Citation: HAYIERBIEK Kulisong, ZHAO Shu-Xian, YANG Yang, ZENG Han. Performance of Nitrogen-Doped Carbon Nanocomposite with Entrapped Enzyme-Based Fuel Cell[J]. Acta Physico-Chimica Sinica, ;2015, 31(9): 1715-1726. doi: 10.3866/PKU.WHXB201506231 shu

Performance of Nitrogen-Doped Carbon Nanocomposite with Entrapped Enzyme-Based Fuel Cell

1.
Chemistry and Chemical Engineering Academy, Xinjiang Normal University, Urumuqi 830054, P. R. China

Received Date: 31 March 2015
Available Online: 23 June 2015
Fund Project: 国家自然科学基金(21363024) (21363024) 新疆师范大学博士科研启动基金(XJNUBS1228) (XJNUBS1228)新疆维吾尔自治区2013年度高校科研计划青年教师培育项目(XJEDU2013S29)资助 (XJEDU2013S29)

A nanocomposite composed of N-doped mesoporous carbon material (NDMPC) and carboxymethylated chitosan (CMCH) was fabricated by mechanical co-mixing and used as an enzyme matrix. A novel glucose/O₂ enzymatic biofuel cell was fabricated with a Nafion ion-exchange membrane consisting of a laccase (Lac)-entrapped biocathode and glucose oxidase-incorporated bioanode. Enzyme electrodes were prepared by the dripping coat and air-dried method. The performance of the laccase-based electrode as a biocathode in a fuel cell and an oxygen electro-chemical sensor was characterized by cyclic voltammetry in combination with the rotating disk electrode technique, linear scanning voltammetry (LSV), and chronoamperometry. UV-Vis spectrometry and graphite furnace atomic absorption spectroscopy were used to investigate the configuration of enzyme molecules on the surface of electrode and to evaluate the enzyme loading of the matrix on the electrode interface. The results from the experiments showed that the laccasebased cathode displayed direct electron transfer between the active centre in laccase (T₁) and the conductive matrix without any external electron mediators (apparent electron transfer rate 0.013 s^-1). A minor overpotential for oxygen reduction (150 mV) was also observed. Through further comparison of the intra-molecule electron relay rate (1000 s^-1), substrate turnover frequency (0.023 s^-1), and previous enzyme-conductive matrix electron transfer rate, quantitative analysis showed that the latter was the rate-determining step in the whole catalytic cycle of the oxygen reduction reaction. This laccase-based electrode as an oxygen electrochemical sensor for detecting oxygen showed a low detection limit (0.04 μmol·dm^-3), high sensitivity (12.1 μA·μmol^-1·dm³), and affinity for oxygen (K_M = 8.2 μmol·dm^-3). This laccase-based cathode also had advantages such as excellent reproducibility, long-term usability, thermal stability, and pH endurance. The results for the fabricated biofuel cell showed an open circuit voltage of 0.38 V and a maximal energy output density of 19.2 μW·cm^-2, maintaining greater than 60% of the initial value even after continuous work for 3 weeks under optimal conditions.
- Laccase,
- Nitrogen-doped meso-porous carbon material,
- Carboxymethylated Chitosan,
- Direct electron transfer,
- Oxygen reduction reaction,
- Electrochemical sensor,
- Bio-fuel cell
1. [1]
  
