Citation: Yun-Long SUN, Jun-Heng HUANG. Improvement of the Selectivity for Hydrogen Peroxide Production via the Synergy of TiO₂ and Graphene[J]. Chinese Journal of Structural Chemistry, ;2022, 41(3): 220308. doi: 10.14102/j.cnki.0254-5861.2011-3299 shu

Improvement of the Selectivity for Hydrogen Peroxide Production via the Synergy of TiO₂ and Graphene

Yun-Long SUN ^{a, b} ,
Jun-Heng HUANG ^a,,

a.
CAS Key Laboratory of Design and Assembly of Functional Nano-structures, Fujian Provincial Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
b.
Fuzhou University, Fuzhou 350108, China

Corresponding author: Jun-Heng HUANG, huangjunheng@fjirsm.ac.cn
Received Date: 28 June 2021
Accepted Date: 14 September 2021

Fund Project: the Natural Science Foundation of Fujian Province 2020J05079

Figures(5)

To replace the four-electron transferred pathway of oxygen reduction reaction (ORR) by two-electron transferred pathway of ORR (2e^- ORR) is desirable for the production of hydrogen peroxide with added-value. The development of electrocatalysts with high selectivity toward 2e^- ORR is of great interest but it is still a challenge. Here, we synthesized the graphene-supported titanium dioxide nanocomposite as the 2e^- ORR catalysts by a combinative process of hydrothermal methods and calcination. Due to the synergistic effect between the graphene with high conductivity and the titanium dioxide with defect sites, the composite TiO₂/graphene exhibits the improved selectivity (up to 90%) for oxygen converting into hydrogen peroxide.
- oxygen reduction reaction,
- hydrogen peroxide,
- titanium dioxide,
- graphene,
- electrochemistry
1. [1]
  Xia, C.; Xia, Y.; Zhu, P.; Fan, L.; Wang, H. Direct electrosynthesis of pure aqueous H₂O₂ solutions up to 20% by weight using a solid electrolyte. Science 2019, 366, 226–231. doi: 10.1126/science.aay1844
2. [2]
  Ciriminna, R.; Albanese, L.; Meneguzzo, F.; Pagliaro, M. Hydrogen peroxide: a key chemical for today's sustainable development. ChemSuschem. 2016, 9, 3374–3381. doi: 10.1002/cssc.201600895
3. [3]
  Campos-Martin, J. M.; Blanco-Brieva, G.; Fierro, J. L. Hydrogen peroxide synthesis: an outlook beyond the anthraquinone process. Angew. Chem. Int. Ed. 2006, 45, 6962–6984. doi: 10.1002/anie.200503779
4. [4]
  Yang, S.; Verdaguer-Casadevall, A.; Arnarson, L.; Silvioli, L.; Čolić, V.; Frydendal, R.; Rossmeisl, J.; Chorkendorff, I.; Stephens, I. E. L. Toward the decentralized electrochemical production of H₂O₂: a focus on the catalysis. ACS Catal. 2018, 8, 4064–4081. doi: 10.1021/acscatal.8b00217
5. [5]
  Siahrostami, S.; Villegas, S. J.; Bagherzadeh Mostaghimi, A. H.; Back, S.; Farimani, A. B.; Wang, H.; Persson, K. A.; Montoya, J. A review on challenges and successes in atomic-scale design of catalysts for electrochemical synthesis of hydrogen peroxide. ACS Catal. 2020, 10, 7495–7511. doi: 10.1021/acscatal.0c01641
6. [6]
  Stamenkovic, V.; Mun, B. S.; Mayrhofer, K. J. J.; Ross, P. N.; Markovic, N. M.; Rossmeisl, J.; Greeley, J.; Nørskov, J. K. Changing the activity of electrocatalysts for oxygen reduction by tuning the surface electronic structure. Angew. Chem. Int. Ed. 2006, 45, 2897–2901. doi: 10.1002/anie.200504386
