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벤조퀴논 포집 폴리에틸렌이민-탄소나노튜브 지지체 기반 효소촉매의 바이오연료전지로서의 성능평가

Performance Evaluation of Biofuel cell using Benzoquinone Entrapped Polyethyleneimine-Carbon nanotube supporter Based Enzymatic Catalyst

  • 안연주 (서울과학기술대학교 에너지환경대학원) ;
  • 정용진 (서울과학기술대학교 에너지환경대학원) ;
  • 권용재 (서울과학기술대학교 에너지환경대학원)
  • Ahn, Yeonjoo (Grad. School of Energy and Environment, Seoul National Univ. of Science and Technology) ;
  • Chung, Yongjin (Grad. School of Energy and Environment, Seoul National Univ. of Science and Technology) ;
  • Kwon, Yongchai (Grad. School of Energy and Environment, Seoul National Univ. of Science and Technology)
  • 투고 : 2016.09.30
  • 심사 : 2016.12.12
  • 발행 : 2017.04.01

초록

본 연구에서는 글루코스 산화효소(glucose oxidase, GOx), 고분자인 폴리에틸렌이민(polyethyleneimine, PEI), 카본나노튜브(carbon nanotube, CNT)와 벤조퀴논(benzoquinone, BQ)을 이용하여 글루코스 바이오연료전지를 위한 바이오 촉매를 합성하였다. 이를 위해, 지지체인 PEI/CNT 복합체에 BQ를 정전기적 인력을 통해 물리적으로 포집한 뒤, GOx를 담지시켜 합성하였다. 이는 기존에 전자 매개체로서 전해질에 풀어서 사용했던 BQ를 전해질이 아닌 촉매 내에 포집하여 촉매를 구성하였다는 개선점이 크며, 그 결과, BQ가 포집되지 않은 촉매 대비, 1.9배 상승한 $34.16{\mu}A/cm^2$의 최대전류밀도를 얻음을 통해 촉매활성이 개선되었음을 증명하였고, 바이오연료전지의 산화극 촉매로 이용 시, BQ가 포집되지 않은 촉매를 이용한 바이오연료전지에 비해 1.2배 상승한 $0.91mW/cm^2$의 최대출력밀도를 얻었다. 이를 통해 바이오연료전지의 산화극을 위한 촉매로서 GOx와 함께 담지된 매개체 BQ를 포함한 촉매 제조 가능성을 확인하였다.

In this study, we synthesized biocatalyst consisting of glucose oxidase (GOx), polyethyleneimine (PEI) and carbon nanotube (CNT) with addition of p-benzoquinone (BQ) that was considered anodic catalysts of enzymatic biofuel cell (EBC). For doing this, PEI/CNT supporter was bonded with BQ by physical entrapping method stemmed from electrostatic attractive force ([BQ/PEI]/CNT). In turn, GOx moiety was further immobilized on the [BQ/PEI]/CNT to form GOx/[BQ/PEI]/CNT catalyst. This catalyst has a special advantage in that the BQ that has been usually dissolved into electrolyte was immobilized on supporter. According to the electrochemical analysis, maximum current density of the GOx/[BQ/PEI]/CNT catalyst was 1.9 fold better than that of the catalyst that did not entrap BQ with the value of $34.16{\mu}A/cm^2$, verifying that catalytic activity of the catalyst was enhanced by adoption of BQ. Also, when it was used as anodic catalyst of the EBC, its maximum power density was 1.2 fold better than that of EBC using the catalyst that did not entrap BQ with the value of $0.91mW/cm^2$. Based on such results, it turned out that the GOx/[BQ/PEI]/CNT catalyst was promising and viable as anodic catalyst of EBC.

