Citation: Qiangwei Li, Mengmeng Zhang, Yongyi Xu, Xiaoqi Quan, Yiao Xu, Wen Liu, Lidong Wang. Constructing heterojunction interface of Co₃O₄/TiO₂ for efficiently accelerating acetaminophen degradation via photocatalytic activation of sulfite[J]. Chinese Chemical Letters, ;2023, 34(3): 107530. doi: 10.1016/j.cclet.2022.05.044 shu

Constructing heterojunction interface of Co₃O₄/TiO₂ for efficiently accelerating acetaminophen degradation via photocatalytic activation of sulfite

Qiangwei Li ^a ,
Mengmeng Zhang ^a ,
Yongyi Xu ^c ,
Xiaoqi Quan ^a ,
Yiao Xu ^a ,
Wen Liu ^b ,
Lidong Wang ^{a, *,}

a.
Department of Environmental Science and Engineering, Hebei Key Lab of Power Plant Flue Gas Multi–Pollutants Control, North China Electric Power University, Baoding 071003, China
b.
The Key Laboratory of Water and Sediment Sciences, Ministry of Education, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
c.
China Power Hua Chuang Electricity Technology Research Company Ltd., Suzhou 215123, China

wld@ncepu.edu.cn

Received Date: 14 January 2022
Revised Date: 29 April 2022
Accepted Date: 12 May 2022
Available Online: 17 May 2022

Figures(6)