7. [7]
  Viswanathan, V.; Hansen, H. A.; Rossmeisl, J.; Nørskov, J. K. Unifying the 2e and 4e reduction of oxygen on metal surfaces. J. Phys. Chem. Lett. 2012, 3, 2948–2951. doi: 10.1021/jz301476w
8. [8]
  Siahrostami, S.; Verdaguer-Casadevall, A.; Karamad, M.; Deiana, D.; Malacrida, P.; Wickman, B.; Escudero-Escribano, M.; Paoli, E. A.; Frydendal, R.; Hansen, T. W.; Chorkendorff, I.; Stephens, I. E. L.; Rossmeisl, J. Enabling direct H₂O₂ production through rational electrocatalyst design. Nat. Mater. 2013, 12, 1137–1143. doi: 10.1038/nmat3795
9. [9]
  Kim, J. H.; Kim, Y. T.; Joo, S. H. Electrocatalyst design for promoting two-electron oxygen reduction reaction: isolation of active site atoms. Curr. Opin. Electrochem. 2020, 2, 109–116.
10. [10]
  Verdaguer, C. A.; Deiana, D.; Karamad, M.; Siahrostami, S.; Malacrida, P.; Hansen, T. W.; Rossmeisl, J.; Chorkendorff, I.; Stephens, I. E. L. Trends in the electrochemical synthesis of H₂O₂: enhancing activity and selectivity by electrocatalytic site engineering. Nano Lett. 2014, 14, 1603–1608. doi: 10.1021/nl500037x
11. [11]
  Shen, R.; Chen, W.; Peng, Q.; Lu, S.; Zheng, L.; Cao, X.; Wang, Y.; Zhu, W.; Zhang, J.; Zhuang, Z.; Chen, C.; Wang, D.; Li, Y. High-concentration single atomic Pt sites on hollow CuS_x for selective O₂ reduction to H₂O₂ in acid solution. Chem. 2019, 5, 2099–2110. doi: 10.1016/j.chempr.2019.04.024
12. [12]
  Pang, Y.; Wang, K.; Xie, H.; Sun, Y.; Titirici, M. M.; Chai, G. L. Mesoporous carbon hollow spheres as efficient electrocatalysts for oxygen reduction to hydrogen peroxide in neutral electrolytes. ACS Catal. 2020, 10, 7434–7442 doi: 10.1021/acscatal.0c00584
13. [13]
  Chen, S.; Chen, Z.; Siahrostami, S.; Kim, T. R.; Nordlund, D.; Sokaras, D.; Nowak, S.; To, J. W.; Higgins, D.; Sinclair, R. Defective carbon-based materials for the electrochemical synthesis of hydrogen peroxide. ACS Sustain. Chem. Eng. 2018, 6, 311–317. doi: 10.1021/acssuschemeng.7b02517
14. [14]
  Tang, C.; Jiao, Y.; Shi, B. Y.; Liu, J. N.; Xie, Z. H.; Chen, X.; Zhang, Q. Coordination tunes selectivity: two-electron oxygen reduction on high-loading molybdenum single-atom catalysts. Angew. Chem. Int. Ed. 2020, 59, 9171–9176. doi: 10.1002/anie.202003842
15. [15]
  Kulkarni, A.; Siahrostami, S.; Patel, A.; Nørskov, J. K. Understanding catalytic activity trends in the oxygen reduction reaction. Chem. Rev. 2018, 118, 2302–2312. doi: 10.1021/acs.chemrev.7b00488
16. [16]
  Liu, X.; Dai, L. Carbon-based metal-free catalysts. Nat. Rev. Mater. 2016, 1, 1–12.
17. [17]
  Lu, Z.; Chen, G.; Siahrostami, S.; Chen, Z.; Liu, K.; Xie, J.; Liao, L.; Wu, T.; Lin, D.; Liu, Y.; Jaramillo, T. F.; Nørskov, J. K.; Cui, Y. High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials. Nat. Catal. 2018, 1, 156–162. doi: 10.1038/s41929-017-0017-x
18. [18]
  Jiang, K.; Zhao, J. J.; Wang, H. T. Catalyst design for electrochemical oxygen reduction toward hydrogen peroxide. Adv. Funct. Mater. 2020, 30, 2003321. doi: 10.1002/adfm.202003321
