Citation: QIU Jiang-Yuan, XIAO Bi-Yuan, QIN Fang-Hong, ZHANG Mei-Ting, WAN Ting, LIU Jin-Ping, CHEN Jian-Hua, HUANG Zai-Ying. Surface-Electronic-State-Modulated, Single-Crystalline (001) α-Fe₂O₃ Nanosheets with Dual Reaction Sites for Efficient Fenton-Like Catalysis[J]. Chinese Journal of Inorganic Chemistry, ;2019, 35(9): 1665-1677. doi: 10.11862/CJIC.2019.199 shu

Surface-Electronic-State-Modulated, Single-Crystalline (001) α-Fe₂O₃ Nanosheets with Dual Reaction Sites for Efficient Fenton-Like Catalysis

1.
College of Chemistry and Chemical Engineering, Guangxi University for Nationalities, Nanning 530006, China
2.
The Sixth Geological Brigade of Hubei Geological Bureau, Xiaogan, Hubei 432000, China
3.
School of Resources, Environment and Materials, Innovation Center for Metal Resources Utilization and Environment Protection, and Guangxi Key Laboratory of Processing for Non-ferrous Metal and eatured Materials, Guangxi University, Nanning 530004, China

Corresponding author: CHEN Jian-Hua, huangzaiyin@163.com HUANG Zai-Ying, jhchen@gxu.edu.cn
Received Date: 18 February 2019
Revised Date: 22 June 2019

Figures(9)

