Citation: Yingsi Wu, Hao Yu, Hongjuan Wang, Feng Peng. Controllable synthesis and catalytic performance of graphene-supported metal oxide nanoparticles[J]. Chinese Journal of Catalysis, ;2014, 35(6): 952-959. doi: 10.1016/S1872-2067(14)60114-5 shu

Controllable synthesis and catalytic performance of graphene-supported metal oxide nanoparticles

1.
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China

Corresponding author: Hao Yu, Feng Peng,
Received Date: 18 March 2014
Available Online: 18 April 2014
Fund Project: 国家自然科学基金(20806027，21273079)；广东省自然科学基金(S20120011275)；新世纪优秀人才支持计划(NCET-12-0190). (20806027，21273079)；广东省自然科学基金(S20120011275)；新世纪优秀人才支持计划(NCET-12-0190)

The size of nanoparticles plays a crucial role in their performance. In this article, three methods, i.e., direct impregnation, homogeneous oxidative precipitation with hydrogen peroxide, and ammonia-catalyzed hydrolysis, were applied to synthesize iron, cobalt, and nickel metal oxide nanoparticles supported on graphene. The influence of the three deposition methods on particle size distribution was investigated. Transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were used to characterize the morphology and structure of the catalysts. The highest dispersion and the most uniform particle size distribution were obtained by the hydrogen peroxide homogeneous oxidative precipitation method. Hydrogen peroxide favors the maximization of the oxygen-containing groups on graphenes, thereby providing sufficient absorption and nucleation sites to give a high dispersion of nanoparticles. In contrast, ammonia accelerates the nucleation speed and results in the largest particle size and inhomogeneity. The catalytic properties of the graphene-supported metal oxide nanoparticles were tested with the oxidation of benzyl alcohol as a probe reaction. The reaction activity decreased in the following order: catalysts prepared by hydrogen peroxide-assisted deposition > direct impregnation > ammonia-catalyzed hydrolysis. The decrease in reaction activity was consistent with the order of increasing catalyst particle sizing shown in transmission electron microscopy images. The catalytic relevance of the particle size showed a necessity for the development of effective methods for size-controlled nanocatalyst synthesis on graphenes.
- Particle size,
- Graphene,
- Metal oxide,
- Hydrogen peroxide,
- Benzyl alcohol
1. [1]
  [1] Balaya P. Energy Environ Sci, 2008, 1: 645
2. [2]
  [2] Cheng M Y, Ye Y S, Chiu T M, Pan C J, Hwang B J. J Power Sources, 2014, 253: 27
3. [3]
  [3] Li Y, Liu Q Y, Shen W J. Dalton Trans, 2011, 40: 5811
4. [4]
  [4] Hu H, Zhao Z B, Wan W B, Gogotsi Y, Qiu J S. Adv Mater, 2013, 25: 2219
5. [5]
  [5] Wang Z L, Xu D, Wang H G, Wu Z, Zhang X B. ACS Nano, 2013, 7: 2422
6. [6]
  [6] Phua P H, Lefort L, Boogers J A F, de Tristany M, Vries J G. Chem Commun, 2009: 3747