19. [19]
  Kim, H. W.; Ross, M. B.; Kornienko, N.; Zhang, L.; Guo, J.; Yang, P.; McCloskey, B. D. Efficient hydrogen peroxide generation using reduced graphene oxide-based oxygen reduction electrocatalysts. Nat. Catal. 2018, 1, 282–290. doi: 10.1038/s41929-018-0044-2
20. [20]
  Zhou, J.; An, X. Q.; Lan, C. H.; Liu, H. J.; Qu, J. H. New insights into the surface-dependent activity of graphitic felts for the electro-generation of H₂O₂. Appl. Surf. Sci. 2020, 509, 144875–144900. doi: 10.1016/j.apsusc.2019.144875
21. [21]
  Cui, Y. Q.; Xu, J. X.; Wang, M. L.; Guan, L. H. Surface oxidation of single-walled-carbon-nanotubes with enhanced oxygen electroreduction activity and selectivity. J. Struct. Chem. 2021, 40, 533–539.
22. [22]
  Wang, K.; Pang, Y. Y.; Huan, X.; Sun, Y.; Chai, G. L. Synergistic effect of Ta₂O₅/FC composites for effective electrosynthesis of hydrogen peroxide from O₂ reduction. J. Struct. Chem. 2021, 40, 225–232.
23. [23]
  Pei, D. N.; Gong, L.; Zhang, A. Y.; Zhang, X.; Chen, J. J.; Mu, Y.; Yu, H. Q. Defective titanium dioxide single crystals exposed by high-energy {001} facets for efficient oxygen reduction. Nat. Commun. 2015, 6, 1–10.
24. [24]
  Chen, J.; Yao, B.; Li, C.; Shi, G. An improved Hummers method for eco-friendly synthesis of graphene oxide. Carbon 2013, 64, 225–229. doi: 10.1016/j.carbon.2013.07.055
25. [25]
  Kim, H. W.; Bukas, V. J.; Park, H.; Park, S.; Diederichsen, K. M.; Lim, J.; Cho, Y. H.; Kim, J.; Kim, W.; Han, T. H.; Voss, J.; Luntz, A. C.; McCloskey, B. D. Mechanisms of two-electron and four-electron electrochemical oxygen reduction reactions at nitrogen-doped reduced graphene oxide. ACS Catal. 2019, 10, 852–863.
26. [26]
  Lu, Z.; Chen, G.; Siahrostami, S.; Chen, Z.; Liu, K.; Xie, J.; Liao, L.; Wu, T.; Lin, D.; Liu, Y.; Jaramillo, T. F.; Nørskov, J. K.; Cui, Y. High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials. Nat. Catal. 2018, 1, 156–162. doi: 10.1038/s41929-017-0017-x
27. [27]
  Sun, Y.; Sinev, I.; Ju, W.; Bergmann, A.; Dresp, S.; Kühl, S.; Spoeri, C.; Schmies, H.; Wang, H.; Bernsmeier, D.; Paul, B.; Schmack, R.; Kraehnert. Efficient electrochemical hydrogen peroxide production from molecular oxygen on nitrogen-doped mesoporous carbon catalysts. ACS Catal. 2018, 8, 2844–2856. doi: 10.1021/acscatal.7b03464
28. [28]
  Li, C. Y.; Shi, Y. Y.; Zhang, Z. C.; Ni, J.; Wang, X. Y.; Lin, J. X.; Lin, B. Y.; Jiang, L. L. Improving the ammonia synthesis activity of Ru/CeO₂ through enhancement of the metal-support interaction. J. Energy Chem. 2021, 60, 403–409. doi: 10.1016/j.jechem.2021.01.031
29. [29]
  Sun, Y. Y.; Sinev, I.; Ju, W.; Bergmann, A.; Dresp, S.; Kühl, S.; Spöri, C.; Schmies, H.; Wang, H.; Bernsmeier, D.; Paul, B.; Schmack, R.; Kraehnert, R.; Cuenya, B. R.; Strasser P. Efficient electrochemical hydrogen peroxide production from molecular oxygen on nitrogen-doped mesoporous carbon catalysts. ACS Catal. 2018, 8, 2844–2856. doi: 10.1021/acscatal.7b03464
30. [30]
