Citation: 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[J]. Chinese Chemical Letters, ;2024, 35(10): 109423. doi: 10.1016/j.cclet.2023.109423 shu

Nano-engineered catalysts for high-performance oxygen reduction reaction

Kunsong Hu ^a ,
Yulong Zhang ^e ,
Jiayi Zhu ^b ,
Jinhua Mai ^a ,
Gang Liu ^d ,
Manoj Krishna Sugumar ^b ,
Xinhua Liu ^{c, *,} ,
Feng Zhan ^{a, *,} ,
Rui Tan ^{b, *,}

a.
School of Resources, Environment and Materials, Guangxi University, Nanning 530004, China
b.
Energy lnnovation Centre, Warwick Manufacture Group, University of Warwick, Coventry CV4 7AL, United Kingdom
c.
School of Transportation Science and Engineering, Beihang University, Beijing 100191, China
d.
IDTECH (Suzhou) Co., Ltd., Suzhou 215217, China
e.
College of Mechatronical and Electrical Engineering, Hebei Agricultural University, Baoding 071001, China

liuxinhua19@buaa.edu.cn

phy_idea@outlook.com

rui.tan@warwick.ac.uk

Received Date: 5 November 2023
Revised Date: 5 December 2023
Accepted Date: 11 December 2023
Available Online: 23 December 2023

Figures(6)