7. [7]
  [7] Lin J K, Qiao B T, Liu J Y, Huang Y Q, Wang A Q, Li L, Zhang W S, Allard L F, Wang X D, Zhang T. Angew Chem Int Ed, 2012, 51: 2920
8. [8]
  [8] Zhu J, Kailasam K, Fischer A, Thomas A. ACS Catal, 2011, 1: 342
9. [9]
  [9] He Q G, Li Q, Khene S, Ren X M, López-Suárez F E, Lozano-Castelló D, Bueno-López A, Wu G. J Phys Chem C, 2013, 117: 8697
10. [10]
  [10] Galvis H M T, Bitter J H, Davidian T, Ruitenbeek M, Dugulan A I, de Jong K P. J Am Chem Soc, 2012, 134: 16207
11. [11]
  [11] Fu T J, Lü J, Li Z H. Ind Eng Chem Res, 2014, 53: 1342
12. [12]
  [12] Yang Y F, Jia L T, Hou B, Li D B, Wang J G, Sun Y H. Catal Lett, 2014, 144: 133
13. [13]
  [13] Pina G, Louis C, Keane M A. Phys Chem Chem Phys, 2003, 5: 1924
14. [14]
  [14] Du A J, Ng Y H, Bell N J, Zhu Z H, Amal R, Smith S C. J Phys Chem Lett, 2011, 2: 894
15. [15]
  [15] Sun Y Q, Shi G Q. J Polym Sci Pt B-Polym Phys, 2013, 51: 231
16. [16]
  [16] Kou R, Shao Y Y, Wang D H, Engelhard M H, Kwak J H, Wang J, Viswanathan V V, Wang C M, Lin Y H, Wang Y, Aksay I A, Liu J. Electrochem Commun, 2009, 11: 954
17. [17]
  [17] Dong X C, Xu H, Wang X W, Huang Y X, Chan-Park M B, Zhang H, Wang L H, Huang W, Chen P. ACS Nano, 2012, 6: 3206
18. [18]
  [18] Gao Y J, Ma D, Hu G, Zhai P, Bao X H, Zhu B, Zhang B S, Su D S. Angew Chem Int Ed, 2011, 50: 10236
19. [19]
  [19] Byon H R, Suntivich J, Shao-Horn Y. Chem Mater, 2011, 23: 3421
20. [20]
  [20] Zhang G Q, Lou X W. Sci Rep, 2013, 3: 1470
21. [21]
  [21] Myung S, Park J, Lee H, Kim K S, Hong S. Adv Mater, 2010, 22: 2045
22. [22]
  [22] Mao S, Lu G H, Yu K H, Bo Z. Chen J H. Adv Mater, 2010, 22: 3521
23. [23]
  [23] Zhang G Q, Xia B Y, Wang X, Lou X W. Adv Mater, 2013, 26: 2408
24. [24]
  [24] Tien H W, Huang Y L, Yang S Y, Wang J Y, Ma C M. Carbon, 2011, 49: 1550
25. [25]
  [25] Ha H W, Choudhury A, Kamal T, Kim D H, Park S Y. ACS Appl Mater Inter, 2012, 4: 4623
26. [26]
  [26] Ji Z Y, Shen X P, Zhu G X, Zhou H, Yuan A H. J Mater Chem, 2012, 22: 3471
27. [27]
  [27] Wu Z S, Ren W C, Wen L, Gao L B, Zhao J P, Chen Z P, Zhou G M, Li F, Cheng H M. ACS Nano, 2010, 4: 3187
28. [28]
  [28] Gotoh K, Kinumoto T, Fujii E, Yamamoto A, Hashimoto H, Ohkubo T, Itadani A, Kuroda Y, Ishida H. Carbon, 2011, 49: 1118
29. [29]
  [29] Liu Y W, Guan M X, Feng L, Deng S L, Bao J F, Xie S Y, Chen Z, Huang R B, Zheng L S. Nanotechnol, 2013, 24: 025604
30. [30]
  [30] Ren L L, Huang S, Fan W, Liu T X. Appl Surf Sci, 2011, 258: 1132
31. [31]
  [31] Zhu J X, Sharma Y K, Zeng Z Y, Zhang X J, Srinivasan M, Mhaisalkar S, Zhang H, Hng H H, Yan Q Y. J Phys Chem C, 2011, 115: 8400
32. [32]
  [32] Fang M, Chen Z X, Wang S Z, Lu H B. Nanotechnol, 2012, 23: 085704
33. [33]
  [33] Fu X B, Yu H, Peng F, Wang H J, Qian Y. Appl Catal A, 2007, 321: 190
34. [34]