  Chisaka, M.; Ishihara, A.; Suito, K.; Ota, K. I.; Muramoto, H. Oxygen reduction reaction activity of nitrogen-doped titanium oxide in acid media. Electrochim. Acta 2013, 88, 697–707. doi: 10.1016/j.electacta.2012.10.137
31. [31]
  García-Serna, J.; Moreno, T.; Biasi, P.; Cocero, M. J.; Mikkola, J. P.; Salmi, T. O. Engineering in direct synthesis of hydrogen peroxide: targets, reactors and guidelines for operational conditions. Green Chem. 2014, 16, 2320–2343 doi: 10.1039/c3gc41600c
32. [32]
  Pan, Z.; Wang, K.; Wang, Y.; Tsiakaras, P.; Song, S. In-situ electrosynthesis of hydrogen peroxide and wastewater treatment application: a novel strategy for graphite felt activation. Appl. Catal. B-Environ. 2018, 237, 392–400. doi: 10.1016/j.apcatb.2018.05.079
33. [33]
  Sun, Z. P.; Sheng, L.; Gong, H.; Song, L.; Jiang, X. L.; Wang, S. Y.; Meng, X. G.; Wang, T.; He, J. P. Electrocatalytic synthesis of hydrogen peroxide over Au/TiO₂ and electrochemical trace of OOH* intermediate. Chem. -Asian J. 2020, 15, 4280–4285. doi: 10.1002/asia.202001089
34. [34]
  Miao, F.; Gao, M. M.; Yu, X.; Xiao, P. W.; Wang, M.; Wang, Y. K.; Wang, S. G.; Wang, X. H. TiO₂ electrocatalysis via three-electron oxygen reduction for highly efficient generation of hydroxyl radicals. Electrochem. Commun. 2020, 113, 106687–106707. doi: 10.1016/j.elecom.2020.106687
35. [35]
  Lazarte, J. P. L.; Dipasupi, R. C.; Pasco, G. Y. S.; Eusebio, R. C P.; Orbecido, A. H.; Doong, R. A.; Liza, B. P. Synthesis of reduced graphene oxide/titanium dioxide nanotubes (RGO/TNT) composites as an electrical double layer capacitor. Nanomaterials 2018, 8, 934–949. doi: 10.3390/nano8110934
36. [36]
  Froschl, T.; Hormann, U.; Kubiak, P.; Kucerova, G.; Pfanzelt, M.; Weiss, C. K.; Behm, R. J.; Husing, N.; Kaiser, U.; Landfesterd, K.; Wohlfahrt-Mehrens, M. High surface area crystalline titanium dioxide: potential and limits in electrochemical energy storage and catalysis. Chem. Soc. Rev. 2012, 41, 5313–5360. doi: 10.1039/c2cs35013k
37. [37]
  Sun, Y. Y.; Silvioli, L.; Sahraie, N. R.; Wen, J.; Li, J. K.; Zitolo, A.; Li, S.; Bagger, A.; Aranarson, L.; Wang, X. L.; Moeller, T.; Bernsmeier, D.; Rossmeisl, J.; Jaouen, F.; Strasser, P. Activity-selectivity trends in the electrochemical production of hydrogen peroxide over single-site metal-nitrogen-carbon catalysts. J. Am. Chem. Soc. 2019, 141, 12372–12381. doi: 10.1021/jacs.9b05576
38. [38]
  Jung, E.; Shin, H.; Lee, B. H.; Efremov, V.; Lee, S. Atomic-level tuning of Co–N–C catalyst for high-performance electrochemical H₂O₂ production. Nat. Mater. 2020, 19, 436–442. doi: 10.1038/s41563-019-0571-5
39. [39]
  Wang, Y. L.; Shi, R.; Shang, L.; Waterhouse, G. I. N.; Zhao, J. Q.; Zhang, Q. H.; Gu, L.; Zhang, T. R. High-efficiency oxygen reduction to hydrogen peroxide catalyzed by nickel single-atom catalysts with tetradentate N₂O₂ coordination in a three-phase flow cell. Angew. Chem. Int. Ed. 2020, 59, 13057–13062. doi: 10.1002/anie.202004841
40. [40]
  Ma, F. H.; Wang, S. H.; Liang, X. Z.; Wang, C. Ni₃B as a highly efficient and selective catalyst for the electrosynthesis of hydrogen peroxide. Appl. Catal. B-Environ. 2020, 279, 119371–119379. doi: 10.1016/j.apcatb.2020.119371
