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Received June 28, 2021
Accepted August 30, 2021
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귀금속 촉매에서 사용되는 질소 전구체가 산소 환원 반응의 활성에 미치는 영향
Effect of Nitrogen Precursors in Non-precious Metal Catalysts on Activity for the Oxygen Reduction Reaction
1한경대학교 식품생명화학공학부, 17579 경기도 안성시 중앙로 327 2 한경대학교
1School of Food Biotechnology and Chemical Engineering, Hankyong National University, 327 Jungang-ro, Anseong, 17579, Korea 2Research Center of Chemical Technology, Hankyong National University, 327 Jungang-ro, Anseong-si, Gyeonggi-do, 17579, Korea
jungw@hknu.ac.kr
Korean Chemical Engineering Research, February 2022, 60(1), 151-158(8), 10.9713/kcer.2022.60.1.151 Epub 24 January 2022
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Abstract
고가의 귀금속 촉매는 고분자 전해질 연료전지의 상업화에 걸림돌로 인식되어 저가의 비귀금속 촉매 연구가 활발하다. 본 연구에서는 Fe-N-C 촉매를 킬레이팅이 가능한 4가지 다른 질소 전구체 N,N,N’,N’-detramethylethylenediamine (TMEDA), 1,2-ethylenediamine (EDA), m-dicyanobenzene (DCB), dicyandiamide (DCDA)를 이용하여 700, 800, 900, 1000 °C에서 합성하였다. 촉매의 물리적 특성은 주사전자현미경, X선 회절분석기, 자동원소분석기를 이용하여 분석하였다. 이를 통해 촉매 표면 형태 및 원소의 분산도와 에너지 분산형 X-선 분광을 적용하여 Fe의 함량을 확인하였다. 또한 비금속 원소의 함량과 Fe의 담지 여부 등을 확인하였다. 전기화학적 특성은 순환 전압전류법과 선형주사전위법을 통해 촉매의 전기화학적 산소 환원에 대한 활성과 전자전달수 등을 분석하였다. 결과에 따르면 질소 전구체로 EDA를 사용하여 800 °C의 소성온도에서 합성한 촉매가 가장 높은 산소 환원 활성을 보였다. 이 연구 결과는 고가의 귀금속을 대체하기 위한 노력에 도움이 될 것으로 예상된다.
Iron and nitrogen coordinated carbon catalyst (Fe-N-C) is the most promising non-precious metal catalyst (NPMC) studied to alternate the Pt-group oxygen reduction reaction (ORR) catalyst. In this work, Fe/N/C type catalysts are prepared by four different nitrogen precursors; N, N, N’, N’-tetramethylethylenediamine (TMEDA), 1,2-ethylenediamine (EDA), m-dicyanobenzene (DCB), dicyandiamide (DCDA) which can chelate a transition metal; In addition, the catalysts conducted the pyrolysis process at four different temperatures of 700, 800, 900, 1000 °C to investigate the ORR activities depend on pyrolysis temperature and to find an appropriate temperature. The characterizations of catalysts were investigated by scanning electron microscope-energy dispersive X-ray spectrometer (SEM-EDS), X-ray diffraction (XRD), and element analysis (EA). The electrocatalytic activity was measured by ORR polarization, also the electron transfer number was calculated from the slope of the K-L plot. The FeNC-EDA-800 which were prepared at pyrolysis temperature of 800 °C with EDA showed better ORR activity than the other catalysts.
Keywords
References
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Lefevre M, Proietti E, Jaouen F, Dodelet JP, Science, 324, 71 (2009)
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Jung WS, Popov BN, ACS Sustain. Chem. Eng., 5(11), 9809 (2017)
Gewirth AA, Varnell JA, DiAscro AM, Chem. Rev., 118(5), 2313 (2018)
Zhang XR, Mollamahale YB, Lyu DD, Liang LZ, Yu F, Qing M, Du YH, Zhang XY, Tian ZQ, Shen PK, J. Catal., 372, 245 (2019)
Li J, Chen S, Li W, Wu R, Ibraheem S, Li J, Ding W, Li L, Wei Z, J. Mater. Chem. A, 6(32), 15504 (2018)
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Lee SJ, Kim SH, Lee SJ, Park NK, Lee JT, Kang M, Ceram. Int., 38(8), 6685 (2012)
Garcia A, Retuerto M, Dominguez C, et al., Appl. Catal. B: Environ., 264, 118507 (2020)
Kose M, Hepokur C, Karakas D, McKee V, Kurtoglu M, Polyhedron, 117, 652 (2016)
Ahmed MS, Begum H, Kim YB, J. Power Sources, 451, 227733 (2020)
Fofana D, Natarajan SK, Hamelin J, Benard P, Energy, 64, 398 (2014)
Mao ZX, Wang MJ, Liu L, Peng L, Chen S, Li L, Li J, Wei Z, Chinese J. Catal., 41(5), 799 (2020)
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Matter PH, Zhang L, Ozkan US, J. Catal., 239(1), 83 (2006)
Huang Y, Liu K, Kan S, Liu P, Hao R, Liu W, Wu Y, Liu H, Liu M, Liu K, Carbon, 171, 1 (2021)
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Sun RM, Yao YQ, Wang AJ, Fang KM, Zhang L, Feng JJ, J. Colloid Interface Sci., 592, 405 (2021)
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Jung WS, Popov BN, Catal. Today, 295, 65 (2017)
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Subramanian NP, Li XG, Nallathambi V, Kumaraguru SP, Colon-Mercado H, Wu G, Lee JW, Popov BN, J. Power Sources, 188(1), 38 (2009)
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Carrillo-Rodriguez JC, Garay-Tapia AM, Escobar-Morales B, et al., Int. J. Hydrog. Energy, 46(51), 26087 (2021)
Zhao H, Zhang Y, Li L, Geng X, Yang H, Zhou W, Sun C, An B, Chinese Chem. Lett., 32(1), 140 (2021)
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Wu Z, Li W, Xia Y, Webley P, Zhao D, J. Mater. Chem., 22(18), 8835 (2012)