The efficient energy conversion of fuel cells is greatly constrained by the slow oxygen reduction reaction (ORR) kinetics, which necessitates the use of highly active metal catalysts such as platinum (Pt). The critical challenge limiting large-scale usage of Pt is the capital cost that can be addressed through a prototypical approach by embedding metal nanoparticles (NPs), e.g., Pt NPs, in the conductive framework. However, previously reported embedding approaches are sophisticated and suffer from limited yields, leading to higher chemical process costs and remaining distant from commercial viability. Here, we report a facile, cost-effective and time-efficient structural tuning approach to synthesizing ultrafine Pt NPs impregnated within a conductive and highly porous carbon framework via a microwave-assisted polyol reduction method. Pt NPs with a uniform size of ~2.27 nm can be successfully integrated within the pores of the carbon framework, enabling homogeneous dispersion. Benefiting from these highly dispersed and ultrafine Pt NPs, the electrochemical surface area (ECSA) is improved to 142.98 m²/g_Pt, 2.25 times higher than that of the commercial counterpart (63.52 m²/g_Pt). Furthermore, our structurally optimized catalyst composite features a remarkably catalytic activity with a high half-wave potential (E_1/2) of 0.895 V and an improved mass activity (MA) of 0.2289 A/mg_Pt, 2.39-fold improvement compared to the commercial counterpart. In addition, orthogonal experiments were designed to identify the key process parameters for fabricating Pt/C catalysts, offering insights for scaled-up and industrial production.
- Fuel cells,
- Oxygen reduction reaction,
- Structural engineering,
- Microwave method,
- Ultrafine nanoparticles
1. [1]
  L. Dai, K. Huang, Y. Xia, Z. Xu, Green Energy Environ. 6 (2021) 193–211. doi: 10.1016/j.gee.2020.09.015
2. [2]
  J. Li, L. Zhang, K. Doyle-Davis, R. Li, X. Sun, Carbon Energy 2 (2020) 488–520. doi: 10.1002/cey2.74
3. [3]
  H. Wan, W. Ma, K. Zhou, et al., Green Energy Environ. 7 (2022) 205–220. doi: 10.1016/j.gee.2021.04.001
4. [4]
  Y. Pan, F.F. Deng, Z. Fang, et al., Chin. Chem. Lett. 32 (2021) 3440–3445. doi: 10.1016/j.cclet.2021.05.067
5. [5]
  M.F. Labata, G. Li, J. Ocon, P.Y.A. Chuang, J. Power Sources 487 (2021) 229356. doi: 10.1016/j.jpowsour.2020.229356
6. [6]
  Z. Qiao, S. Hwang, X. Li, et al., Energy Environ. Sci. 12 (2019) 2830–2841. doi: 10.1039/c9ee01899a
7. [7]
  L. Huang, S. Zaman, X. Tian, et al., Acc. Chem. Res. 54 (2021) 311–322. doi: 10.1021/acs.accounts.0c00488
8. [8]
  Y. Wang, Y. Pang, H. Xu, A. Martinez, K.S. Chen, Energy Environ. Sci. 15 (2022) 2288–2328. doi: 10.1039/d2ee00790h
9. [9]
  J. Liu, T. Zhang, G.I.N. Waterhouse, J. Mater. Chem. A 8 (2020) 23142–23161. doi: 10.1039/d0ta09092a
10. [10]
  K. Jiao, J. Xuan, Q. Du, et al., Nature 595 (2021) 361–369. doi: 10.1038/s41586-021-03482-7
11. [11]
  H. Zeng, X. Liu, F. Chen, et al., ACS Appl. Mater. Interfaces 12 (2020) 52549–52559. doi: 10.1021/acsami.0c13597
12. [12]
  C. Zhang, R. Lu, C. Liu, et al., Adv. Sci. 9 (2022) 2104768. doi: 10.1002/advs.202104768
13. [13]
  Q. Ji, L. Bi, J. Zhang, H. Cao, X.S. Zhao, Energy Environ. Sci. 13 (2020) 1408–1428. doi: 10.1039/d0ee00092b
14. [14]
  X.T. Wang, T. Ouyang, L. Wang, J.H. Zhong, Z.Q. Liu, Angew. Chem. Int. Ed. 59 (2020) 6492–6499. doi: 10.1002/anie.202000690
15. [15]
  D. Banham, J. Zou, S. Mukerjee, et al., J. Power Sources 490 (2021) 229515. doi: 10.1016/j.jpowsour.2021.229515
16. [16]
  W. Li, C. Han, K. Zhang, S. Chou, S. Dou, J. Mater. Chem. A 9 (2021) 6671–6693. doi: 10.1039/d1ta00203a
17. [17]
  X. Duan, F. Cao, R. Ding, et al., Adv. Energy Mater. 12 (2022) 2103144. doi: 10.1002/aenm.202103144
18. [18]
  Q. Ma, H. Jin, J Zhu, et al., Adv. Sci. 8 (2021) 2102209. doi: 10.1002/advs.202102209
19. [19]
  Q. Chen, X. Tan, Y. Liu, et al., J. Mater. Chem. A 8 (2020) 5773–5811. doi: 10.1039/c9ta11618d
20. [20]
  C. Zhang, Z. Feng, Y. Lei, et al., J. Colloid Interface Sci. 628 (2022) 174–188. doi: 10.4103/gmit.gmit_19_22
21. [21]
  J. Cheng, C. Lyu, G. Dong, et al., Electrochim. Acta 454 (2023) 142364. doi: 10.1016/j.electacta.2023.142364
22. [22]
