Citation: YANG Xiao-Kun, CHEN A-Ling, YI Qing-Feng. Easy Preparation of N-Doped Graphene-like Nanosheets as Excellent Metal-Free Cathodic Electrocatalysts of Zn-Air Battery[J]. Chinese Journal of Inorganic Chemistry, ;2021, 37(1): 157-170. doi: 10.11862/CJIC.2021.001 shu

Easy Preparation of N-Doped Graphene-like Nanosheets as Excellent Metal-Free Cathodic Electrocatalysts of Zn-Air Battery

1.
School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan, Hunan 411201, China
2.
Hunan Provincial Key Lab of Advanced Materials for New Energy Storage and Conversion, Xiangtan, Hunan 411201, China

Corresponding author: YI Qing-Feng, yqfyy2001@hnust.edu.cn
Received Date: 19 July 2020
Revised Date: 28 October 2020

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Carbon-based materials have been paid much attention due to their own good electroactivity and resources availability. Herein, we reported a simple and versatile synthesis strategy for the preparation of nitrogen-doped and metal-free carbon catalysts with excellent oxygen reduction reaction (ORR) electroactivity. Using dicyandiamide (DCD) as nitrogen source and sucrose, β-cyclodextrin and chitosan as different carbon sources, N-doped graphene-like nanosheet samples CN-nanosh(suc), CN-nanosh(cyc) and CN-nanosh(ch) were prepared by an easy pyrolysis of their mixture. The samples exhibited outstanding ORR electroactivity in alkaline media with a comparable performance to the benchmark Pt/C. Alkaline Zn-air battery with the prepared sample CN-nanosh(suc) as the cathodic catalyst displayed the maximum power density of 201.33 mW·cm^-2, and its discharge time can last for more than 50 h at a constant current density of 100 mA·cm^-2, which is close to the optimum values of the similar Zn-air battery with the metal-free cathodic electrocatalysts reported so far.
- oxygen reduction reaction,
- Zn-air battery,
- electrochemistry,
- energy conversion,
- nanoparticles
1. [1]
  Yuan W J, Li J H, Xie A J, Chen P, Li S K, Shen Y H. Electrochim. Acta, 2015, 165:29-35 doi: 10.1016/j.electacta.2015.02.242
2. [2]
  Zhang J T, Zhao Z H, Xia Z H, Dai L M. Nat. Nanotechnol., 2015, 10(5):444-452
3. [3]
  Zheng Y, Jiao Y, Chen J, Liu J, Liang L, Du A J, Zhang W M, Zhu Z H, Smith S C, Jaroniec M. J. Am. Chem. Soc., 2011, 133(50):20116-20119 doi: 10.1021/ja209206c
4. [4]
  Zhan W C, Guo Y, Gong X Q, Guo Y L, Wang Y Q, Lu G Z. Chinese J. Catal., 2014, 35(8):1238-1250 doi: 10.1016/S1872-2067(14)60189-3
5. [5]
  Chen Z, Higgins D, Chen Z G. Carbon, 2010, 48:3057-3065 doi: 10.1016/j.carbon.2010.04.038
6. [6]
