Citation: Wenbiao Zhang, Bolong Yang, Zhonghua Xiang. Atomically dispersed Cu-based metal-organic framework directly for alkaline polymer electrolyte fuel cells[J]. Chinese Chemical Letters, ;2025, 36(2): 109630. doi: 10.1016/j.cclet.2024.109630 shu

Atomically dispersed Cu-based metal-organic framework directly for alkaline polymer electrolyte fuel cells

Wenbiao Zhang ^{a, b} ,
Bolong Yang ^a ,
Zhonghua Xiang ^{a, *,}

a.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
b.
Sungrow Hydrogen Sci.&Tech. Co., Ltd., Hefei 230088, China

xiangzh@mail.buct.edu.cn

Received Date: 2 January 2024
Revised Date: 28 January 2024
Accepted Date: 7 February 2024
Available Online: 14 February 2024

Figures(5)

Atomically dispersed Cu-based single-metal-site catalysts (Cu-N-C) have emerged as a frontier for electrocatalytic oxygen reduction reactions (ORR) because they can effectively optimize the d-band center of the Cu active site and provide appropriate adsorption/desorption energy for oxygen-containing intermediates. Metal-organic frameworks (MOFs) show excellent prospects in many fields because of their structural regularity and designability, but their direct use for electrocatalysis has been rarely reported due to the low intrinsic conductivity. Here, a MOF material (Cu-TCNQ) with highly regular single-atom copper active centers was successfully prepared using a solution chemical reaction method. Subsequently, Cu-TCNQ and graphene oxide (GO) were directly self-assembled to form a Cu-TCNQ/GO composite, which improved the conductivity of the catalyst while maintained the atomically precise controllability. The resistivity of the Cu-TCNQ/GO decreased by three orders of magnitude (1663.6–2.7 W/cm) compared with pure Cu-TCNQ. The half-wave potential was as high as 0.92 V in 0.1 mol/L KOH, even better than that of commercial 20% Pt/C. In alkaline polymer electrolyte fuel cells (APEFCs), the open-circuit voltage and power density of Cu-TCNQ/GO electrode reached 0.95 V and 320 mW/cm², respectively, which suggests that Cu-TCNQ/GO has a good potential for application as a cathode ORR catalyst.
- Metal-organic frameworks,
- Single-metal-site catalysts,
- Cu-TCNQ/GO,
- Oxygen reduction reaction,
- Alkaline polymer electrolyte fuel cells
1. [1]
  B.L. Yang, X.L. Li, Q. Cheng, et al., Nano Energy 101 (2022) 107565. doi: 10.1016/j.nanoen.2022.107565
2. [2]
  Q.H. Li, H.Q. Peng, Y.M. Wang, et al., Angew. Chem. Int. Ed. 58 (2019) 1442–1446. doi: 10.1002/anie.201812662
3. [3]
  P. Qin, S. Zhu, M. Mu, et al., Chin. Chem. Lett. 34 (2023) 108620. doi: 10.1016/j.cclet.2023.108620
4. [4]
  B.L. Yang, B.J. Li, Z.H. Xiang, Nano Res. 16 (2023) 1338–1361. doi: 10.1007/s12274-022-4682-y
5. [5]
  Y. Wang, Y. Pan, L.K. Zhu, et al., Carbon 146 (2019) 671–679. doi: 10.1016/j.carbon.2019.02.002
6. [6]
  F. Zhang, X. Liu, Y. Chen, et al., Chin. Chem. Lett. 34 (2023) 108142. doi: 10.1016/j.cclet.2023.108142
7. [7]
  G.B. Chen, P. Liu, Z.Q. Liao, et al., Adv. Mater. 32 (2020) 1907399. doi: 10.1002/adma.201907399
