Citation: JIAO Jin-Zhen, LI Shi-Hui, HUANG Bi-Chun. Preparation of Manganese Oxides Supported on Graphene Catalysts and Their Activity in Low-Temperature NH₃-SCR[J]. Acta Physico-Chimica Sinica, ;2015, 31(7): 1383-1390. doi: 10.3866/PKU.WHXB201504292 shu

Preparation of Manganese Oxides Supported on Graphene Catalysts and Their Activity in Low-Temperature NH₃-SCR

1.
1 College of Environment and Energy, South China University of Technology, Guangzhou 510006, P. R. China;
2 Key Laboratory of the Ministry of Education for Pollution Control and Ecosystem Restoration in Industry Clusters, South China University of Technology, Guangzhou 510006, P. R. China

Received Date: 7 January 2015
Available Online: 29 April 2015
Fund Project: 国家自然科学基金(51478191)资助项目 (51478191)

Graphene oxide ( ) was synthesized using an improved Hummers method. Subsequently, catalysts of manganese oxides (at varying loadings) supported on graphene (MnO_x/GR) were prepared by hydrothermal reaction for application in the selective catalytic reduction (SCR) of NO_x with NH₃ at low temperatures. The structural properties and catalytic performance were evaluated by Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, X-ray powder diffraction (XRD), transmission electron microscopy (TEM), N₂ adsorption-desorption, X-ray photoelectron spectroscopy (XPS), and H₂ temperature-programmed reduction (H₂-TPR). The characterization results indicated that abundant functional groups existed on the surface of the prepared that could combine with manganese during preparation of the catalysts. Manganese oxide entities, with different crystallinities (MnO, Mn₃O₄, or MnO₂), were dispersed on the surface of graphene. The results of the catalytic studies showed that the MnO_x/GR catalysts prepared with different MnO_x loadings all exhibited excellent low-temperature SCR activities. The catalyst with 20%(w) MnO_x displayed the best activity, which was attributed to the high content of high-valent manganese and oxygen adsorbed onto the catalyst surface, as well as to the enhancement in redox abilities and the addition of active sites at low temperatures.
- Selective catalytic reduction,
- Nitrogen oxide,
- Graphene,
- Graphene oxide,
- Manganese oxide
1. [1]
  