  Zhu H Y, Zhang S, Huang Y X, Wu L H, Sun S H. Nano Lett., 2013, 13(6):2947-2951 doi: 10.1021/nl401325u
7. [7]
  Yi Q F, Zhang Y H, Liu X P, Xiang B L, Yang Y H. J. Mater. Sci., 2014, 49:729-736 doi: 10.1007/s10853-013-7754-2
8. [8]
  Yi Q F, Zhang Y H, Liu X P, Yang Y H. Sci. China Chem., 2014, 57:739-747 doi: 10.1007/s11426-013-5027-1
9. [9]
  Yu L, Yi Q F, Yang X K, Li G. Chemistry Select, 2018, 3:12603-12612
10. [10]
  Wang Y C, Zhou T, Jiang K, Da P M, Zheng G F. Adv. Energy Mater., 2014, 4(16):1400696 doi: 10.1002/aenm.201400696
11. [11]
  Fan X J, Peng Z W, Ye R Q, Zhou H Q, Guo X. ACS Nano, 2015, 9(7):7407-7418 doi: 10.1021/acsnano.5b02420
12. [12]
  Ma T Y, Dai S, Jaroniec M, Qiao S Z. Angew. Chem., 2014, 126(28):7409-7413 doi: 10.1002/ange.201403946
13. [13]
  Deng Z L, Yi Q F, Zhang Y Y, Nie H D. J. Electroanal. Chem., 2017, 803:95-103 doi: 10.1016/j.jelechem.2017.09.025
14. [14]
  Gong K P, Du F, Xia Z H, Durstoch M, Dai L. Science, 2009, 323(5915):760-764 doi: 10.1126/science.1168049
15. [15]
  Yu P P, Zhang Z M, Zheng L X, Teng F, Hu L F, Fang X S. Adv. Energy Mater., 2016, 6(20):1601111 doi: 10.1002/aenm.201601111
16. [16]
  Lin Z Y, Song M K, Ding Y, Liu Y, Liu M L, Wong C P. Phy. Chem. Chem. Phy., 2012, 14(10):3381-3387 doi: 10.1039/c2cp00032f
17. [17]
  Jin J T, Pan F P, Jiang L H, Fu X G, Sun G Q. ACS Nano, 2014, 8:3313-3321 doi: 10.1021/nn404927n
18. [18]
  Preuss K, Kannuchamy V K, Marinovic A, Isaacs M, Wilson K, Abrahams I, Titirici M M. J. Energy Chem., 2016, 25:228-235 doi: 10.1016/j.jechem.2016.01.001
19. [19]
  Wu H H, Wang J, Wang G X, Cai F, Ye Y F, Jiang Q K, Sun S C. Nano Energy, 2016, 30:801-809 doi: 10.1016/j.nanoen.2016.09.016
20. [20]
  Zheng Y, Jiao Y, Li L H, Xing T, Chen Y, Jaroniec M, Qiao S Z. ACS Nano, 2014, 8:5290-5296 doi: 10.1021/nn501434a
21. [21]
  Yang X K, Yi Q F, Sheng K, Wang T. Ionics, 2019, 25:4817-4830 doi: 10.1007/s11581-019-03022-4
22. [22]
  Yu L, Yi Q F, Yang X K, Chen Y. Sci. China Mater., 2019, 62(9):1251-1264 doi: 10.1007/s40843-019-9439-9
23. [23]
  Sheng K, Yi Q F, Hou L F, Chen A L. J. Electrochem. Soc., 2020, 167:070560 doi: 10.1149/1945-7111/ab8646
24. [24]
  Wang Q C, Ji Y J, Lei Y P, Wang Y B, Wang Y D, Li Y Y, Wang S Y. ACS Energy Lett., 2018, 3(5):1183-1191 doi: 10.1021/acsenergylett.8b00303
25. [25]
  Cao J Y, Hu Y, Chen L J, Xu J, Chen Z D. Int. J. Hydrogen Energy, 2017, 42(5):2931-2942 doi: 10.1016/j.ijhydene.2017.01.029
26. [26]
  Zhang H M, Chen J Y, Li Y B, Liu P R, Wang Y, An T C, Zhao H J. Electrochim. Acta, 2015, 165:7-13 doi: 10.1016/j.electacta.2015.02.240
27. [27]