Intrinsically poor reactivity restricts hematite (α-Fe₂O₃) from heterogeneous Fenton systems. Usually, metal ion doping, noble metal loading, and compounding with other compounds to enhance their catalytic activity are necessary, making them complex, expensive, and difficult to control. Here a surface-electronic-state-modulation-based concept applied to hematite is presented. This concept enables hematite with dual reaction sites as highly reactive and reusable Fenton-like catalysts for efficient catalytic oxidation of recalcitrant organics, via activation of H₂O₂ and without any extra energy input. The rhodamine B degradation rate constants for α-Fe₂O_3-x-330/H₂O₂ systems were 0.834 h^-1, when pH=4, and have a much wider pH working window (pH=2~10) than traditional Fenton systems. Meanwhile, the used catalyst can be easily recovered by magnetic separation. Oxygen vacancy and Fe(Ⅱ) on defective α-Fe₂O_3-x surfaces have been confirmed as the active sites for H₂O₂ activation, while the adjacent vacancy oxygens site adsorbs organic molecules and thus improves the Fenton-like catalytic performance. These findings may not only extend the environment applications of pure transition metal oxide but also stimulate new opportunities for the same as many other transition metal oxides by surface electronic-state modulation.
- α-Fe₂O₃ nanosheets,
- heterogeneous fenton catalysis,
- hydroxyl radical,
- dual reaction sites,
- surface-electronic-state-modulated
1. [1]
  Shannon M A, Bohn P W, Elimelech M, et al. Nature, 2008, 452(7185):301-310 doi: 10.1038/nature06599
2. [2]
  Garrido-Ramírez E G, Theng B K G, Mora M L. Appl. Clay Sci., 2010, 47(3):182-192
3. [3]
  De Laat J, Le T G. Appl. Catal. B, 2006, 66(1/2):137-146
4. [4]
  Masarwa M, Cohen H, Meyerstein D, et al. J. Am. Chem. Soc., 1988, 110(13):4293-4297 doi: 10.1021/ja00221a031
5. [5]
  Neyens E, Baeyens J. J. Hazard. Mater., 2003, 98(1/2/3):33-50
6. [6]
  Haber F, Weiss J. Proc. R. Soc. London Ser. A, 1934, 147(861):332-351 doi: 10.1098/rspa.1934.0221
7. [7]
  Bossmann S H, Oliveros E, Göb S, et al. Water Sci. Technol., 2001, 44(5):257-262 doi: 10.2166/wst.2001.0300
8. [8]
  Bo J, Zheng J, Xiu L, et al. Chem. Eng. J., 2013, 215-216(3):969-978
9. [9]
  Qin Y, Song F, Ai Z, et al. Environ. Sci. Technol., 2015, 49(13):7948-7956 doi: 10.1021/es506110w
10. [10]
  Li T, Zhao Z, Wang Q, et al. Water Res., 2016, 105:479-486 doi: 10.1016/j.watres.2016.09.019
11. [11]
  Jiang C, Garg S, Waite T D. Environ. Sci. Technol., 2015, 49(24):-
12. [12]
  Wang Y, Zhao H, Li M, et al. Appl. Catal. B, 2014, 147:534-545 doi: 10.1016/j.apcatb.2013.09.017
13. [13]
  Morris R V, Lauer H V, Lawson C A, et al. J. Geophys. Res:Solid Earth, 1985, 90(B4):3126-3144 doi: 10.1029/JB090iB04p03126
14. [14]
  Hosseini S G, Ahmadi R, Ghavi A, et al. Powder Technol., 2015, 278:316-322 doi: 10.1016/j.powtec.2015.03.032
15. [15]
  Yang X, Xu X, Xu J, et al. J. Am. Chem. Soc., 2013, 135(43):16058-16061 doi: 10.1021/ja409130c
16. [16]
  Mahadik M A, Shinde S S, Pathan H M, et al. J. Photochem. Photobiol. B, 2014, 141:315-324 doi: 10.1016/j.jphotobiol.2014.10.014
17. [17]
  Guo L, Chen F, Fan X, et al. Appl. Catal. B, 2010, 96(1/2):162-168
18. [18]
  Ai Z, Lu L, Li J, et al. J. Phys. Chem. C, 2007, 111(11):4087-4093 doi: 10.1021/jp065559l
19. [19]
  Hendriksen B L M, Ackermann M D, Van Rijn R, et al. Nat. Chem., 2010, 2(9):730 doi: 10.1038/nchem.728
20. [20]
  Martinez U, Hansen J Ø, Lira E, et al. Phys. Rev. Lett., 2012, 109(15):155501 doi: 10.1103/PhysRevLett.109.155501
21. [21]
  Li H, Li J, Ai Z, et al. Angew. Chem., Int. Ed, 2018, 57(1):122-138 doi: 10.1002/anie.201705628
22. [22]
  Mao C, Cheng H, Tian H, et al. Appl. Catal. B, 2018, 228:87-96 doi: 10.1016/j.apcatb.2018.01.018
23. [23]
  Li H, Shang J, Yang Z, et al. Environ. Sci. Technol, 2017, 51(10):5685-5694 doi: 10.1021/acs.est.7b00040
24. [24]
  Xing M, Xu W, Dong C, et al. Chemistry, 2018, 6(4):1359-1372
25. [25]
  Song Z, Wang B, Yu J, et al. Appl. Surf. Sci., 2017, 413:292-301 doi: 10.1016/j.apsusc.2017.04.011
26. [26]
  Zhou X, Lan J, Liu G, et al. Angew. Chem. Int. Ed., 2012, 51(1):178-182 doi: 10.1002/anie.201105028
27. [27]
  Niu H, Lu J, Song J J, et al. Ind. Eng. Chem. Res., 2016, 55(31):8527-8533 doi: 10.1021/acs.iecr.6b00984
28. [28]
  De Faria D L A, Lopes F N. Vib. Spectrosc., 2007, 45(2):117-121 doi: 10.1016/j.vibspec.2007.07.003
29. [29]
  Xu J S, Zhu Y J. ACS Appl. Mater. Interfaces, 2012, 4(9):4752 doi: 10.1021/am301123f
30. [30]
  Nasrazadani S, Raman A. Corros. Sci., 1993, 34(8):1355-1365 doi: 10.1016/0010-938X(93)90092-U
31. [31]
  Xu X N, Wolfus Y, Shaulov A, et al. J. Appl. Phys., 2002, 91(7):4611-4616 doi: 10.1063/1.1457544
32. [32]
  Wu J, Mao S, Ye Z G, et al. ACS Appl. Mater. Interfaces, 2010, 2(6):1561-1564 doi: 10.1021/am1002052
33. [33]
  Cao W, Tan O K, Pan J S, et al. Mater. Chem. Phys., 2002, 75(1):67-70
34. [34]
  Liao A Z, Chen J B, Wang C W, et al. J. Vac. Sci. Technol., B, 2016, 34(2):1-8
35. [35]
  Wang J, Wang C W, Li Y, et al. Thin Solid Films, 2008, 516(21):7689-7694 doi: 10.1016/j.tsf.2008.03.023
36. [36]
  Guan M, Xiao C, Zhang J, et al. J. Am. Chem. Soc., 2013, 135(28):10411-10417 doi: 10.1021/ja402956f
37. [37]
  Chen J, Li Y F, Sit P, et al. J. Am. Chem. Soc., 2013, 135:18774-18777 doi: 10.1021/ja410685m
38. [38]
  Gonzalez-Olmos R, Holzer F, Kopinke F D, et al. Appl. Catal. A:General., 2011, 398:44-53 doi: 10.1016/j.apcata.2011.03.005
39. [39]
  Dixon W T, Norman R O C. Nature, 1962, 196:891-892 doi: 10.1038/196891a0
40. [40]
  Baltrusaitis J, Cwiertny D M, Grassian V H. Phys. Chem. Chem. Phys., 2007, 9:5542-5554 doi: 10.1039/b709167b
41. [41]
  Grosvenor A P, Kobe B A, Mcintyre N S. Surf. Sci., 2004, 572(2):217-227
42. [42]
  Huang X, Hou X, Jia F, et al. ACS Appl. Mater. Interfaces, 2017, 9(10):8751-8758 doi: 10.1021/acsami.6b16600
43. [43]
  Hou X, Huang X, Jia F, et al. Environ. Sci. Technol, 2017, 51(9):5118-5126 doi: 10.1021/acs.est.6b05906
44. [44]
  Xu Y, Lv K, Xiong Z, et al. J. Phys. Chem. C, 2007, 111(51):19024-19032 doi: 10.1021/jp076364w
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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

Surface-Electronic-State-Modulated, Single-Crystalline (001) α-Fe2O3 Nanosheets with Dual Reaction Sites for Efficient Fenton-Like Catalysis

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通讯作者: 陈斌, bchen63@163.com

Surface-Electronic-State-Modulated, Single-Crystalline (001) α-Fe₂O₃ Nanosheets with Dual Reaction Sites for Efficient Fenton-Like Catalysis