8. [8]
  X.Y. Xie, L.S. Peng, H.Z. Yang, et al., Adv. Mater. 33 (2021) 2101038. doi: 10.1002/adma.202101038
9. [9]
  Y.J. Chen, S.F. Ji, Y.G. Wang, et al., Angew. Chem. Int. Ed. 56 (2017) 6937–6941. doi: 10.1002/anie.201702473
10. [10]
  J. Qiao, Z. Bao, L. Kong, et al., Chin.e Chem. Lett. 34 (2023) 108318. doi: 10.1016/j.cclet.2023.108318
11. [11]
  H.X. Zhong, K.H. Ly, M.C. Wang, et al., Angew. Chem. Int. Ed. 131 (2019) 10787–10792. doi: 10.1002/ange.201907002
12. [12]
  B.L. Yang, Q. Han, L.K. Han, et al., Adv. Mater. 35 (2023) 2208661. doi: 10.1002/adma.202208661
13. [13]
  M.H. Liu, S.J. Liu, C.X. Cui, et al., Angew. Chem. Int. Ed. 61 (2022) e202213522. doi: 10.1002/anie.202213522
14. [14]
  R. Bao, Z.H. Xiang, Z.L. Qiao, et al., Angew. Chem. Int. Ed. 62 (2023) e202216751. doi: 10.1002/anie.202216751
15. [15]
  B.L. Yang, H.F. Yu, X.D. Jia, et al., ACS Appl. Mater. Interfaces 15 (2023) 23316–23327. doi: 10.1021/acsami.3c03203
16. [16]
  K.M. Zhao, S.Q. Liu, Y.Y. Li, et al., Adv. Energy Mater. 12 (2022) 2103588. doi: 10.1002/aenm.202103588
17. [17]
  X.L. Li, Z.H. Xiang, Nat. Commun. 13 (2022) 57. doi: 10.1038/s41467-021-27735-1
18. [18]
  C. Zhang, B. An, L. Yang, et al., J. Mater. Chem. A 4 (2016) 4457–4463. doi: 10.1039/C6TA00768F
19. [19]
  S.H. Liang, R.J. Chen, P.W. Yu, et al., Chem. Commun. 53 (2017) 11453–11456. doi: 10.1039/C7CC06555H
20. [20]
  I.E.L. Stephens, J. Rossmeisl, I. Chorkendorff, Science 354 (2016) 1378–1379. doi: 10.1126/science.aal3303
21. [21]
  K. Jiao, J. Xuan, Q. Du, et al., Nature 595 (2021) 361–369. doi: 10.1038/s41586-021-03482-7
22. [22]
  X.X. Wang, M.T. Swihart, G. Wu, Nat. Catal. 2 (2019) 578–589. doi: 10.1038/s41929-019-0304-9
23. [23]
  Z.Y. Mei, S. Cai, G.F. Zhao, et al., Chem. Eng. J. 430 (2022) 132691. doi: 10.1016/j.cej.2021.132691
24. [24]
  T.V.M. Sreekanth, G.R. Dillip, P.C. Nagajyothi, et al., Appl. Catal. B: Environ. 285 (2021) 119793. doi: 10.1016/j.apcatb.2020.119793
25. [25]
  S.J. Liu, M.H. Liu, X.W. Li, et al., Carbon Energy 5 (2023) 1–11.
26. [26]
  K.Y. Zou, M.Z. Jiang, Z.X. Zhao, et al., Chem. Eng. J. 476 (2023) 146793. doi: 10.1016/j.cej.2023.146793
27. [27]
  R. Ren, L.T. Yang, Z. Lin, et al., J. Mater. Chem. A 10 (2022) 22781–22790. doi: 10.1039/D2TA06228C
28. [28]
  D. Wu, Y.C. Wei, X. Ren, et al., Adv. Mater. 30 (2018) 1705366. doi: 10.1002/adma.201705366
29. [29]
  Z.Q. Deng, C.Q. Ma, S.H. Yan, et al., J. Mater. Chem. A 9 (2021) 20345–20349. doi: 10.1039/D1TA05281K
30. [30]
  J. Ma, E. Zhou, C. Fan, et al., Chem. Commun. 54 (2018) 5578–5581. doi: 10.1039/C8CC00802G
31. [31]
  Q. Li, P.F. Yan, G.F. Hou, et al., Dalt. Trans. 42 (2013) 7810–7815. doi: 10.1039/c3dt50261a
32. [32]
  K.Y. Zou, Z.R. Song, X. Gao, et al., Angew. Chem. Int. Ed. 60 (2021) 17070–17079. doi: 10.1002/anie.202103569
33. [33]
  B.L. Yang, J.K. Hou, Y.Y. Mi, et al., Next Sustain. 2 (2023) 100014. doi: 10.1016/j.nxsust.2023.100014
34. [34]