  K. Paperzh, A. Alekseenko, O. Safronenko, et al., Colloid Interface Sci. Commun. 45 (2021) 100517. doi: 10.1016/j.colcom.2021.100517
23. [23]
  F. Sun, R. Su, Y. Zhou, et al., ACS Appl. Mater. Interfaces 14 (2022) 41079–41085. doi: 10.1021/acsami.2c11910
24. [24]
  H. Zhong, L. Alberto Estudillo-Wong, Y. Gao, Y. Feng, N. Alonso-Vante, J. Energy Chem. 59 (2021) 615–625. doi: 10.1016/j.jechem.2020.11.033
25. [25]
  D. Liu, J. Zhang, D. Liu, et al., J. Phys. Chem. Lett. 13 (2022) 2019–2026. doi: 10.1021/acs.jpclett.1c04005
26. [26]
  M. Xie, T. Chu, X. Wang, et al., Int. J. Hydrogen Energy 47 (2022) 28074–28085. doi: 10.1016/j.ijhydene.2022.06.131
27. [27]
  A.M. Jauhar, Z. Ma, M. Xiao, et al., J. Power Sources 473 (2020) 228607. doi: 10.1016/j.jpowsour.2020.228607
28. [28]
  D.D. Qin, Y. Tang, G. Ma, et al., Int. J. Hydrogen Energy 46 (2021) 25771–25781. doi: 10.1016/j.ijhydene.2021.05.096
29. [29]
  W. Zhang, J. Li, Z. Wei, Small 19 (2023) 2300112. doi: 10.1002/smll.202300112
30. [30]
  T. Lu, H. Wang, Nano Res. 15 (2022) 9764–9778. doi: 10.1007/s12274-022-4157-1
31. [31]
  Z. Ma, H. Tian, G. Meng, et al., Sci. China Mater. 63 (2020) 2517–2529. doi: 10.1007/s40843-020-1449-2
32. [32]
  B. Garlyyev, K. Kratzl, M. Rück, et al., Angew. Chem. Int. Ed. 58 (2019) 9596–9600. doi: 10.1002/anie.201904492
33. [33]
  Y. Wang, X. Zheng, D. Wang, Nano Res. 15 (2021) 1730–1752.
34. [34]
  Q. Wang, M. Ming, S. Niu, et al., Adv. Energy Mater. 8 (2018) 1801698. doi: 10.1002/aenm.201801698
35. [35]
  X. Li, W.X. Chen, J. Zhao, W. Xing, Z.D. Xu, Carbon 43 (2005) 2168–2174. doi: 10.1016/j.carbon.2005.03.030
36. [36]
  R. Zeng, K. Wang, W. Shao, et al., Chin. J. Catal. 41 (2020) 820–829. doi: 10.1016/S1872-2067(19)63456-X
37. [37]
  E. Antolini, F. Cardellini, E. Giacometti, G. Squadrito, JMatS 37 (2002) 133–139.
38. [38]
  J. Salgado, E. Antolini, E. Gonzalez, J. Power Sources 141 (2005) 13–18. doi: 10.1016/j.jpowsour.2004.08.048
39. [39]
  Y. Li, X. Zhu, Y. Chen, S. Zhang, J. Li, J. Liu, J. Energy Chem. 47 (2020) 138–145. doi: 10.1016/j.jechem.2019.12.004
40. [40]
  J. Yang, W. Li, D. Wang, Y. Li, Adv. Mater. 32 (2020) 2003300. doi: 10.1002/adma.202003300
41. [41]
  K. Sang, J. Zuo, X. Zhang, et al., Green Energy Environ. 8 (2023) 619–625. doi: 10.1016/j.gee.2022.12.006
42. [42]
  G. Ren, M. Shi, S. Liu, et al., Chem. Eng. J. 454 (2023) 140158. doi: 10.1016/j.cej.2022.140158
43. [43]
  R.G. Rao, R. Blume, M.T. Greiner, et al., ACS Catal. 12 (2022) 7344–7356. doi: 10.1021/acscatal.2c01063
44. [44]
  B.A. Lu, L.F. Shen, J. Liu, et al., ACS Catal. 11 (2020) 355–363.
45. [45]
  Z. Mao, C. Ding, X. Liu, et al., ACS Catal. 12 (2022) 8848–8856. doi: 10.1021/acscatal.2c01052
46. [46]
  E. Pajootan, S. Omanovic, S. Coulombe, Chem. Eng. J. 426 (2021) 131706. doi: 10.1016/j.cej.2021.131706
47. [47]
  J. Kong, Y.H. Qin, T.L. Wang, C.W. Wang, Int. J. Hydrogen Energy 45 (2020) 1991–1997. doi: 10.1016/j.ijhydene.2019.11.016
48. [48]
  J. Bai, S. Ke, J. Song, et al., ACS Appl. Mater. Interfaces 14 (2022) 5287–5297. doi: 10.1021/acsami.1c20823
49. [49]
  G.T. Song, Y. Wang, Y. Qi, W.M. Li, L.X. Zhang, Rare Met. 39 (2019) 784–791. doi: 10.1145/3343031.3350996
50. [50]
  D. Liu, S. Gao, J. Xu, et al., Appl. Surf. Sci. 604 (2022) 154466. doi: 10.1016/j.apsusc.2022.154466
51. [51]
  D. Nechiyil, M.S. Garapati, R.C. Shende, et al., J. Colloid Interface Sci. 561 (2020) 439–448. doi: 10.1016/j.jcis.2019.11.015
52. [52]
  R. Sharma, S. Gyergyek, S.M. Andersen, ACS Appl. Energy Mater. 5 (2022) 705–716. doi: 10.1021/acsaem.1c03189
53. [53]
  J. Quinson, M. Inaba, S. Neumann, et al., ACS Catal. 8 (2018) 6627–6635. doi: 10.1021/acscatal.8b00694
54. [54]
  Q. Dong, Z. Mo, H. Wang, et al., ACS Sustain. Chem. Eng. 8 (2020) 6979–6989. doi: 10.1021/acssuschemeng.0c00132
55. [55]
  X. Wang, J. Zheng, R. Fu, J. Ma, Chin. J. Catal. 32 (2011) 599–605. doi: 10.1016/S1872-2067(10)60213-6
56. [56]
  S. Wu, Y. Liu, Y. Ren, Q. Wei, Y. Sun, Nano Res. 15 (2021) 4886–4892.
57. [57]
  Y. Xin, T. Nagata, K. Kato, T. Shirai, ACS Appl. Nano Mater. 5 (2022) 4305–4315. doi: 10.1021/acsanm.2c00236
58. [58]
  F. Wang, X. Liu, B. Jiang, et al., J. Colloid Interface Sci. 635 (2023) 514–523. doi: 10.1016/j.jcis.2022.12.160
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