Achieving efficient degradation of organic pollutants via activation of sulfite is meaningful but challenging. Herein, we have constructed a heterogeneous catalyst system involving Co₃O₄ and TiO₂ nanoparticles to form the p-n heterojunction (Co₃O₄/TiO₂) to degrade acetaminophen (ACE) through photocatalytic activation of sulfite. Specifically, X-ray photoelectron spectroscopy analysis and theoretical calculations provide compelling evidence of electron transfer from Co₃O₄ to TiO₂ at the heterointerface. The interfacial electron redistribution of Co₃O₄/TiO₂ tunes the adsorption energy of HSO₃^‒/SO₃^2‒ in sulfite activation process for enhanced the catalytic activity. Owing to its unique heterointerface, the degradation efficiency of ACE reached 96.78% within 10 min. The predominant active radicals were identified as ^•OH, h⁺, and SO_x^•− through radical quenching experiments and electron spin resonance capture. Besides, the possible degradation pathway was deduced by monitoring the generated intermediate products. Thereafter, the enhanced roles of well-engineered compositing interface in photocatalytic activation of sulfite for complete degradation of ACE were unveiled that it can improve light absorption ability, facilitate the generation of active species, and optimize reactive pathways. Considering that sulfite is a waste from flue gas desulfurization process, the photocatalytic activation of sulfite system will open up new avenues of beneficial use of air pollutants for the removal of pharmaceutical wastewater.
- Sulfite,
- Photocatalytic activation,
- Charge transfer,
- Heterojunction interface,
- Degradation mechanism
1. [1]
  D. Guo, S. You, F. Li, Y. Liu, Chin. Chem. Lett. 33 (2022) 1–10. doi: 10.1016/j.cclet.2021.06.027
2. [2]
  T. Luo, Y. Yuan, D. Zhou, et al., Chem. Eng. J. 363 (2019) 329–336. doi: 10.1016/j.cej.2019.01.114
3. [3]
  J. Qi, J. Liu, F. Sun, et al., Chin. Chem. Lett. 32 (2021) 1814–1818. doi: 10.1016/j.cclet.2020.11.026
4. [4]
  P. Hu, M. Long, Appl. Catal. B 181 (2016) 103–117. doi: 10.1016/j.apcatb.2015.07.024
5. [5]
  M. Ma, L. Chen, J. Zhao, W. Liu, H. Ji, Chin. Chem. Lett. 30 (2019) 2191–2195. doi: 10.1016/j.cclet.2019.09.031
6. [6]
  X. Lei, M. You, F. Pan, et al., Chin. Chem. Lett. 30 (2019) 2216–2220. doi: 10.1016/j.cclet.2019.05.039
7. [7]
  J. Li, Y.J. Li, Z.K. Xiong, et al., Chin. Chem. Lett. 30 (2019) 2139–2146. doi: 10.1016/j.cclet.2019.04.057
8. [8]
  L. Chen, M. Tang, C. Chen, et al., Environ. Sci. Technol. 51 (2017) 12663–12671. doi: 10.1021/acs.est.7b03705
9. [9]
  W. Deng, H. Zhao, F. Pan, et al., Environ. Sci. Technol. 51 (2017) 13372–13379. doi: 10.1021/acs.est.7b04206
10. [10]
  R. Dewil, D. Mantzavinos, I. Poulios, M.A. Rodrigo, J. Environ. Manag. 195 (2017) 93–99. doi: 10.1016/j.jenvman.2017.04.010
11. [11]
  Z. Wang, F. Bai, L. Cao, et al., Chin. Chem. Lett. 33 (2022) 4766–4770. doi: 10.1016/j.cclet.2022.01.003
12. [12]
  H. Dong, G. Wei, W. Fan, et al., Chemosphere 196 (2018) 593–597. doi: 10.1016/j.chemosphere.2017.12.194
13. [13]
  L. Chen, X. Peng, J. Liu, J. Li, F. Wu, Ind. Eng. Chem. Res. 51 (2012) 13632–13638. doi: 10.1021/ie3020389
14. [14]
  D. Zhou, L. Chen, J. Li, F. Wu, Chem. Eng. J. 346 (2018) 726–738. doi: 10.1016/j.cej.2018.04.016
15. [15]
  P. Xie, Y. Guo, Y. Chen, et al., Chem. Eng. J. 314 (2017) 240–248. doi: 10.1016/j.cej.2016.12.094
16. [16]
  Y. Yuan, S. Yang, D. Zhou, F. Wu, J. Hazard. Mater. 307 (2016) 294–301. doi: 10.1016/j.jhazmat.2016.01.012
17. [17]
  B. Jiang, S. Xin, Y. Liu, et al., J. Hazard. Mater. 343 (2018) 1–9. doi: 10.1016/j.jhazmat.2017.09.015
18. [18]