  Chen D W, Zou Y Q, Wang S Y. Mater. Today Energy, 2019, 12:250-268 doi: 10.1016/j.mtener.2019.01.006
28. [28]
  Shinde S S, Lee C H, Sami A, Kim D H, Lee S U, Lee J H. ACS Nano, 2017, 11(1):347-357 doi: 10.1021/acsnano.6b05914
29. [29]
  Lai L F, Potts J R, Zhan D, Wang L, Poh C K, Tang C H, Gong H, Shen Z X, Lin J Y, Ruoff R S. Energy Environ. Sci., 2012, 5(7):7936-7942 doi: 10.1039/c2ee21802j
30. [30]
  Meng Y, Gu D, Zhang F Q, Shi Y F, Zhao D Y. Angew. Chem. Int. Ed., 2005, 44(43):7053-7059 doi: 10.1002/anie.200501561
31. [31]
  Deng Z L, Yi Q F, Li G, Chen Y, Yang X K, Nie H D. Electrochim. Acta, 2018, 279:1-9 doi: 10.1016/j.electacta.2018.05.069
32. [32]
  Wei C T, Wang H J, Eid K, Kim J, Kim J H, Alothman Z A, Wang L. Chem.-Eur. J., 2016, 23:637-643
33. [33]
  Yang J Q, Zhou X L, Wu D H, Zhao X D, Zhou Z. Adv. Mater., 2016, 29(6):1604108
34. [34]
  Qie L, Chen W M, Xiong X Q, Hu C C, Zou F, Hu P, Huang Y H. Adv. Sci., 2015, 2(12):1500195
35. [35]
  Tamilarasan P, Ramaprabhu S. J. Mater. Chem. A, 2015, 3(1):101-108
36. [36]
  Xue H R, Wang T, Guo H, Fan X L. RSC Adv., 2014, 4(101):57724-57732 doi: 10.1039/C4RA09939G
37. [37]
  Qu K, Zheng Y, Dai S, Qiao S Z. Nanoscale, 2015, 7(29):12598-12605 doi: 10.1039/C5NR03089G
38. [38]
  Cong H P, Wang P, Gong M, Yu S H. Nano Energy, 2014, 3:55-63 doi: 10.1016/j.nanoen.2013.10.010
39. [39]
  Ferrari A, Basko D M. Nat Nanotechnol., 2013, 8(4):235-246
40. [40]
  Zhang N F, Zhou Y M, Yang X Y, Tang C L, Wu H, Zhong N S. RSC Adv., 2014, 4(34):17549-17554 doi: 10.1039/c3ra47853j
41. [41]
  Yang C, Xu Y Y, Zhang C, Sun Z C, Chen C S, Li X H, Jiang S Z, Man B Y. Nanoscale Res. Lett., 2014, 9(1):394 doi: 10.1186/1556-276X-9-394
42. [42]
  Yu H J, Shang L, Bian T, Shi R, Waterhouse G I N, Zhao Y F, Zhou C, Wu L Z, Tung C H, Zhang T R. Adv. Mater., 2016, 28(25):5140 doi: 10.1002/adma.201670178
43. [43]
  Gupta S, Qiao L, Zhao S, Xu H, Lin Y, Devaguptapu S V, Wang X L, Swihart M T, Wu G. Adv. Energy Mater., 2016, 6(22):1601198 doi: 10.1002/aenm.201601198
44. [44]
  Wang M, Yang Z Z, Wang J Q, Li H, Gu L, Yu Y. Small, 2015, 11(40):5330 doi: 10.1002/smll.201570245
45. [45]
  Raccichini R, Varzi A, Passerini S, Scrosati B. Nat. Mater., 2014, 14(3):271-279
46. [46]
  Ning R, Ge C J, Liu Q, Tian J Q, Asiri A M, Alamry K A, Li C M, Sun X P. Carbon, 2014, 78:60-69 doi: 10.1016/j.carbon.2014.06.048
47. [47]
  Li J C, Zhao S Y, Hou P X, Fang R P, Liu C, Liang J, Cheng H M. Nanoscale, 2015, 7(45):19201-19206 doi: 10.1039/C5NR05998D
48. [48]
  Wasalathilake K C, Galpaya D G, Ayoko G A, Yan C. Carbon, 2018, 137:282-290 doi: 10.1016/j.carbon.2018.05.036
49. [49]