  (1) Qi, G.; Yang, R.T. Appl. Catal. B: Environ. 2003, 44, 217. doi: 10.1016/S0926-3373(03)00100-0
2. [2]
  (2) Park, T. S.; Jeong, S. K.; Hong, S. H.; Hong, S. C. Ind. Eng. Chem. Res. 2001, 40, 4491. doi: 10.1021/ie010218+
3. [3]
  (3) Huang, B. C.; Huang, R.; Jin, D. J.; Ye, D. Q. Catal. Today 2007, 126, 279. doi: 10.1016/j.cattod.2007.06.002
4. [4]
  (4) Thirupathi, B.; Smirniotis, P. G. Appl. Catal. B: Environ. 2011, 110, 195. doi: 10.1016/j.apcatb.2011.09.001
5. [5]
  (5) Huang, P.; Pan, S.W.; Huang, B. C.; Cheng, H.; Ye, D. Q.; Wu, J. L.; Fu, M. L.; Lu, S. L. Acta Phys. -Chim. Sin. 2013, 29, 176. [黄萍, 盘思伟, 黄碧纯, 程华, 叶代启, 吴军良, 付名利, 卢圣良. 物理化学学报, 2013, 29, 176.] doi: 10.3866/PKU.WHXB201210094
6. [6]
  (6) Ma, Z. X.; Yang, H. S.; Liu, F.; Zhang, X. B. Appl. Catal. A: Gen. 2013, 467, 450. doi: 10.1016/j.apcata.2013.08.020
7. [7]
  (7) Tang, X. L.; Hao, J. M.; Yi, H. H.; Li, J. H. Catal. Today 2007, 126, 406. doi: 10.1016/j.cattod.2007.06.013
8. [8]
  (8) Masaaki, Y.; Akinori, Y.; Isao, Mochida. Appl. Catal. A 1998, 173, 239. doi: 10.1016/S0926-860X(98)00182-3
9. [9]
  (9) Wang, L. S.; Huang, B. C.; Su, Y. X.; Zhou, G. Y.; Wang, K. L.; Luo, H. C.; Ye, D. Q. Chem. Eng. J. 2012, 192, 232. doi: 10.1016/j.cej.2012.04.012
10. [10]
  (10) Fang, C.; Zhang, D. S.; Cai, S. X.; Zhang, L.; Huang, L.; Li, H. R.; Maitarad, P.; Shi, L. Y.; Gao, R. H.; Zhang, J. P. Nanoscale 2013, 5, 9199. doi: 10.1039/c3nr02631k
11. [11]
  (11) Pourkhalil, M.; Moghaddam, A. Z.; Rashidi, A.; Towfighi, J.; Mortazavi, Y. Appl. Surf. Sci. 2013, 279, 250. doi: 10.1016/j.apsusc.2013.04.076
12. [12]
  (12) Li, N.; Geng, Z. F.; Cao, M. H.; Ren, L.; Zhao, X. Y.; Liu, B.; Tian, Y.; Hu, C.W. Carbon 2013, 54, 124. doi: 10.1016/j.carbon.2012.11.009
13. [13]
  (13) Bruno, F. M.; Philippe, S. Catal. Sci. Technol. 2012, 2, 54.
14. [14]
  (14) Moussa, S. O.; Panchakarla, L. S.; Ho, M. Q.; El-Shall, M. S. ACS Catal. 2014, 4, 535. doi: 10.1021/cs4010198
15. [15]
  (15) Gilje, S.; Han, S.; Wang, M. S.; Wang, K. L.; Kaner, R. B. Nano Lett. 2007, 7, 3394. doi: 10.1021/nl0717715
16. [16]
  (16) Chen, D. Y.; Chen, W. X.; Ma, L.; Ji, G.; Chang, K.; Lee, J. Y. Mater.Today 2014, 17, 184. doi: 10.1016/j.mattod.2014.04.001
17. [17]
  (17) Li, L.; Seng, K. H.; Liu, H. K.; Nevirkovets, I. P.; Guo, Z. P. Electrochim. Acta 2013, 87, 801. doi: 10.1016/j.electacta.2012.08.127
18. [18]
  (18) Li, M.; Liu, Q.; Jia, Z. J.; Xu, X. C.; Cheng, Y. F.; Zheng, Y. F.; Xi, T. F.; Wei, S. C. Carbon 2014, 67, 185. doi: 10.1016/j.carbon.2013.09.080
19. [19]
  (19) Lu, X.; Song, C.; Chang, C.; Teng, Y.; Tong, Z.; Tang, X. Ind. Eng. Chem. Res. 2014, 53, 11601. doi: 10.1021/ie5016969
20. [20]
  (20) Romero, H. E.; Joshi, P.; Gupta, A. K.; Gutierrez, H. R.; Cole, M.W.; Tadigadapa, S. A.; Ekluud, P. C. Nanotechnology 2009, 20, 245501. doi: 10.1088/0957-4484/20/24/245501
21. [21]
  (21) Chen, S.; Zhu, J.W.; Wu, X. D.; Han, Q. F.; Wang, X. ACS Nano 2010, 4, 2822. doi: 10.1021/nn901311t
22. [22]
  (22) Marcano, D. C.; Kosynkin, D. V.; Berlin, J. M.; Sinitskii, A.; Sun, Z. Z.; Slesarev, A.; Alemany, L. B.; Lu, W.; Tour, J. M. ACS Nano 2010, 4, 4806. doi: 10.1021/nn1006368
23. [23]
  (23) Tang, X. L.; Hao, J. M.; Yi, H. H.; Ning, P. J. Rare Earths 2007, 25, 240. doi: 10.1016/S1002-0721(07)60479-7
24. [24]
  (24) Jeong, H.; Lee, Y. P.; Jin, M. H.; Kim, E. S.; Bae, J. J.; Lee, Y. H. Chem. Phys. Lett. 2009, 470, 255. doi: 10.1016/j.cplett.2009.01.050
25. [25]
  (25) Gu, Z.; Li, C.; Wang, G.; Zhang, L.; Li, X.; Wang, W.; Jin, S. J. Polym. Sci. Part B: Polym. Phys. 2010, 48, 1329. doi: 10.1002/polb.v48:12
26. [26]
  (26) Kai, K.; Yoshida, Y.; Kobayashi, Y.; Kageyama, H.; Saito, G. Dalton Trans. 2011, 41, 825.