키워드

참고문헌

  1. Lee, S. H., Kim, Y. S., Chu, C. H., Na, I. C., Lee, J. H. and Park, K. P., "Effect of Fabrication Method of Cathode on OCV in Enzyme Fuel Cells," Korean Chem. Eng. Res., 54(2), 171-174(2016). https://doi.org/10.9713/kcer.2016.54.2.171
  2. Lee, S. H., Hwang, B. C., Lee, H. R., Kim, Y. S., Chu, C. H., Na, I. C. and Park, K. P., "Effect of Fabrication Method of Anode on Performance in Enzyme Fuel Cells," Korean Chem. Eng. Res., 53(6), 667-671(2015). https://doi.org/10.9713/kcer.2015.53.6.667
  3. Wilson, R., "Glucose Oxidase: An Ideal Enzyme," Biosens. Bioelectron., 7, 165-185(1992). https://doi.org/10.1016/0956-5663(92)87013-F
  4. Ivnitski, D., Artyushkova, K., Rincon, R. A., Atanassov, P., Luckarift, H. R. and Johnson, G. R. "Entrapment of Enzymes and Carbon Nanotubes in Biologically Synthesized Silica: Glucose Oxidase-Catalyzed Direct Electron Transfer," Small, 4(3), 357-364(2008). https://doi.org/10.1002/smll.200700725
  5. Barton, S. C., Gallaway, J. and Atanassov, P., "Enzymatic Biofuel Cells for Implantable and Microscale Devices," Chem. Rev. 104, 4867-4886(2004). https://doi.org/10.1021/cr020719k
  6. Van Nguyen, K. and Minteer, S. D., "Investigating DNA Hydrogels as a New Biomaterial for Enzyme Immobilization in Biobatteries," Chemical Communications, 51(66), 13071-13073(2015). https://doi.org/10.1039/C5CC04810A
  7. Osadebe, I., Conghaile, P. O., Kavanagh, P., and Leech, D., "Glucose Oxidation by Osmium Redox Polymer Mediated Enzyme Electrodes Operating at Low Potential and in Oxygen, for Application to Enzymatic Fuel Cells," Electrochimica Acta, 182, 320-326(2015). https://doi.org/10.1016/j.electacta.2015.09.088
  8. Hyun, K. H., Han, S. W., Koh, W. and Kwon, Y., "Fabrication of Biofuel Cell Containing Enzyme Catalyst Immobilized by Layer-by-layer Method," Journal of Power Sources, 286, 197-203(2015). https://doi.org/10.1016/j.jpowsour.2015.03.136
  9. Chung, Y., Hyun, K. and Kwon, Y., "Fabrication of Biofuel Cell Improved by $\pi$-Conjugated Electron Pathway Effect Induced from a New Enzyme Catalyst Employing Terephthalaldehyde," Nanoscale, 8, 1161-1168(2016). https://doi.org/10.1039/C5NR06703K
  10. Chung, Y., Ahn, Y., Christwardana, M., Kim, H. and Kwon, Y., "Development of a Glucose Oxidase-based Biocatalyst Adopting Both Physical Entrapment and Crosslinking and its Use in Biofuel Cells," Nanoscale, 8, 9201-9210(2016). https://doi.org/10.1039/C6NR00902F
  11. Mandler, D., Kaminski, A. and Willner, I., "Application of Polyethyleneimine- quinone Modified Electrodes for Voltammetric Measurements of pH," Electrochimica acta, 37(15), 2765-2767(1992). https://doi.org/10.1016/0013-4686(92)85204-X
  12. Wang, J., "Electrochemical Glucose Biosensors," Chem. Rev., 108, 814-825(2008). https://doi.org/10.1021/cr068123a
  13. Laviron, E., "General Expression of the Linear Potential Sweep Voltammogram in the Case of Diffusionless Electrochemical Systems," J. Electroanal. Chem., 101, 19-28(1979). https://doi.org/10.1016/S0022-0728(79)80075-3
  14. Kamin, R. A. and Wilson, G. S., "Rotating Ring-disk Enzyme Electrode for Biocatalysis Kinetic Studies and Characterization of the Immobilized Enzyme Layer," Anal. Chem., 52(8), 1198-1205(1980). https://doi.org/10.1021/ac50058a010
  15. Ayato, Y., Suganuma, T., Seta, H., Yamagiwa, K., Shiroishi, H., and Kuwano, J., "Synthesis and Application of Carbon Nanotubes to Glucose Biofuel Cell with Glucose Oxidase and p-Benzoquinone," Journal of The Electrochemical Society, 162(14), F1482-F1486(2015). https://doi.org/10.1149/2.0621514jes

피인용 문헌

  1. Performance evaluation of glucose oxidation reaction using biocatalysts adopting different quinone derivatives and their utilization in enzymatic biofuel cells vol.36, pp.3, 2019, https://doi.org/10.1007/s11814-018-0218-2