  B. Jiang, X. Wang, Y. Liu, et al., J. Hazard. Mater. 304 (2016) 457–466. doi: 10.1016/j.jhazmat.2015.11.011
19. [19]
  L. Chen, T. Luo, S. Yang, et al., Environ. Chem. Lett. 16 (2018) 599–603. doi: 10.1007/s10311-017-0696-1
20. [20]
  Y. Yuan, D. Zhao, J. Li, et al., Catal. Today 313 (2018) 155–160. doi: 10.1016/j.cattod.2017.12.004
21. [21]
  Z. Liu, S. Yang, Y. Yuan, et al., J. Hazard. Mater. 324 (2017) 583–592. doi: 10.1016/j.jhazmat.2016.11.029
22. [22]
  Q. Pang, G. Liao, X. Hu, Q. Zhang, Z. Xu, J. Inorg. Mater. 34 (2019) 219–224. doi: 10.15541/jim20180379
23. [23]
  V. Vaiano, O. Sacco, M. Matarangolo, Catal. Today 315 (2018) 230–236. doi: 10.1016/j.cattod.2018.02.002
24. [24]
  Q. Li, Y. Liu, Z. Wan, et al., Chin. Chem. Lett. 33 (2022) 3835–3841. doi: 10.1016/j.cclet.2021.12.025
25. [25]
  Z. Wang, Z. Lin, S. Shen, W. Zhong, S. Cao, Chin. J. Catal. 42 (2021) 710–730. doi: 10.1016/S1872-2067(20)63698-1
26. [26]
  P. Xia, S. Cao, B. Zhu, et al., Angew. Chem. Int. Ed. 59 (2020) 5218–5225. doi: 10.1002/anie.201916012
27. [27]
  J. Qi, X. Yang, P. Pan, et al., Environ. Sci. Technol. 56 (2022) 5200–5212. doi: 10.1021/acs.est.1c08806
28. [28]
  H. Wang, Q. Gao, H. Li, et al., Chem. Eng. J. 368 (2019) 377–389. doi: 10.1016/j.cej.2019.02.124
29. [29]
  H. Li, Q. Gao, G. Wang, et al., Chem. Eng. J. 392 (2020) 123819. doi: 10.1016/j.cej.2019.123819
30. [30]
  I. Rabani, R. Zafar, K. Subalakshmi, et al., J. Hazard. Mater. 407 (2021) 124360. doi: 10.1016/j.jhazmat.2020.124360
31. [31]
  H. Zhang, J. Wang, X. Zhang, B. Li, X. Cheng, Chem. Eng. J. 369 (2019) 834–844. doi: 10.1016/j.cej.2019.03.132
32. [32]
  L. Xu, Q. Jiang, Z. Xiao, Angew. Chem. Int. Ed. 55 (2016) 5277–5281. doi: 10.1002/anie.201600687
33. [33]
  S. Liu, J. Huang, L. Cao, et al., Mater. Sci. Semicond. Proc. 25 (2014) 106–111. doi: 10.1016/j.mssp.2013.09.021
34. [34]
  J. Zhong, A. Wang, G. Li, et al., J. Mater. Chem. A 22 (2012) 5656–5665. doi: 10.1039/c2jm15863a
35. [35]
  Q. Wang, Y. Cui, R. Huang, et al., Chem. Eng. J. 383 (2020) 123142. doi: 10.1016/j.cej.2019.123142
36. [36]
  Y. Shieh, Y. Chang, Thin Solid. Films 518 (2010) 7464–7467. doi: 10.1016/j.tsf.2010.05.025
37. [37]
  R. Tang, S. Zhou, Z. Yuan, L. Yin, Adv. Funct. Mater. 27 (2017) 1701102. doi: 10.1002/adfm.201701102
38. [38]
  J. Yang, H. Liu, W.N. Martens, R.L. Frost, J. Phy. Chem. C 114 (2010) 111–119. doi: 10.1021/jp908548f
39. [39]
  Q. Yang, H. Choi, D.D. Dionysiou, Appl. Catal. B 74 (2007) 170–178. doi: 10.1016/j.apcatb.2007.02.001
40. [40]
  X. Dong, B. Ren, X. Zhang, et al., Appl. Catal. B 272 (2020) 118971. doi: 10.1016/j.apcatb.2020.118971
41. [41]
  G. Yang, Y. Jiao, H. Yan, Adv. Mater. 32 (2020) 2000455. doi: 10.1002/adma.202000455
42. [42]
  M. Anpo, M. Takeuchi, J. Catal. 216 (2003) 505–516. doi: 10.1016/S0021-9517(02)00104-5
43. [43]
  D. Barreca, C. Massignan, S. Daolio, et al., Chem. Mater. 13 (2001) 588–593. doi: 10.1021/cm001041x
44. [44]
  C. Gao, Q. Meng, K. Zhao, et al., Adv. Mater. 28 (2016) 6485–6490. doi: 10.1002/adma.201601387
45. [45]
  Q. Chen, L. Chen, J. Qi, et al., Chin. Chem. Lett. 30 (2019) 1214–1218. doi: 10.1016/j.cclet.2019.03.002
46. [46]
  X. Tao, P. Pan, T. Huang, et al., Chem. Eng. J. 395 (2020) 125186. doi: 10.1016/j.cej.2020.125186
47. [47]
  S. Guo, H. Tang, L. You, et al., Chin. Chem. Lett. 32 (2021) 2828–2832. doi: 10.1016/j.cclet.2021.01.019
48. [48]
  F. Chen, Q. Yang, F. Yao, et al., Chem. Eng. J. 355 (2019) 624–636. doi: 10.1016/j.cej.2018.08.182
49. [49]
  Y. Wang, S. Indrawirawan, X. Duan, Chem. Eng. J. 266 (2015) 12–20. doi: 10.1016/j.cej.2014.12.066
50. [50]