  (1) Armstrong, F. A.; Hirst, J. Pro Natl. Acad. Sci. U. S. A. 2011, 108, 14049. doi: 10.1073/pnas.1103697108
2. [2]
  (2) Hussein, L.; Rubenwolf, S.; Von Stetten V.; Urban, G.; Zengerle, R.; Krueger, M.; Kerzenmacher, S. Biosens. Bioelectron. 2011, 26, 4133. doi: 10.1016/j.bios.2011.04.008
3. [3]
  (3) Martinez-Ortiz, J.; Flores, R.; Vazquez-Duhalt, R. Biosens. Bioelectron. 2011, 26, 2626. doi: 10.1016/j.bios.2010.11.022
4. [4]
  (4) Qiao, Y.; Li, C. M. J. Mater. Chem. 2011, 21, 4027. doi: 10.1039/C0JM02871A
5. [5]
  (5) Zayats, M.; Katz, E.; Baron, R.; Willner, I. A. J. Am. Chem. Soc. 2005, 127, 12400. doi: 10.1021/ja052841h
6. [6]
  (6) Liu, Y.; Qu, X. H.; Guo, H. W.; Chen, H. J.; Liu, B. F.; Dong, S. J. Biosens. Bioelectron. 2006, 21, 2195. doi: 10.1016/j.bios.2005.11.014
7. [7]
  (7) Klis, M.; Karbarz, M.; Stojek, Z.; Rogalski, J.; Bilewicz, R. J. Phys. Chem. C. 2009, 113, 6062. doi: 10.1021/jp8094159
8. [8]
  (8) Jensen, U. B.; Lorcher, S.; Vagin, M.; Chevallier, J.; Shipovskov, S.; Koroleva, O.; Besenbacher, F.; Ferapontova, E. Electrochim. Acta 2012, 62, 218. doi: 10.1016/j.electacta.2011.12.026
9. [9]
  (9) Osman, M. H.; Shah, A. A.; Walsh, F. C. Biosens. Bioelectron. 2011, 26, 3087. doi: 10.1016/j.bios.2011.01.004
10. [10]
  (10) Ramasamy, R. P.; Luckarift, H. R.; Ivnitski, D. M.; Atanassov, P. B.; Johnson, G. R. Chem. Commun. 2010, 46, 6045. doi: 10.1039/c0cc00911c
11. [11]
  (11) Mao, F.; Mano, N.; Heller, A. J. Am. Chem. Soc. 2003, 125, 4951. doi: 10.1021/ja029510e
12. [12]
  (12) Barriere, F.; Ferry, Y.; Rochefort, D.; Leech, D. Electrochem. Commun. 2004, 6, 237. doi: 10.1016/j.elecom.2003.12.006
13. [13]
  (13) Xian, Y. Z.; Xian, Y.; Zhou, L. H.; Wu, F. H.; Ling, Y.; Jin, L, T. Electrochem. Commun. 2007, 9, 142. doi: 10.1016/j.elecom. 2006.08.049
14. [14]
  (14) Wei, W.; Li, P. P.; Li, Y.; Cao, X. D.; Liu, S. Q. Electrochem. Commun. 2012, 22, 181. doi: 10.1016/j.elecom.2012.06.021
15. [15]
  (15) Trohalaki, S.; Pachter, R.; Luckarift, H. R.; Johnson, G. R. Fuel Cells 2012, 12, 656. doi: 10.1002/fuce.v12.4
16. [16]
  (16) Miyake, T.; Yoshino, S.; Yamada, T.; Hata, K.; Nishizawa, M. J. Am. Chem. Soc. 2011, 133, 5129. doi: 10.1021/ja111517e
17. [17]
  (17) Zeng, H.; Liao, L. W.; Li, M. F.; Tao, Q.; Kang, J.; Chen, Y. X. Acta Phys. -Chim. Sin. 2010, 26, 3217. [曾涵, 廖铃文, 李明芳, 陶骞, 康婧, 陈艳霞. 物理化学学报, 2010, 26, 3217.] doi: 10.3866/PKU.WHXB20101208
18. [18]
  (18) Zhu, Y. F.; Kaskel, S.; Shi, J. L.; Wage, T.; Pee, K. H. V. Chem. Mater. 2007, 19, 6408. doi: 10.1021/cm071265g
19. [19]
  (19) Pang, H. L.; Liu, J.; Hu, D.; Zhang, X. H.; Chen, J. H. Electrochim. Acta 2010, 55, 6611. doi: 10.1016/j.electacta. 2010.06.013
20. [20]
  (20) Kulisong, H.; Zeng, H. Chin. J. Appl. Chem. 2013, 30, 1194. [库里松•哈衣尔别克, 曾涵. 应用化学, 2013, 30, 1194.]
21. [21]
  (21) Vinu, A. Adv. Funct. Mater. 2008, 18, 816.
22. [22]
  (22) Qiu, H. J.; Xu, C. X.; Huang, X. R.; Ding, Y.; Qu, Y. B.; Gao, P. J. J. Phys. Chem. C. 2008, 112, 14781. doi: 10.1021/jp805600k
23. [23]
  (23) Zhao, H. Y.; Zhou, H. M.; Zhang, J. X.; Zheng, W.; Zheng, Y. F. Biosens. Bioelectron. 2009, 25, 463. doi: 10.1016/j.bios. 2009.08.005
24. [24]
  (24) Santucci, R.; Ferri, T.; Morpur , L.; Savini, I.; Avigliano, L. Biochem. J. 1998, 332, 611.
25. [25]
  (25) Zheng, H.; Hu, J. B.; Li, Q. L. Acta Chim. Sin. 2006, 64, 806. [郑华, 胡劲波, 李启隆. 化学学报, 2006, 64, 806.]
26. [26]
  (26) Freguia, S.; Virdis, B.; Harnisch, F.; Keller, J. Electrochim. Acta 2012, 82, 165. doi: 10.1016/j.electacta.2012.03.014
27. [27]
  (27) Cracknell, J. A.; Vincent, K. A.; Armstrong, F. A. Chem. Rev. 2008, 108, 2439. doi: 10.1021/cr0680639
28. [28]