27. [27]
  (27) Buciuman, F.; Patcas, F.; Craciun, R.; Zahn, D. R. T. Phys. Chem. Chem. Phys. 1999, 1, 185. doi: 10.1039/a807821a
28. [28]
  (28) Ferrari, A. C.; Basko, D. M. Nat. Nanotechnology 2013, 8, 235. doi: 10.1038/nnano.2013.46
29. [29]
  (29) Li, B.; Zhou, L.; Wu, D.; Peng, H. L.; Yan, K.; Zhou, Y.; Liu, Z. F. ACS Nano 2011, 5, 5957. doi: 10.1021/nn201731t
30. [30]
  (30) Voggu, R.; Das, B.; Rout, C. S.; Rao, C. N. R. J. Phys.: Condens. Matter 2008, 20, 472204. doi: 10.1088/0953-8984/20/47/472204
31. [31]
  (31) Lee, J.; Novoselov, K. S.; Shin, H. S. ACS Nano 2011, 5, 608. doi: 10.1021/nn103004c
32. [32]
  (32) Jiang, L.; Yao, M.; Liu, B.; Li, Q.; Liu, R.; Lv, H.; Lu, S.; ng, C.; Zou, B.; Cui, T.; Liu, B. B. Crystengcomm 2013, 15, 3739. doi: 10.1039/c3ce27109a
33. [33]
  (33) Han, Y. F.; Chen, F. X.; Zhong, Z. Y.; Ramesh, K.; Widjaja, E.; Chen, L.W. Catal. Commun. 2006, 7, 739. doi: 10.1016/j.catcom.2006.08.006
34. [34]
  (34) Huang, H. C.; Ye, D. Q.; Huang, B. C.; Wei, Z. L. Catal. Today 2008, 139, 100. doi: 10.1016/j.cattod.2008.08.028
35. [35]
  (35) Lu, P.; Li, C. T.; Zeng, G. M.; He, L. J.; Peng, D. L.; Cui, H. F.; Li, S. H.; Zhai, Y. B. Appl. Catal. B 2010, 96, 157. doi: 10.1016/j.apcatb.2010.02.014
36. [36]
  (36) Zhang, J. T.; Xiong, Z. G.; Zhao, X. S. J. Mater. Chem. 2011, 21, 3634. doi: 10.1039/c0jm03827j
37. [37]
  (37) Park, E.; Kim, M.; Jung, H.; Chin, S.; Jurng, J. ACS Catal. 2013, 3, 1518. doi: 10.1021/cs3007846
38. [38]
  (38) Ponce, S.; Peña, M. A.; Fierro, J. L. G. Appl. Catal. B: Environ. 2000, 24, 193. doi: 10.1016/S0926-3373(99)00111-3
39. [39]
  (39) Kang, M.; Park, E. D.; Kim, J. M.; Yie, J. E. Appl. Catal. A: Gen. 2007, 327, 261. doi: 10.1016/j.apcata.2007.05.024
40. [40]
  (40) Yang, C.; Liu, X. Q.; Huang, B. C.; Wu, Y. M. Acta Phys. -Chim. Sin. 2014, 30, 1805. [杨超, 刘小青, 黄碧纯, 吴友明. 物理化学学报, 2014, 30, 1805.] doi: 10.3866/PKU.WHXB201407162
1. [1]
  Zhuo WANG , Junshan ZHANG , Shaoyan YANG , Lingyan ZHOU , Yedi LI , Yuanpei LAN . Preparation and photocatalytic performance of CeO₂-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1708-1718. doi: 10.11862/CJIC.20240067
2. [2]
  Zhihuan XU , Qing KANG , Yuzhen LONG , Qian YUAN , Cidong LIU , Xin LI , Genghuai TANG , Yuqing LIAO . Effect of graphene oxide concentration on the electrochemical properties of reduced graphene oxide/ZnS. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1329-1336. doi: 10.11862/CJIC.20230447
3. [3]
  Zeyu XU , Anlei DANG , Bihua DENG , Xiaoxin ZUO , Yu LU , Ping YANG , Wenzhu YIN . Evaluation of the efficacy of graphene oxide quantum dots as an ovalbumin delivery platform and adjuvant for immune enhancement. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1065-1078. doi: 10.11862/CJIC.20240099
4. [4]
  Yunting Shang , Yue Dai , Jianxin Zhang , Nan Zhu , Yan Su . Something about RGO (Reduced Graphene Oxide). University Chemistry, 2024, 39(9): 273-278. doi: 10.3866/PKU.DXHX202306050
5. [5]
  Yan LIU , Jiaxin GUO , Song YANG , Shixian XU , Yanyan YANG , Zhongliang YU , Xiaogang HAO . Exclusionary recovery of phosphate anions with low concentration from wastewater using a CoNi-layered double hydroxide/graphene electronically controlled separation film. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1775-1783. doi: 10.11862/CJIC.20240043
6. [6]
  Ping ZHANG , Chenchen ZHAO , Xiaoyun CUI , Bing XIE , Yihan LIU , Haiyu LIN , Jiale ZHANG , Yu'nan CHEN . Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1965-1974. doi: 10.11862/CJIC.20240014
7. [7]