  Y. Chen, G. Zhang, H. Liu, J. Qu, Angew. Chem. Int. Ed. 58 (2019) 8134–8138. doi: 10.1002/anie.201903531
51. [51]
  C. Diaz-Uribe, M. Daza, F. Martinez, J. Photochem. Photobiol. A 215 (2010) 172–178. doi: 10.1016/j.jphotochem.2010.08.013
52. [52]
  L. Yang, L.E. Yu, M.B. Ray, Water Res. 42 (2008) 3480–3488. doi: 10.1016/j.watres.2008.04.023
53. [53]
  X. Yu, D. Cabooter, R. Dewil, Sci. Total Environ. 688 (2019) 65–74. doi: 10.1016/j.scitotenv.2019.06.210
54. [54]
  M. Entezari, H. Godini, A. Sheikhmohammadi, A. Esrafili, J. Water Process Eng. 32 (2019) 100983. doi: 10.1016/j.jwpe.2019.100983
1. [1]
  Teng Wang , Jiachun Cao , Juan Li , Didi Li , Zhimin Ao . A novel photocatalytic mechanism of volatile organic compounds degradation on BaTiO₃ under visible light: Photo-electrons transfer from photocatalyst to pollutant. Chinese Chemical Letters, 2025, 36(3): 110078-. doi: 10.1016/j.cclet.2024.110078
2. [2]
  Haiyan Yin , Abdusalam Ablez , Zhuangzhuang Wang , Weian Li , Yanqi Wang , Qianqian Hu , Xiaoying Huang . Novel open-framework chalcogenide photocatalysts: Cobalt cocatalyst valence state modulating critical charge transfer pathways towards high-efficiency hydrogen evolution. Chinese Journal of Structural Chemistry, 2025, 44(4): 100560-100560. doi: 10.1016/j.cjsc.2025.100560
3. [3]
  Shu-Ran Xu , Fang-Xing Xiao . Metal halide perovskites quantum dots: Synthesis, and modification strategies for solar CO2 conversion. Chinese Journal of Structural Chemistry, 2023, 42(12): 100173-100173. doi: 10.1016/j.cjsc.2023.100173
4. [4]
  Haibo Ye , Qianyu Li , Juan Li , Didi Li , Zhimin Ao . Review on the abiotic degradation of biodegradable plastic poly(butylene adipate-terephthalate): Mechanisms and main factors of the degradation. Chinese Chemical Letters, 2025, 36(1): 109861-. doi: 10.1016/j.cclet.2024.109861
5. [5]
  Yuchen Wang , Yaoyu Liu , Xiongfei Huang , Guanjie He , Kai Yan . Fe nanoclusters anchored in biomass waste-derived porous carbon nanosheets for high-performance supercapacitor. Chinese Chemical Letters, 2024, 35(8): 109301-. doi: 10.1016/j.cclet.2023.109301
6. [6]
  Zhen Shi , Wei Jin , Yuhang Sun , Xu Li , Liang Mao , Xiaoyan Cai , Zaizhu Lou . Interface charge separation in Cu2CoSnS4/ZnIn2S4 heterojunction for boosting photocatalytic hydrogen production. Chinese Journal of Structural Chemistry, 2023, 42(12): 100201-100201. doi: 10.1016/j.cjsc.2023.100201
7. [7]
  Xiaotao Jin , Yanlan Wang , Yingping Huang , Di Huang , Xiang Liu . Percarbonate activation catalyzed by nanoblocks of basic copper molybdate for antibiotics degradation: High performance, degradation pathways and mechanism. Chinese Chemical Letters, 2024, 35(10): 109499-. doi: 10.1016/j.cclet.2024.109499
8. [8]
  Yihu Ke , Shuai Wang , Fei Jin , Guangbo Liu , Zhiliang Jin , Noritatsu Tsubaki . Charge transfer optimization: Role of Cu-graphdiyne/NiCoMoO4 S-scheme heterojunction and Ohmic junction. Chinese Journal of Structural Chemistry, 2024, 43(12): 100458-100458. doi: 10.1016/j.cjsc.2024.100458
9. [9]
  Chunxiu Yu , Zelin Wu , Hongle Shi , Lingyun Gu , Kexin Chen , Chuan-Shu He , Yang Liu , Heng Zhang , Peng Zhou , Zhaokun Xiong , Bo Lai . Insights into the electron transfer mechanisms of peroxydisulfate activation by modified metal-free acetylene black for degradation of sulfisoxazole. Chinese Chemical Letters, 2024, 35(8): 109334-. doi: 10.1016/j.cclet.2023.109334
10. [10]
  Qiang Zhang , Weiran Gong , Huinan Che , Bin Liu , Yanhui Ao . S doping induces to promoted spatial separation of charge carriers on carbon nitride for efficiently photocatalytic degradation of atrazine. Chinese Journal of Structural Chemistry, 2023, 42(12): 100205-100205. doi: 10.1016/j.cjsc.2023.100205