  (28) Stolarczyk, K.; Lyp, D.; Zelechowska, K.; Biernat, J. F.; Rogalski, J.; Bilewicz, R. Electrochim. Acta 2012, 79, 74. doi: 10.1016/j.electacta.2012.06.050
29. [29]
  (29) Wang, X. J.; Latonen, R. M.; Sjoberg-Eerola, P.; Eriksson, J. E.; Bobacka, J.; Boer, H.; Bergelin, M. J. Phys. Chem. C 2011, 111, 5919.
30. [30]
  (30) Zhang, L. L.; Bai, L.; Xu, M.; Han, L.; Dong, S. J. Nano Ener. 2015, 11, 48. doi: 10.1016/j.nanoen.2014.10.020
31. [31]
  (31) Tsujimura, S.; Kamitaka, Y.; Kano, K. Fuel Cells 2007, 7, 463.
32. [32]
  (32) Soukharev, V.; Mano, N.; Heller, A. J. Am. Chem. Soc. 2004, 126, 8368. doi: 10.1021/ja0475510
33. [33]
  (33) Mano, N.; Kim, H. H.; Zhang, Y. C.; Heller, A. J. Am. Chem. Soc. 2002, 124, 6480. doi: 10.1021/ja025874v
34. [34]
  (34) Jiang, D. S.; Long, S. Y.; Huang, J.; Xiao, H. Y.; Zhou, J. Y. Bio. Eng. J. 2005, 25, 15. doi: 10.1016/j.bej.2005.03.007
35. [35]
  (35) Masson, J. F.; Kranz, C.; Mizaikoff, B. Anal. Chem. 2007, 79, 8531. doi: 10.1021/ac071090u
36. [36]
  (36) Liu, Y.; Wang, M. K.; Zhao, F.; Xu, Z. A.; Dong, S. J. Biosens. Bioelectron. 2005, 21, 984. doi: 10.1016/j.bios.2005.03.003
37. [37]
  (37) Ikeda, T. Electrochim. Acta 2012, 82, 158. doi: 10.1016/j.electacta.2012.01.114
38. [38]
  (38) Zheng, W.; Zhao, H. Y.; Zhang, J. X.; Zhou, H. M.; Xu, X. X.; Zheng, Y. F.; Wang, Y. B.; Cheng, Y.; Jang, B. Z. Electrochem. Commun. 2010, 12, 869. doi: 10.1016/j.elecom.2010.04.006
39. [39]
  (39) Katz, E.; Willner, I.; Kotlyar, A. B. J. Electroanal. Chem. 1999, 479, 64. doi: 10.1016/S0022-0728(99)00425-8
40. [40]
  (40) Li, X.; Zhang, L.; Su, L.; Ohsaka, T.; Mao, L. Fuel Cells 2019, 9, 85. doi: 10.1002/fuce.v9:1
41. [41]
  (41) Ammam, M.; Fransaer, J. Biotechnol. Bioeng. 2012, 109, 1601. doi: 10.1002/bit.v109.7
1. [1]
  Lu XU , Chengyu ZHANG , Wenjuan JI , Haiying YANG , Yunlong FU . Zinc metal-organic framework with high-density free carboxyl oxygen functionalized pore walls for targeted electrochemical sensing of paracetamol. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 907-918. doi: 10.11862/CJIC.20230431
2. [2]
  Xiaofeng Zhu , Bingbing Xiao , Jiaxin Su , Shuai Wang , Qingran Zhang , Jun Wang . Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides. Acta Physico-Chimica Sinica, 2024, 40(12): 2407005-. doi: 10.3866/PKU.WHXB202407005
3. [3]
  Hailang JIA , Hongcheng LI , Pengcheng JI , Yang TENG , Mingyun GUAN . Preparation and performance of N-doped carbon nanotubes composite Co₃O₄ as oxygen reduction reaction electrocatalysts. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 693-700. doi: 10.11862/CJIC.20230402
4. [4]
  Jing SU , Bingrong LI , Yiyan BAI , Wenjuan JI , Haiying YANG , Zhefeng Fan . Highly sensitive electrochemical dopamine sensor based on a highly stable In-based metal-organic framework with amino-enriched pores. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1337-1346. doi: 10.11862/CJIC.20230414
5. [5]
  Jiarong Feng , Yejie Duan , Chu Chu , Dezhen Xie , Qiu'e Cao , Peng Liu . Preparation and Application of a Streptomycin Molecularly Imprinted Electrochemical Sensor: A Suggested Comprehensive Analytical Chemical Experiment. University Chemistry, 2024, 39(8): 295-305. doi: 10.3866/PKU.DXHX202401016
6. [6]
  Hao XU , Ruopeng LI , Peixia YANG , Anmin LIU , Jie BAI . Regulation mechanism of halogen axial coordination atoms on the oxygen reduction activity of Fe-N₄ site: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 695-701. doi: 10.11862/CJIC.20240302
7. [7]
  Shuhui Li , Xucen Wang , Yingming Pan . Exploring the Role of Electrochemical Technologies in Everyday Life. University Chemistry, 2025, 40(3): 302-307. doi: 10.12461/PKU.DXHX202406059
