[논문]테레프탈알데하이드의 전자전달 강화효과에 따른 헴 단백질 모방 촉매의 성능 향상 및 이를 이용한 비분리막형 과산화수소 연료전지

전시은; 안희연; 정용진

doi:10.9713/kcer.2022.60.4.588

테레프탈알데하이드의 전자전달 강화효과에 따른 헴 단백질 모방 촉매의 성능 향상 및 이를 이용한 비분리막형 과산화수소 연료전지
Effect of Terephthalaldehyde to Facilitate Electron Transfer in Heme-mimic Catalyst and Its Use in Membraneless Hydrogen Peroxide Fuel Cell 원문보기

Korean chemical engineering research = 화학공학, v.60 no.4, 2022년, pp.588 - 593

전시은 (한국교통대학교 교통.에너지융합전공) , 안희연 (한국교통대학교 교통.에너지융합전공) , 정용진 (한국교통대학교 교통.에너지융합전공)

초록
AI-Helper

본 논문에서는 hemin, 폴리에틸렌이민(PEI) 및 탄소나노튜브(CNT)를 이용하여 제조 CNT/PEI/hemin/PEI 복합재에 가교제인 테레프탈알데하이드(TPA)를 첨가하여 전자전달이 개선된 과산화수소 환원 반응(HPRR) 촉매를 합성하였다. 합성된 촉매(CNT/PEI/hemin/PEI/TPA)를 과산화수소 10 mM 농도에서 HPRR 반응성을 확인한 결과, 0.2 V (vs. Ag/AgCl)에서 0.2813 mA cm^-2의 전류 밀도로 나타났으며, 이는 가교하지 않은 촉매(CNT/PEI/hemin/PEI)와 범용 가교제인 글루타르알데하이드(GA)에 의해 가교된 촉매(CNT/PEI/hemin/PEI/GA)에 비해 각각 2.43 및 1.87배 증가하였다. CNT/PEI/hemin/PEI/TPA의 HPRR 개시전위는 0.544 V로서 CNT/PEI/hemin/PEI와 CNT/PEI/hemin/PEI/GA의 0.511 및 0.471 V에 비하여 원활한 전자전달에 의해 개선되었음을 확인할 수 있었다. 이는 전기화학 임피던스 분광법(EIS)을 이용한 분석 결과에서도 확인되었는데, CNT/PEI/hemin/PEI/GA의 경우, 전자전달을 방해하는 가교제의 도입에 따라 CNT/PEI/hemin/PEI에 비하여 높은 전자전달저항을 나타낸 반면, CNT/PEI/hemin/PEI/TPA는 6.2% 감소하여, 가장 낮은 전자전달저항을 나타냈다. 막이 없는 흐름형 과산화수소 연료전지를 이용한 평가에서도, CNT/PEI/hemin/PEI/TPA를 환원극으로 활용한 전지의 최대 출력 밀도가 36.34±1.41 μWcm^-2로, CNT/PEI/hemin/PEI (27.87±0.95 μWcm^-2)와 CNT/PEI/hemin/PEI/GA(25.57±1.32 μWcm^-2) 보다 높게 측정되어, TPA는 전자전달을 개선 성능을 확인할 수 있었다.

Abstract ▼ AI-Helper

Terephthalaldehyde (TPA) is introduced as a cross liker to enhance electron transfer of hemin-based cathodic catalyst consisting of polyethyleneimine (PEI), carbon nanotube (CNT) for hydrogen peroxide reduction reaction (HPRR). In the cyclic voltammetry (CV) test with 10 mM H2O2 in phosphate buffer solution (pH 7.4), the current density for HPRR of the suggested catalyst (CNT/PEI/hemin/PEI/TPA) shows 0.2813 mA cm-2 (at 0.2 V vs. Ag/AgCl), which is 2.43 and 1.87 times of non-cross-linked (CNT/PEI/hemin/PEI) and conventional cross liker (glutaraldehyde, GA) used catalyst (CNT/PEI/hemin/PEI/GA), respectively. In the case of onset potential for HPRR, that of CNT/PEI/hemin/PEI/TPA is observed at 0.544 V, while those of CNT/PEI/hemin/PEI and CNT/PEI/hemin/PEI/GA are 0.511 and 0.471 V, respectively. These results indicate that TPA plays a role in facilitating electron transfer between the electrodes and substrates due to the π-conjugated cross-linking bonds, whereas conventional GA cross-linker increases the overpotential by interrupting electron and mass transfer. Electrochemical impedance spectroscopy (EIS) results also display the same tendency. The charge transfer resistance (Rct) of CNT/PEI/hemin/PEI/TPA decreases about 6.2% from that of CNT/PEI/hemin/PEI, while CNT/PEI/hemin/PEI/GA shows the highest Rct. The polarization curve using each catalyst also supports the superiority of TPA cross liker. The maximum power density of CNT/PEI/hemin/PEI/TPA (36.34±1.41 μWcm-2) is significantly higher than those of CNT/PEI/hemin/PEI (27.87±0.95 μWcm-2) and CNT/PEI/hemin/PEI/GA (25.57±1.32 μWcm-2), demonstrating again that the cathode using TPA has the best performance in HPRR.