41. [41]
  Chen, S. C.; Chen, Z. H.; Siahrostami, S. Defective carbon-based materials for the electrochemical synthesis of hydrogen peroxide. ACS Sustain. Chem. Eng. 2018, 6, 311–317. doi: 10.1021/acssuschemeng.7b02517
1. [1]
  Xiaoxia WANG , Ya'nan GUO , Feng SU , Chun HAN , Long SUN . Synthesis, structure, and electrocatalytic oxygen reduction reaction properties of metal antimony-based chalcogenide clusters. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1201-1208. doi: 10.11862/CJIC.20230478
2. [2]
  Jie XIE , Hongnan XU , Jianfeng LIAO , Ruoyu CHEN , Lin SUN , Zhong JIN . Nitrogen-doped 3D graphene-carbon nanotube network for efficient lithium storage. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1840-1849. doi: 10.11862/CJIC.20240216
3. [3]
  Ruiqing LIU , Wenxiu LIU , Kun XIE , Yiran LIU , Hui CHENG , Xiaoyu WANG , Chenxu TIAN , Xiujing LIN , Xiaomiao FENG . Three-dimensional porous titanium nitride as a highly efficient sulfur host. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 867-876. doi: 10.11862/CJIC.20230441
4. [4]
  Hongyi LI , Aimin WU , Liuyang ZHAO , Xinpeng LIU , Fengqin CHEN , Aikui LI , Hao HUANG . Effect of Y(PO₃)₃ double-coating modification on the electrochemical properties of Li[Ni_0.8Co_0.15Al_0.05]O₂. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1320-1328. doi: 10.11862/CJIC.20230480
5. [5]
  Haijing Cui , Weihao Zhu , Chuning Yue , Ming Yang , Wenzhi Ren , Aiguo Wu . Recent progress of ultrasound-responsive titanium dioxide sonosensitizers in cancer treatment. Chinese Chemical Letters, 2024, 35(10): 109727-. doi: 10.1016/j.cclet.2024.109727
6. [6]
  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
7. [7]
  Kunsong Hu , Yulong Zhang , Jiayi Zhu , Jinhua Mai , Gang Liu , Manoj Krishna Sugumar , Xinhua Liu , Feng Zhan , Rui Tan . Nano-engineered catalysts for high-performance oxygen reduction reaction. Chinese Chemical Letters, 2024, 35(10): 109423-. doi: 10.1016/j.cclet.2023.109423
8. [8]
  Jing Cao , Dezheng Zhang , Bianqing Ren , Ping Song , Weilin Xu . Mn incorporated RuO₂ nanocrystals as an efficient and stable bifunctional electrocatalyst for oxygen evolution reaction and hydrogen evolution reaction in acid and alkaline. Chinese Chemical Letters, 2024, 35(10): 109863-. doi: 10.1016/j.cclet.2024.109863
9. [9]
  Zhipeng Wan , Hao Xu , Peng Wu . Selective oxidation using in-situ generated hydrogen peroxide over titanosilicates. Chinese Journal of Structural Chemistry, 2024, 43(6): 100298-100298. doi: 10.1016/j.cjsc.2024.100298
10. [10]
  Qiang Cao , Xue-Feng Cheng , Jia Wang , Chang Zhou , Liu-Jun Yang , Guan Wang , Dong-Yun Chen , Jing-Hui He , Jian-Mei Lu . Graphene from microwave-initiated upcycling of waste polyethylene for electrocatalytic reduction of chloramphenicol. Chinese Chemical Letters, 2024, 35(4): 108759-. doi: 10.1016/j.cclet.2023.108759
11. [11]