8. [8]
  Meiqing Yang , Lu Wang , Haozi Lu , Yaocheng Yang , Song Liu . Recent Advances of Functional Nanomaterials for Screen-Printed Photoelectrochemical Biosensors. Acta Physico-Chimica Sinica, 2025, 41(2): 100018-. doi: 10.3866/PKU.WHXB202310046
9. [9]
  Hao BAI , Weizhi JI , Jinyan CHEN , Hongji LI , Mingji LI . Preparation of Cu₂O/Cu-vertical graphene microelectrode and detection of uric acid/electroencephalogram. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1309-1319. doi: 10.11862/CJIC.20240001
10. [10]
  Fengqiao Bi , Jun Wang , Dongmei Yang . Specialized Experimental Design for Chemistry Majors in the Context of “Dual Carbon”: Taking the Assembly and Performance Evaluation of Zinc-Air Fuel Batteries as an Example. University Chemistry, 2024, 39(4): 198-205. doi: 10.3866/PKU.DXHX202311069
11. [11]
  Jinyi Sun , Lin Ma , Yanjie Xi , Jing Wang . Preparation and Electrocatalytic Nitrogen Reduction Performance Study of Vanadium Nitride@Nitrogen-Doped Carbon Composite Nanomaterials: A Recommended Comprehensive Chemistry Experiment. University Chemistry, 2024, 39(4): 184-191. doi: 10.3866/PKU.DXHX202310094
12. [12]
  Zhuo Wang , Xue Bai , Kexin Zhang , Hongzhi Wang , Jiabao Dong , Yuan Gao , Bin Zhao . MOF模板法合成氮掺杂碳材料用于增强电化学钠离子储存和去除. Acta Physico-Chimica Sinica, 2025, 41(3): 2405002-. doi: 10.3866/PKU.WHXB202405002
13. [13]
  Xiangyu CAO , Jiaying ZHANG , Yun FENG , Linkun SHEN , Xiuling ZHANG , Juanzhi YAN . Synthesis and electrochemical properties of bimetallic-doped porous carbon cathode material. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 509-520. doi: 10.11862/CJIC.20240270
14. [14]
  Tiantian MA , Sumei LI , Chengyu ZHANG , Lu XU , Yiyan BAI , Yunlong FU , Wenjuan JI , Haiying YANG . Methyl-functionalized Cd-based metal-organic framework for highly sensitive electrochemical sensing of dopamine. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 725-735. doi: 10.11862/CJIC.20230351
15. [15]
  Qiaoqiao BAI , Anqi ZHOU , Xiaowei LI , Tang LIU , Song LIU . Construction of pressure-temperature dual-functional flexible sensors and applications in biomedicine. Chinese Journal of Inorganic Chemistry, 2024, 40(12): 2259-2274. doi: 10.11862/CJIC.20240128
16. [16]
  Yingxian Wang , Tianye Su , Limiao Shen , Jinping Gao , Qinghe Wu . Introduction of Chinese Lacquer from the Perspective of Chemistry: Popularizing Chemistry in Lacquer and Inherit Lacquer Art. University Chemistry, 2024, 39(5): 371-379. doi: 10.3866/PKU.DXHX202312015
17. [17]
  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
18. [18]
  Qinjin DAI , Shan FAN , Pengyang FAN , Xiaoying ZHENG , Wei DONG , Mengxue WANG , Yong ZHANG . Performance of oxygen vacancy-rich V-doped MnO₂ for high-performance aqueous zinc ion battery. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 453-460. doi: 10.11862/CJIC.20240326
19. [19]
  Pengcheng Yan , Peng Wang , Jing Huang , Zhao Mo , Li Xu , Yun Chen , Yu Zhang , Zhichong Qi , Hui Xu , Henan Li . Engineering Multiple Optimization Strategy on Bismuth Oxyhalide Photoactive Materials for Efficient Photoelectrochemical Applications. Acta Physico-Chimica Sinica, 2025, 41(2): 100014-. doi: 10.3866/PKU.WHXB202309047
20. [20]
  Xue Dong , Xiaofu Sun , Shuaiqiang Jia , Shitao Han , Dawei Zhou , Ting Yao , Min Wang , Minghui Fang , Haihong Wu , Buxing Han . 碳修饰的铜催化剂实现安培级电流电化学还原CO₂制C₂₊产物. Acta Physico-Chimica Sinica, 2025, 41(3): 2404012-. doi: 10.3866/PKU.WHXB202404012

Get Citation

PDF

XML

Metrics

PDF Downloads(269)
Abstract views(895)
HTML views(32)

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