  T. Yang, X.N. Mao, Y. Zhang, et al., Nat. Commun. 12 (2021) 6022. doi: 10.1038/s41467-021-26316-6
35. [35]
  Y.T. Qu, Z.J. Li, W.X. Chen, et al., Nat. Catal. 1 (2018) 781–786. doi: 10.1038/s41929-018-0146-x
36. [36]
  T. Wang, R. Yang, N.E. Shi, et al., Small 15 (2019) 1902410. doi: 10.1002/smll.201902410
37. [37]
  Z. Wang, C. Zhu, H. Tan, et al., Adv. Funct. Mater. 31 (2021) 2104735. doi: 10.1002/adfm.202104735
38. [38]
  J. Yang, W.G. Liu, M.Q. Xu, et al., J. Am. Chem. Soc. 143 (2021) 14530–14539. doi: 10.1021/jacs.1c03788
1. [1]
  Jiayu Huang , Kuan Chang , Qi Liu , Yameng Xie , Zhijia Song , Zhiping Zheng , Qin Kuang . Fe-N-C nanostick derived from 1D Fe-ZIFs for Electrocatalytic oxygen reduction. Chinese Journal of Structural Chemistry, 2023, 42(10): 100097-100097. doi: 10.1016/j.cjsc.2023.100097
2. [2]
  Tengjia Ni , Xianbiao Hou , Huanlei Wang , Lei Chu , Shuixing Dai , Minghua Huang . Controllable defect engineering based on cobalt metal-organic framework for boosting oxygen evolution reaction. Chinese Journal of Structural Chemistry, 2024, 43(1): 100210-100210. doi: 10.1016/j.cjsc.2023.100210
3. [3]
  Longlong Geng , Huiling Liu , Wenfeng Zhou , Yong-Zheng Zhang , Hongliang Huang , Da-Shuai Zhang , Hui Hu , Chao Lv , Xiuling Zhang , Suijun Liu . Construction of metal-organic frameworks with unsaturated Cu sites for efficient and fast reduction of nitroaromatics: A combined experimental and theoretical study. Chinese Chemical Letters, 2024, 35(8): 109120-. doi: 10.1016/j.cclet.2023.109120
4. [4]
  Muhammad Riaz , Rakesh Kumar Gupta , Di Sun , Mohammad Azam , Ping Cui . Selective adsorption of organic dyes and iodine by a two-dimensional cobalt(II) metal-organic framework. Chinese Journal of Structural Chemistry, 2024, 43(12): 100427-100427. doi: 10.1016/j.cjsc.2024.100427
5. [5]
  Jinli Chen , Shouquan Feng , Tianqi Yu , Yongjin Zou , Huan Wen , Shibin Yin . Modulating Metal-Support Interaction Between Pt3Ni and Unsaturated WOx to Selectively Regulate the ORR Performance. Chinese Journal of Structural Chemistry, 2023, 42(10): 100168-100168. doi: 10.1016/j.cjsc.2023.100168
6. [6]
  Fereshte Hassanzadeh-Afruzi , Mina Azizi , Iman Zare , Ehsan Nazarzadeh Zare , Anwarul Hasan , Siavash Iravani , Pooyan Makvandi , Yi Xu . Advanced metal-organic frameworks-polymer platforms for accelerated dermal wound healing. Chinese Chemical Letters, 2024, 35(11): 109564-. doi: 10.1016/j.cclet.2024.109564
7. [7]
  Fahui Xiang , Lu Li , Zhen Yuan , Wuji Wei , Xiaoqing Zheng , Shimin Chen , Yisi Yang , Liangji Chen , Zizhu Yao , Jianwei Fu , Zhangjing Zhang , Shengchang Xiang . Enhanced C₂H₂/CO₂ separation in tetranuclear Cu(Ⅱ) cluster-based metal-organic frameworks by adjusting divider length of pore space partition. Chinese Chemical Letters, 2025, 36(3): 109672-. doi: 10.1016/j.cclet.2024.109672
8. [8]
  Yaxin Sun , Huiyu Li , Shiquan Guo , Congju Li . Metal-based cathode catalysts for electrocatalytic ORR in microbial fuel cells: A review. Chinese Chemical Letters, 2024, 35(5): 109418-. doi: 10.1016/j.cclet.2023.109418