  Yuan Dong , Mutian Ma , Zhenyang Jiao , Sheng Han , Likun Xiong , Zhao Deng , Yang Peng . Effect of electrolyte cation-mediated mechanism on electrocatalytic carbon dioxide reduction. Chinese Chemical Letters, 2024, 35(7): 109049-. doi: 10.1016/j.cclet.2023.109049
12. [12]
  Guan-Nan Xing , Di-Ye Wei , Hua Zhang , Zhong-Qun Tian , Jian-Feng Li . Pd-based nanocatalysts for oxygen reduction reaction: Preparation, performance, and in-situ characterization. Chinese Journal of Structural Chemistry, 2023, 42(11): 100021-100021. doi: 10.1016/j.cjsc.2023.100021
13. [13]
  Min Song , Qian Zhang , Tao Shen , Guanyu Luo , Deli Wang . Surface reconstruction enabled o-PdTe@Pd core-shell electrocatalyst for efficient oxygen reduction reaction. Chinese Chemical Letters, 2024, 35(8): 109083-. doi: 10.1016/j.cclet.2023.109083
14. [14]
  Fabrice Nelly Habarugira , Ducheng Yao , Wei Miao , Chengcheng Chu , Zhong Chen , Shun Mao . Synergy of sodium doping and nitrogen defects in carbon nitride for promoted photocatalytic synthesis of hydrogen peroxide. Chinese Chemical Letters, 2024, 35(8): 109886-. doi: 10.1016/j.cclet.2024.109886
15. [15]
  Tiantian Li , Ruochen Jin , Bin Wu , Dongming Lan , Yunjian Ma , Yonghua Wang . A novel insight of enhancing the hydrogen peroxide tolerance of unspecific peroxygenase from Daldinia caldariorum based on structure. Chinese Chemical Letters, 2024, 35(4): 108701-. doi: 10.1016/j.cclet.2023.108701
16. [16]
  Jin Long , Xingqun Zheng , Bin Wang , Chenzhong Wu , Qingmei Wang , Lishan Peng . Improving the electrocatalytic performances of Pt-based catalysts for oxygen reduction reaction via strong interactions with single-CoN₄-rich carbon support. Chinese Chemical Letters, 2024, 35(5): 109354-. doi: 10.1016/j.cclet.2023.109354
17. [17]
  Peng Wang , Daijie Deng , Suqin Wu , Li Xu . Cobalt-based deep eutectic solvent modified nitrogen-doped carbon catalyst for boosting oxygen reduction reaction in zinc-air batteries. Chinese Journal of Structural Chemistry, 2024, 43(1): 100199-100199. doi: 10.1016/j.cjsc.2023.100199
18. [18]
  Shiyu Pan , Bo Cao , Deling Yuan , Tifeng Jiao , Qingrui Zhang , Shoufeng Tang . Complexes of cupric ion and tartaric acid enhanced calcium peroxide Fenton-like reaction for metronidazole degradation. Chinese Chemical Letters, 2024, 35(7): 109185-. doi: 10.1016/j.cclet.2023.109185
19. [19]
  Tian Cao , Xuyin Ding , Qiwen Peng , Min Zhang , Guoyue Shi . Intelligent laser-induced graphene sensor for multiplex probing catechol isomers. Chinese Chemical Letters, 2024, 35(7): 109238-. doi: 10.1016/j.cclet.2023.109238
20. [20]
  Rui Liu , Jinbo Pang , Weijia Zhou . Monolayer water shepherding supertight MXene/graphene composite films. Chinese Journal of Structural Chemistry, 2024, 43(10): 100329-100329. doi: 10.1016/j.cjsc.2024.100329

Get Citation

PDF

XML

Metrics

PDF Downloads(11)
Abstract views(503)
HTML views(55)

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

Improvement of the Selectivity for Hydrogen Peroxide Production via the Synergy of TiO2 and Graphene

Metrics

通讯作者: 陈斌, bchen63@163.com

Improvement of the Selectivity for Hydrogen Peroxide Production via the Synergy of TiO₂ and Graphene