L. Q.; Shi, Z. F.; Han, L. Y.; Yuan, H. X.; Li, B.; Dong, L. H.; Wang, F.; Sun, C. Z. J. Phys. Chem. C 2017, 121, 12757.
[28] Kim, S. H.; Lee, Y. J.; Kim, D. H.; Lee, Y. J. ACS Appl. Mater. Interfaces 2018, 10, 660.
[29] Nguyen, H. T. T.; Doan, D. N. A.; Truong, T. J. Mol. Catal. A:Chem. 2017, 426, 141.
[30] Liu, K. J.; Yu, Q. B.; Liu, J. L.; Wang, K.; Han, Z. C.; Xuan, Y. N.; Qin, Q. New J. Chem. 2017, 41, 13993.
[31] Hu, H.; Cai, S. X.; Li, H. R.; Huang, L.; Shi, L. Y.; Zhang, D. S. ACS Catal. 2015, 5, 6069.
[32] Qin, Y. L.; Huang, L.; Zheng, J. X.; Ren, Q. Inorg. Chem. Commun. 2016, 72, 78.
[33] Gao, F. Y.; Tang, X. L.; Yi, H. H.; Li, J. Y.; Zhao, S. Z.; Wang, J. G.; Chu, C.; Li, C. L. Chem. Eng. J. 2017, 317, 20.
[34] Dietzel, P. D. C.; Morita, Y.; Blom, R.; Fjellvag, H. Angew. Chem. Int. Ed. 2005, 44, 6354.
[35] Yan, L. T.; Cao, L.; Dai, P. C.; Gu, X.; Liu, D. D.; Li, L. J.; Wang, Y.; Zhao, X. B. Adv. Funct. Mater. 2017, 27, 1703455.
[36] Jiang, H. X.; Wang, Q. Y.; Wang, H. Q.; Chen, Y. F.; Zhang, M. H. ACS Appl. Mater. Interfaces 2016, 8, 26817.

双金属MOF-74-CoMn催化剂的制备及其CO选择性催化还原技术应用

Synthesis of Bimetallic MOF-74-CoMn Catalyst and Its Application in Selective Catalytic Reduction of NO with CO

PDF

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Pengfei Zhu, Chensi Lou, Yuhan Shi, Chuanyi Wang. Study on Preparation of Ag/AgCl/ZIF-8 Composite and Photocatalytic NO Oxidation Performance [J]. Acta Chimica Sinica, 2022, 80(10): 1385-1393.
[2]	Tong Jiao, Xue-lian Xu, Lei Zhang, You-yun Weng, Yu-bing Weng, Zhi-xian Gao. Research on CuO/CeO₂-ZrO₂/SiC Monolithic Catalysts for Hydrogen Production by Methanol Steam Reforming [J]. Acta Chimica Sinica, 2021, 79(4): 513-519.
[3]	Yong Li, Xu Wang, Xilei Xie, Jian Zhang, Bo Tang. Progress in Organic Fluorescent Probes and Photocontrolled Releasers for Carbon Monoxide [J]. Acta Chimica Sinica, 2021, 79(1): 36-44.
[4]	Zhang Xiaolei, Tian Gan, Zhang Xia, Wang Qing, Gu Zhanjun. Controlled Release of Carbon Monoxide Based on Nanomaterials and Their Biomedical Applications [J]. Acta Chim. Sinica, 2019, 77(5): 406-417.
[5]	Song Congying, Sun Xun, Ye Ke, Zhu Kai, Cheng Kui, Yan Jun, Cao Dianxue, Wang Guiling. Electrocatalytic Activity of MnO₂ Supported on Reduced Graphene Oxide Modified Ni Foam for H₂O₂ Reduction [J]. Acta Chim. Sinica, 2017, 75(10): 1003-1009.
[6]	Tong Zhenkun, Fang Shan, Zheng Hao, Zhang Xiaogang. Zn₂GeO₄ Nanorods@Graphene Composite as Anode Materials for Li-ion Batteries [J]. Acta Chim. Sinica, 2016, 74(2): 185-190.
[7]	Hao Rui, Deng Xiao, Yang Yibiao, Chen Deyong. Research Progress in Preparation and Applications of ZnO Nanowire/rod Arrays by Hydrothermal Method [J]. Acta Chimica Sinica, 2014, 72(12): 1199-1208.
[8]	Wu Zhicheng, Pan Danmei, Chen Zhi, Lin Zhang. Synthesis of Flaky Flame-retardant Magnesium Hydroxide with High Dispersion [J]. Acta Chimica Sinica, 2012, 70(19): 2045-2048.
[9]	Chen Huajun, Xu Fuqiu, Xue Dong, Yang Yongfu, Zhang Qiufen. Hydrothermal Synthesis and Characterization of Ag-doped Hydroxyapatite Antibacterial Agent [J]. Acta Chimica Sinica, 2012, 70(12): 1362-1366.
[10]	LIAO Wei-Ping, YANG Liu, WANG Fei, HU Yu-Feng, SHENG Zhong-Yi. Performance Study for Low-temperature SCR Catalysts Based on Mn-Ce Prepared by Different Methods [J]. Acta Chimica Sinica, 2011, 69(22): 2723-2728.
[11]	LI Yue-Jun, CAO Tie-Ping, WANG Chang-Hua, SHAO Chang-Lu. Fabrication and Enhanced Photocatalytic Properties of CeO₂/TiO₂ Composite Nanofibers [J]. Acta Chimica Sinica, 2011, 69(21): 2597-2602.
[12]	LI Yan-Hua, HUANG Ke-Long. Synthesis and Capacitance Performance of Co₃O₄/CoO/Co/graphite Composite [J]. Acta Chimica Sinica, 2011, 69(18): 2185-2190.
[13]	YE Qing, YAN Li-Na, HUO Fei-Fei, WANG Hai-Ping, CHENG Shui-Yuan, KANG Tian-Fang. Copper Impregnated Fe-pillared Sodium-treated Sepiolite (Fe-NaPILCS) for Selective Catalytic Reduction of NO with C₃H₆ [J]. Acta Chimica Sinica, 2011, 69(13): 1524-1532.
[14]	LIU Wei, LI Xi-Lin, LIU Juan, HAN Xia, YAN Jing-Hui, KANG Zhen-Hui, LIAN Hong-Zhou. Influence of Gd^3＋Doping on Properties of NaY(MoO₄)₂∶Eu^3＋Phosphors [J]. Acta Chimica Sinica, 2011, 69(13): 1565-1569.
[15]	LIANG Ying, LIU Hua-Jun, LU Jun, TIAN Zhi-Gao. Hydrothermal Synthesis and Electrochemical Performance of Bi₂O₃ Nano-sheets [J]. Acta Chimica Sinica, 2010, 68(19): 1977-1980.