  Xiaofeng Zhu , Bingbing Xiao , Jiaxin Su , Shuai Wang , Qingran Zhang , Jun Wang . Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides. Acta Physico-Chimica Sinica, 2024, 40(12): 2407005-. doi: 10.3866/PKU.WHXB202407005
8. [8]
  Xin Han , Zhihao Cheng , Jinfeng Zhang , Jie Liu , Cheng Zhong , Wenbin Hu . Design of Amorphous High-Entropy FeCoCrMnBS (Oxy) Hydroxides for Boosting Oxygen Evolution Reaction. Acta Physico-Chimica Sinica, 2025, 41(4): 100033-. doi: 10.3866/PKU.WHXB202404023
9. [9]
  .
  CCS Chemistry | 超分子活化底物为自由基促进高效选择性光催化氧化
  . CCS Chemistry, 2025, 7(10.31635/ccschem.025.202405229): -.
10. [10]
  Qianwen Han , Tenglong Zhu , Qiuqiu Lü , Mahong Yu , Qin Zhong . 氢电极支撑可逆固体氧化物电池性能及电化学不对称性优化. Acta Physico-Chimica Sinica, 2025, 41(1): 2309037-. doi: 10.3866/PKU.WHXB202309037
11. [11]
  Xueyu Lin , Ruiqi Wang , Wujie Dong , Fuqiang Huang . 高性能双金属氧化物负极的理性设计及储锂特性. Acta Physico-Chimica Sinica, 2025, 41(3): 2311005-. doi: 10.3866/PKU.WHXB202311005
12. [12]
  Chuanming GUO , Kaiyang ZHANG , Yun WU , Rui YAO , Qiang ZHAO , Jinping LI , Guang LIU . Performance of MnO₂-0.39IrO_x composite oxides for water oxidation reaction in acidic media. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1135-1142. doi: 10.11862/CJIC.20230459
13. [13]
  Peng YUE , Liyao SHI , Jinglei CUI , Huirong ZHANG , Yanxia GUO . Effects of Ce and Mn promoters on the selective oxidation of ammonia over V₂O₅/TiO₂ catalyst. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 293-307. doi: 10.11862/CJIC.20240210
14. [14]
  Xiaotian ZHU , Fangding HUANG , Wenchang ZHU , Jianqing ZHAO . Layered oxide cathode for sodium-ion batteries: Surface and interface modification and suppressed gas generation effect. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 254-266. doi: 10.11862/CJIC.20240260
15. [15]
  Lina Guo , Ruizhe Li , Chuang Sun , Xiaoli Luo , Yiqiu Shi , Hong Yuan , Shuxin Ouyang , Tierui Zhang . 层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响. Acta Physico-Chimica Sinica, 2025, 41(1): 2309002-. doi: 10.3866/PKU.WHXB202309002
16. [16]
  Yaping ZHANG , Tongchen WU , Yun ZHENG , Bizhou LIN . Z-scheme heterojunction β-Bi₂O₃ pillared CoAl layered double hydroxide nanohybrid: Fabrication and photocatalytic degradation property. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 531-539. doi: 10.11862/CJIC.20240256
17. [17]
  Endong YANG , Haoze TIAN , Ke ZHANG , Yongbing LOU . Efficient oxygen evolution reaction of CuCo₂O₄/NiFe-layered bimetallic hydroxide core-shell nanoflower sphere arrays. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 930-940. doi: 10.11862/CJIC.20230369
18. [18]
  Caixia Lin , Zhaojiang Shi , Yi Yu , Jianfeng Yan , Keyin Ye , Yaofeng Yuan . Ideological and Political Design for the Electrochemical Synthesis of Benzoxathiazine Dioxide Experiment. University Chemistry, 2024, 39(2): 61-66. doi: 10.3866/PKU.DXHX202309005
19. [19]
  Zhenlin Zhou , Siyuan Chen , Yi Liu , Chengguo Hu , Faqiong Zhao . A New Program of Voltammetry Experiment Teaching Based on Laser-Scribed Graphene Electrode. University Chemistry, 2024, 39(2): 358-370. doi: 10.3866/PKU.DXHX202308049
20. [20]
  Tianqi Bai , Kun Huang , Fachen Liu , Ruochen Shi , Wencai Ren , Songfeng Pei , Peng Gao , Zhongfan Liu . 石墨烯厚膜热扩散系数与微观结构的关系. Acta Physico-Chimica Sinica, 2025, 41(3): 2404024-. doi: 10.3866/PKU.WHXB202404024

Get Citation

PDF

XML

Metrics

PDF Downloads(364)
Abstract views(462)
HTML views(2)

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

Preparation of Manganese Oxides Supported on Graphene Catalysts and Their Activity in Low-Temperature NH3-SCR

Metrics

通讯作者: 陈斌, bchen63@163.com

Preparation of Manganese Oxides Supported on Graphene Catalysts and Their Activity in Low-Temperature NH₃-SCR