주제어

표/그림 (7)

그림 Fig. 1. a) Chemical structures of GA and TPA, b) catalytic structure of CNT/PEI/hemin/PEI/TPA.
그림 Fig. 2. CVs of CNT/PEI/hemin/PEI/TPA prepared with different TPA concentration a) 0, b) 0.0005, c) 0.005, d) 0.05, e) 0.5, and f) 1 mg ml^-1) with or without 10mM H₂O₂ injection. g) The plot of current densities (at 0.2 V) of HPRR vs. TPA concentration. For CV tests, N₂ purged 0.1M PBS (pH 7.4) was used as an electrolyte and potential scan rate was 20 mV s^-1.
그림 Fig. 3. CVs of a) CNT/PEI/hemin/PEI, b) CNT/PEI/hemin/PEI/GA and c) CNT/PEI/hemin/PEI/TPA with or without 10 mM H₂O₂. d) Comparison of the redox reaction of hemin in the catalytsts. The N₂-purged 0.1 M PBS solution (pH 7.4) was employed as the electrolyte, and the scan rate was 20 mV s^-1.
그림 Fig. 4. CVs of a) CNT/PEI/hemin/PEI, b) CNT/PEI/hemin/PEI/GA, and c) CNT/PEI/hemin/PEI/TPA, and the plot of the scan rate vs. peak current densities of d) CNT/PEI/hemin/PEI, e) CNT/ PEI/hemin/PEI/GA, and f) CNT/PEI/hemin/PEI/TPA. The N₂-purged 10 mM H₂O₂ in 0.1 M PBS solution (pH 7.4) was employed as the electrolyte, and the scan rates were varied as 20, 40, 60, 80, 100, 120, 140, and 160 mV s^-1.
그림 Fig. 5. Nyquist plots of CNT/PEI/hemin/PEI, CNT/PEI/hemin/PEI/ GA, and CNT/PEI/hemin/PEI/TPA with 10 mM potassium ferricyanide in 0.1 M PBS.
그림 Fig. 6. a) Photograph of 3D printed flow-type membraneless fuel cell, and b) the polarization curves of HPFC using CNT/PEI/hemin/PEI, CNT/PEI/hemin/PEI/GA, and CNT/PEI/hemin/PEI/TPA as cathodes (10 mM H₂O₂ injected). For the test, 20 mL min^-1 (10 mM H₂O₂ in 0.1 M PBS) of fuel was supplied to the cell.
표 Table 1.MPD and OCV of CNT/PEI/hemin/PEI, CNT/PEI/hemin/ PEI/GA, and CNT/PEI/hemin/PEI/TPA

참고문헌 (17)

Fawzy, S., Osman, A.I., Doran, J. and Rooney, D.W., "StrateGies for Mitigation of Climate Change: A Review," Environ. Chem. Lett., 18(6), 2069-2094(2020).

상세보기
Chen, M. T., Duan, J. J., Feng, J. J., Mei, L. P., Jiao, Y., Zhang, L. and Wang, A. J., "Iron, Rhodium-codoped Ni 2 P Nanosheets Arrays Supported on Nickel Foam as an Efficient Bifunctional Electrocatalyst for Overall Water Splitting," J. Colloid Interface Sci., 605, 888-896(2022).

상세보기
Abe, J. O., Popoola, A. P. I., Ajenifuja, E. and Popoola, O. M., "Hydrogen Energy, Economy and Storage: Review and Recommendation," Int. J. Hydrog. Energy., 44(29), 15072-15086(2019).

상세보기
Fukuzumi, S., Yamada, Y. and Karlin, K. D., "Hydrogen Peroxide as a Sustainable Energy Carrier: Electrocatalytic Production of Hydrogen Peroxide and the Fuel Cell," Electrochim. Acta., 82, 493-511(2012).

상세보기
Miglbauer, E., Wojcik, P. J. and Glowacki, E. D., "Single-compartment hydrogen peroxide fuel cells with poly(3,4-ethylenedioxythiophene) cathodes," Chem. Commun., 54(84), 11873-11876(2018).

상세보기
Xue, Y., Wang, Y., Pan, Z. and Sayama, K., "Electrochemical and Photoelectrochemical Water Oxidation for Hydrogen Peroxide Production," Angew. Chem. Int. Ed., 60(19), 10469-10480(2021).

상세보기
Liu, J., Zou, Y., Jin, B., Zhang, K. and Park, J. H., "Hydrogen Peroxide Production from Solar Water Oxidation," ACS Energy Lett., 4(12), 3018-3027(2019).