11. [11]
  Xingmin Chen , Yunyun Wu , Yao Tang , Peishen Li , Shuai Gao , Qiang Wang , Wen Liu , Sihui Zhan . Construction of Z-scheme Cu-CeO₂/BiOBr heterojunction for enhanced photocatalytic degradation of sulfathiazole. Chinese Chemical Letters, 2024, 35(7): 109245-. doi: 10.1016/j.cclet.2023.109245
12. [12]
  Yun-Xin Huang , Lin-Qian Yu , Ke-Yu Chen , Hao Wang , Shou-Yan Zhao , Bao-Cheng Huang , Ren-Cun Jin . Biochar with self-doped N to activate peroxymonosulfate for bisphenol-A degradation via electron transfer mechanism: The active edge graphitic N site. Chinese Chemical Letters, 2024, 35(9): 109437-. doi: 10.1016/j.cclet.2023.109437
13. [13]
  Xin Jiang , Han Jiang , Yimin Tang , Huizhu Zhang , Libin Yang , Xiuwen Wang , Bing Zhao . g-C₃N₄/TiO_2-X heterojunction with high-efficiency carrier separation and multiple charge transfer paths for ultrasensitive SERS sensing. Chinese Chemical Letters, 2024, 35(10): 109415-. doi: 10.1016/j.cclet.2023.109415
14. [14]
  Yuan Teng , Zichun Zhou , Jinghua Chen , Siying Huang , Hongyan Chen , Daibin Kuang . Dual atom-bridge effect promoting interfacial charge transfer in 2D/2D Cs₃Bi₂Br₉/BiOBr epitaxial heterojunction for efficient photocatalysis. Chinese Chemical Letters, 2025, 36(2): 110430-. doi: 10.1016/j.cclet.2024.110430
15. [15]
  Yadan Luo , Hao Zheng , Xin Li , Fengmin Li , Hua Tang , Xilin She . 调节O,S共掺杂C₃N₄中的活性氧生成以促进光催化降解微塑料. Acta Physico-Chimica Sinica, 2025, 41(6): 100052-. doi: 10.1016/j.actphy.2025.100052
16. [16]
  Chunyan Yang , Qiuyu Rong , Fengyin Shi , Menghan Cao , Guie Li , Yanjun Xin , Wen Zhang , Guangshan Zhang . Rationally designed S-scheme heterojunction of BiOCl/g-C₃N₄ for photodegradation of sulfamerazine: Mechanism insights, degradation pathways and DFT calculation. Chinese Chemical Letters, 2024, 35(12): 109767-. doi: 10.1016/j.cclet.2024.109767
17. [17]
  Xing Xiao , Yunling Jia , Wanyu Hong , Yuqing He , Yanjun Wang , Lizhi Zhao , Huiqin An , Zhen Yin . Sulfur-defective ZnIn2S4 nanosheets decorated by TiO2 nanosheets with exposed {001} facets to accelerate charge transfer for efficient photocatalytic hydrogen evolution. Chinese Journal of Structural Chemistry, 2024, 43(12): 100474-100474. doi: 10.1016/j.cjsc.2024.100474
18. [18]
  Guixu Pan , Zhiling Xia , Ning Wang , Hejia Sun , Zhaoqi Guo , Yunfeng Li , Xin Li . Preparation of high-efficient donor-π-acceptor system with crystalline g-C3N4 as charge transfer module for enhanced photocatalytic hydrogen evolution. Chinese Journal of Structural Chemistry, 2024, 43(12): 100463-100463. doi: 10.1016/j.cjsc.2024.100463
19. [19]
  Zhinan GUO , Junli WANG , Qiang ZHAO , Zhifang JIA , Zuopeng LI , Kewei WANG , Yong GUO . Cu₂O/Bi₂CrO₆ Z-scheme heterojunction: Construction and photocatalytic degradation properties for tetracycline. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 741-752. doi: 10.11862/CJIC.20240403
20. [20]
  Jianyin He , Liuyun Chen , Xinling Xie , Zuzeng Qin , Hongbing Ji , Tongming Su . ZnCoP/CdLa₂S₄肖特基异质结的构建促进光催化产氢. Acta Physico-Chimica Sinica, 2024, 40(11): 2404030-. doi: 10.3866/PKU.WHXB202404030

Get Citation

PDF

XML

Metrics

PDF Downloads(3)
Abstract views(395)
HTML views(36)

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

Constructing heterojunction interface of Co3O4/TiO2 for efficiently accelerating acetaminophen degradation via photocatalytic activation of sulfite

Metrics

通讯作者: 陈斌, bchen63@163.com

Constructing heterojunction interface of Co₃O₄/TiO₂ for efficiently accelerating acetaminophen degradation via photocatalytic activation of sulfite