9. [9]
  Ze Liu , Xiaochen Zhang , Jinlong Luo , Yingjian Yu . Application of metal-organic frameworks to the anode interface in metal batteries. Chinese Chemical Letters, 2024, 35(11): 109500-. doi: 10.1016/j.cclet.2024.109500
10. [10]
  Rui Wang , He Qi , Haijiao Zheng , Qiong Jia . Light/pH dual-responsive magnetic metal-organic frameworks composites for phosphorylated peptide enrichment. Chinese Chemical Letters, 2024, 35(7): 109215-. doi: 10.1016/j.cclet.2023.109215
11. [11]
  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
12. [12]
  Xiao-Hong Yi , Chong-Chen Wang . Metal-organic frameworks on 3D interconnected macroporous sponge foams for large-scale water decontamination: A mini review. Chinese Chemical Letters, 2024, 35(5): 109094-. doi: 10.1016/j.cclet.2023.109094
13. [13]
  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
14. [14]
  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
15. [15]
  Quanyou Guo , Yue Yang , Tingting Hu , Hongqi Chu , Lijun Liao , Xuepeng Wang , Zhenzi Li , Liping Guo , Wei Zhou . Regulating local electron transfer environment of covalent triazine frameworks through F, N co-modification towards optimized oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(1): 110235-. doi: 10.1016/j.cclet.2024.110235
16. [16]
  Xudong Zhao , Yuxuan Wang , Xinxin Gao , Xinli Gao , Meihua Wang , Hongliang Huang , Baosheng Liu . Anchoring thiol-rich traps in 1D channel wall of metal-organic framework for efficient removal of mercury ions. Chinese Chemical Letters, 2025, 36(2): 109901-. doi: 10.1016/j.cclet.2024.109901
17. [17]
  Sixiao Liu , Tianyi Wang , Lei Zhang , Chengyin Wang , Huan Pang . Cerium-based metal-organic framework-modified natural mineral vermiculite for photocatalytic nitrogen fixation under visible-light irradiation. Chinese Chemical Letters, 2025, 36(3): 110058-. doi: 10.1016/j.cclet.2024.110058
18. [18]
  Yatian Deng , Dao Wang , Jinglan Cheng , Yunkun Zhao , Zongbao Li , Chunyan Zang , Jian Li , Lichao Jia . A new popular transition metal-based catalyst: SmMn₂O₅ mullite-type oxide. Chinese Chemical Letters, 2024, 35(8): 109141-. doi: 10.1016/j.cclet.2023.109141
19. [19]
  Shaojie Ding , Henan Wang , Xiaojing Dai , Yuru Lv , Xinxin Niu , Ruilian Yin , Fangfang Wu , Wenhui Shi , Wenxian Liu , Xiehong Cao . Mn-modulated Co–N–C oxygen electrocatalysts for robust and temperature-adaptative zinc-air batteries. Chinese Journal of Structural Chemistry, 2024, 43(7): 100302-100302. doi: 10.1016/j.cjsc.2024.100302
20. [20]
  Jialin Cai , Yizhe Chen , Ruiwen Zhang , Cheng Yuan , Zeyu Jin , Yongting Chen , Shiming Zhang , Jiujun Zhang . Interfacial Pt-N coordination for promoting oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(2): 110255-. doi: 10.1016/j.cclet.2024.110255

Get Citation

PDF

XML

Metrics

PDF Downloads(1)
Abstract views(204)
HTML views(11)

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