  Dettlaff A, Sawczak M, Klugmann-Radziemska E, Czylkowski D, Miotk R, Wilamowska-Zawłocka M. RSC Adv., 2017, 7(51):31940-31949 doi: 10.1039/C7RA04707J
50. [50]
  Liu G, Li X G, Ganesan P, Popov B N. Electrochim. Acta, 2010, 55(8):2853-2858 doi: 10.1016/j.electacta.2009.12.055
51. [51]
  Rao C V, Cabrera C R, Ishikawa Y. J. Phys. Chem. Lett., 2010, 1(18):2622-2627 doi: 10.1021/jz100971v
52. [52]
  Tang C, Wang B, Wang H F, Zhang Q. Adv. Mater., 2017, 29(37):1703185 doi: 10.1002/adma.201703185
53. [53]
  Wan K, Long G F, Liu, M Y, Du L, Liang Z X, Tsiakaras P. Appl. Catal. B, 2015, 165:566-571 doi: 10.1016/j.apcatb.2014.10.054
54. [54]
  Choi C H, Park S H, Woo S I. Green Chem., 2011, 13(2):406-412
55. [55]
  Sahraie N R, Paraknowitsch J P, Göbel C, Thomas A, Strasser P. J. Am. Chem. Soc., 2014, 136(41):14486-14497
56. [56]
  Zhu C Z, Li H, Fu S F, Du D, Lin Y H. Chem. Soc. Rev., 2016, 45:517-531
57. [57]
  Ai K, Liu Y L, Ruan C P, Lu L H, Lu G M. Adv. Mater., 2013, 25(7):998-1003
58. [58]
  Yang Z, Yao Z, Li G F, Fang J Y, Nie H G, Liu Z, Zhou X M, Chen X A, Huang S M. ACS Nano, 2012, 6(1):205-211
59. [59]
  Chen Z, Yu A P, Higgins D, Li H, Wang H J, Chen Z W. Nano Lett., 2012, 12:1946-1952
60. [60]
  Fu G T, Cui Z M, Chen Y F, Li Y T, Tang Y W, Goodenough J B. Adv. Energy Mater., 2016, 7:1601172
61. [61]
  Liu L Z, Zeng G, Chen J X, Bi L L, Dai L M, Wen Z H. Nano Energy, 2018, 49:393-406
62. [62]
  Xu N N, Zhang Y X, Zhang T, Liu Y Y, Qiao J L. Nano Energy, 2019, 57:176-185
63. [63]
  Li C L, Wu M C, Liu R. Appl. Catal. B, 2019, 244:150-158
64. [64]
  Wan W J, Liu X J, Li H Y, Peng X Y, Xi D S, Luo J. Appl. Catal. B, 2019, 240:193-200
65. [65]
  Pei Z X, Hong F, Huang Y, Xue Q Z, Yang C Y, Zhu M S, Wang Z F. Energy Environ. Sci., 2017, 10(3):742-749
66. [66]
  Wang Q C, Ji Y J, Lei Y P, Wang Y B, Wang Y D, Li Y Y, Wang S Y. ACS Energy Lett., 2018, 3(5):1183-1191
67. [67]
  Shinde S S, Lee C H, Jung J Y, Wagh N K, Kim S H, Kim D H, Lin C, Lee S U, Lee J H. Energy Environ. Sci., 2019, DOI:10.1039/c8ee02679c doi: 10.1039/c8ee02679c
68. [68]
  Tang Z J, Pei Z X, Wang Z F, Li H F, Zeng J, Ruan Z H, Huang Y, Zhu M S, Xue Q, Yu J, Zhi C Y. Carbon, 2018, 130:532-543
69. [69]
  Shinde S S, Lee C H, Yu J Y, Kim D H, Lee S U, Lee L H. ACS Nano, 2018, 12(1):596-608
70. [70]
  Tang C, Wang B, Wang H F, Zhang Q. Adv. Mater., 2017, 29(37):1703185
71. [71]
  Li Y M, Yan Z, Wang Q D, Ye H T, Li M L, Zhu L W, Cao X B. Electrochim. Acta, 2018, 282:224-232
72. [72]
  Shinde S, Yu J Y, Song J W, Nam Y H, Kim D H, Lee D H. Nanoscale Horiz., 2017, 2(6):333-341
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