  [34] Wu Y S, Yu H, Peng F, Wang H J. Mater Lett, 2012, 67: 245
35. [35]
  [35] Chen Y T, Wang H P, Liu C J, Zeng Z Y, Zhang H, Zhou C M, Jia X L, Yang Y H. J Catal, 2012, 289: 105
36. [36]
  [36] Chen H, Tang Q H, Chen Y T, Yan Y B, Zhou C M, Guo Z, Jia X L, Yang Y H. Catal Sci Technol, 2013, 3: 328
37. [37]
  [37] Zhou C M, Chen H, Yan Y B, Jia X L, Liu C J, Yang Y H. Catal Today, 2013, 211: 104
38. [38]
  [38] Zhou X T, Ji H B. Chin J Catal (周贤太, 纪红兵. 催化学报), 2012, 33: 1906
39. [39]
  [39] Wu S X, He Q Y, Zhou C M, Qi X Y, Huang X, Yin Z Y, Yang Y H, Zhang H. Nanoscale, 2012, 4: 2478
40. [40]
  [40] Ali S R, Chandra P, Latwal M, Jain S K, Bansal V K, Singh S P. Chin J Catal (催化学报), 2011, 32: 1844
41. [41]
  [41] Kovtyukhova N I, Ollivier P J, Martin B R, Mallouk T E, Chizhik S A, Buzaneva E V, Gorchinskiy A D. Chem Mater, 1999, 11: 771
42. [42]
  [42] Zhang J T, Xiong Z G, Zhao X S. J Mater Chem, 2011, 21: 3634
43. [43]
  [43] Tuxen A, Carenco S, Chintapalli M, Chuang C H, Escudero C, Pach E, Jiang B, Borondics F, Beberwyck B, Alivisatos A P, Thornton G, Pong W F, Guo J H, Perez R, Besenbacher F, Salmeron M. J Am Chem Soc, 2013, 135: 2273
44. [44]
  [44] Wang C M, Baer D R, Amonette J E, Engelhard M H, Antony J, Qiang Y. J Am Chem Soc, 2009, 131: 8824
45. [45]
  [45] Koo B, Xiong H, Slater M D, Prakapenka V B, Baasubramanian M, Podsiadlo P, Johnson C S, Rajh T, Shevchenko E V. Nano Lett, 2012, 12: 2429
46. [46]
  [46] Yan J, Zhao Z W, Pan L K. Phys Status Solidi (A), 2011, 208: 2335
47. [47]
  [47] Zhang Y J, Hu W B, Li B, Peng C, Fan C H, Huang Q. Nanotechnol, 2011, 22: 345601
48. [48]
  [48] Li Y J, Li Y J, Zhu E B, McLouth T, Chiu C Y, Huang X Q, Huang Y. J Am Chem Soc, 2012, 134: 12326
49. [49]
  [49] Chuang T J, Brundle C R, Rice D W. Surf Sci, 1976, 59: 413
50. [50]
  [50] Ji H B, Wang T T, Zhang M Y, Chen Q L, Gao X N. React Kinet Catal Lett, 2007, 90: 251
51. [51]
  [51] Tuxen A, Carenco S, Chintapalli M, Chuang C H, Escudero C, Pach E, Jiang P, Borondics F, Beberwyck B, Alivisatos A P, Thornton G, Pong W F, Guo J H, Perez R, Besenbacher F, Salmeron M. J Am Chem Soc, 2013, 135: 2273
52. [52]
  [52] Yu Y B, Zhao J J, Han X, Zhang Y, Qin X B, Wang B Y. Chin J Catal (余运波, 赵娇娇, 韩雪, 张燕, 秦秀波, 王宝义. 催化学报), 2013, 34: 283
53. [53]
  [53] Yan X H, Zhang G R, Xu B Q. Chin J Catal (严祥辉, 张贵荣, 徐柏庆. 催化学报), 2013, 34: 1992
54. [54]
  [54] Zhang K J, Zhang L X, Chen X, He X, Wang X G, Dong S M, Han P X, Zhang C J, Wang S, Gu L, Cui G L. J Phys Chem C, 2012, 117: 858
55. [55]
  [55] Liao L, Zhang Q H, Su ZH, Zhao Z Z, Wang Y N, Li Y, Lu X X, Wei D G, Feng G Y, Yu Q K, Cai X J, Zhao J M, Ren Z F, Fang H, Robles-Hernandez F, Baldelli S, Bao J M. Nat Nanotechnol, 2014, 9: 69
56. [56]
  [56] Zhu L H, Zheng L, Du K Q, Fu H, Li Y H, You G R, Chen B H. RSC Adv, 2013, 3: 713
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