상세보기
Wu, J., Mehmood, A., Zhang, G., Wu, S., Ali, G. and Kucernak, A., "Highly selective O 2 Reduction to H 2 O 2 Catalyzed by Cobalt Nanoparticles Supported on Nitrogen-doped Carbon in Alkaline Solution," ACS Catal., 11(9), 5035-5046(2021).

상세보기
Ji, J., Chung, Y. and Kwon, Y., "The effect of a vitamin B 12 based catalyst on hydrogen peroxide oxidation reactions and the performance evaluation of a membraneless hydrogen peroxide fuel cell under physiological pH conditions," J. Mater. Chem. C., 8(8), 2749-2755(2020).

상세보기
An, H., Jeon, H., Ji, J., Kwon, Y. and Chung, Y., "Amine Axial Ligand-coordinated Cobalt Phthalocyanine-based Catalyst for Flow-type Membraneless Hydrogen Peroxide Fuel Cell or Enzymatic Biofuel Cell," J. Energy Chem., 58, 463-471(2021).

상세보기
Jeon, S., An, H., Ji, J., Kwon, Y. and Chung, Y., "High Temperature-induced Myoglobin-mimic Catalytic Structure Having High Axial Ligand Content for One-compartment Hydrogen Peroxide Fuel Cells," Int. J. Energy Res., 46(4), 4142-4155(2022).

상세보기
Jeon, S., An, H. and Chung, Y., "High Performance of the Flowtype One-compartment Hydrogen Peroxide Fuel Cell using Buckypaper and Narrow Fuel Pathway under Physiological Conditions," Sustain. Energy Fuels., 6(3), 841-850(2022).

상세보기
Reuillard, B., Gentil, S., Carriere, M., Le Goff, A. and Cosnier, S., "Biomimetic Versus Enzymatic High-potential ElectrocataLytic Reduction of Hydrogen Peroxide on a Functionalized Carbon Nanotube Electrode," Chem. Sci., 6(9), 5139-5143(2015).

상세보기
Wang, G. X., Zhou, Y., Wang, M., Bao, W. J., Wang, K. and Xia, X. H., "Structure Orientation of Hemin Self-assembly Layer Determining the Direct Electron Transfer Reaction," ChemComm., 51(4), 689-692(2015).
Chung, Y., Hyun, K. H. and Kwon, Y., "Fabrication of a Biofuel Cell Improved by the π-Conjugated Electron Pathway Effect Induced from a New Enzyme Catalyst Employing Terephthalaldehyde," Nanoscale., 8(2), 1161-1168(2016).

상세보기
Hyun, K. H., Han, S. W., Koh, W. G. and Kwon, Y., "Fabrication of Biofuel Cell Containing Enzyme Catalyst Immobilized by Layerby-layer Method," J. Power Sources., 286, 197-203(2015).

상세보기
Chung, Y., Christwardana, M., Tannia, D. C., Kim, K. J. and Kwon, Y., "Biocatalyst Including Porous Enzyme Cluster Composite Immobilized by Two-step Crosslinking and Its Utilization as Enzymatic Biofuel Cell," J. Power Sources., 360, 172-179(2017).

상세보기

저자의 다른 논문 :

표제어: PCR

동의어: Packet Collision Rate

용어 설명 출처 목록 (6)

용어 설명: PCR은 세균 특이성이 있는 primer를 이용하여 적은 수의 세균이 있을지라도 쉽게 검출할 수 있는 유용한 방법이며, 이를 이용하여 구강 내 치면세균막이나 타액에서 직접 세균을 검출할 수 있게 되었다[8].

내보내기 구분	파일저장 인쇄 메일전송
구성항목	기본정보 상세정보 관리번호, 논문명, 저널/프로시딩명, 저자 , 발행년, 권, 호, 시작페이지, 끝페이지, 발행기관 관리번호, 논문명, 대등논문명, 저자 , 저널/프로시딩명, 발행기관, 발행년, 발행언어, 권, 호, 시작페이지, 끝페이지, ISBN, ISSN, 주제분야, 키워드, 초록(한글), 초록(영문), 저자(소속기관)
저장형식	Text(ASCII format) Excel format RefWorks Direct Export RIS format (for Reference Manager, ProCite, EndNote), Scholar's Aids, Mendeley
메일정보	받는사람 (필수) @ 보내는사람 (선택) @ 제목 내용 KISTI 검색결과 이메일 서비스
안내	총 건의 자료가 검색되었습니다. 다운받으실 자료의 인덱스를 입력하세요. (1-10,000) 검색결과의 순서대로 최대 10,000건 까지 다운로드가 가능합니다. 데이타가 많을 경우 속도가 느려질 수 있습니다.(최대 2~3분 소요) 다운로드 파일은 UTF-8 형태로 저장됩니다. 파일의 내용이 제대로 보이지 않을실 때는 웹브라우저 상단의 보기 -> 인코딩 -> 자동선택 여부를 확인하십시오. ~ Text(ASCII format) Excel format