[논문]과량의 니켈 첨가로 합성된 NiO와 Co3O4가 도핑된 La(CoNi)O3 페로브스 카이트의 알칼리용액에서 산소환원 및 발생반응 특성

버링; 임형렬; 이홍기; 박경세; 심중표

doi:10.7316/khnes.2021.32.1.41

과량의 니켈 첨가로 합성된 NiO와 Co3O4가 도핑된 La(CoNi)O3 페로브스 카이트의 알칼리용액에서 산소환원 및 발생반응 특성
Characterization of NiO and Co3O4-Doped La(CoNi)O3 Perovskite Catalysts Synthesized from Excess Ni for Oxygen Reduction and Evolution Reaction in Alkaline Solution 원문보기

한국수소 및 신에너지학회 논문집 = Transactions of the Korean Hydrogen and New Energy Society, v.32 no.1, 2021년, pp.41 - 52

버링 (군산대학교 나노화학공학과) , 임형렬 (우석대학교 연료전지 지역혁신센터) , 이홍기 (우석대학교 연료전지 지역혁신센터) , 박경세 (군산대학교 화학과) , 심중표 (군산대학교 나노화학공학과)

Abstract ▼ AI-Helper

NiO and Co3O4-doped porous La(CoNi)O3 perovskite oxides were prepared from excess Ni addition by a hydrothermal method using porous silica template, and characterized as bifunctional catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) for Zn-air rechargeable batteries in alkaline solution. Excess Ni induced to form NiO and Co3O4 in La(CoNi)O3 particles. The NiO and Co3O4-doped porous La(CoNi)O3 showed high specific surface area, up to nine times of conventionally synthesized perovskite oxide, and abundant pore volume with similar structure. Extra added Ni was partially substituted for Co as B site of ABO3 perovskite structure and formed to NiO and Co3O4 which was highly dispersed in particles. Excess Ni in La(CoNi)O3 catalysts increased OER performance (259 mA/㎠ at 2.4 V) in alkaline solution, although the activities (211 mA/㎠ at 0.5 V) for ORR were not changed with the content of excess Ni. La(CoNi)O3 with excess Ni showed very stable cyclability and low capacity fading rate (0.38 & 0.07 ㎶/hour for ORR & OER) until 300 hours (~70 cycles) but more excess content of Ni in La(CoNi)O3 gave negative effect to cyclability.

주제어

표/그림 (12)

그림 Fig. 1. Schematic diagram of synthetic process and oxygen reaction on catalyst
표 Table 1. BET properties and crystalline size of LCO and LCNx samples
그림 Fig. 2. XRD patterns of prepared catalysts
그림 Fig. 3. SEM images of (a) LCO, (b) LCN0.2, (c) LCN0.4, and (d) LCN0.8 catalysts
그림 Fig. 4. TEM images of (a) LCO, (b) LCN0.2, (c) LCN0.4, and (d) LCN0.8 catalysts
그림 Fig. 6. La 3d and Ni 2p core level spectra of X-ray photo-electron spectroscopy for LCO and LCNx
그림 Fig. 5. (a) Pore size distributions and (b) nitrogen adsorp-tion- desorption isotherms of LCO and LCNx
그림 Fig. 7. Co 2p_3/2 (a-d) and O 1s (e-h) XPS spectra and repre-sentative fitting for four different catalysts (a, e) LCO, (b, f) LCN0.2, (c, g) LCN0.4, and (d, h) LCN0.8, respectively
표 Table 2. Surface atomic ratios of different samples derived from XPS
그림 Fig. 9. Charge/discharge cycling of (a) LCO, (b) LCN0.2, (c) LCN0.4 and (d) LCN0.8 at 20 mA/cm² with 2 hours per step
그림 Fig. 8. (a) Linear sweep voltammograms, (b) current of 20th cycle at 0.5 and 2.4 V, and Tafel slopes of (c) ORR and (d) OER for LCO and LCNx electrodes
표 Table 3. Summary of stability test for continuous cycling

AI 본문요약
AI-Helper

* AI 자동 식별 결과로 적합하지 않은 문장이 있을 수 있으니, 이용에 유의하시기 바랍니다.

제안 방법

The electrochemical characterization of the bi functional air electrodes for ORR and OER was conducted in an 8 M KOH solution using a three-elec- trode system. The working electrode was cut into a round shape which area is 1 cm².
In the three-elec- trode system, KOH solution was contact with the catalytic layer and the air went to catalytic layer through the gas diffusion layer (carbon paper). The linear sweep voltammetry (LSV) was conducted to measure current according to cell potential using a potentio- stat/galvanostat (WBCS3000, WonATech Co. Ltd., Seoul, Korea). The cell potential was scanned at a scan rate of 1 mV/s for 20 times between 0.
The physical and chemical properties of samples were characterized by X-ray diffraction (XRD, PANalytical, EMPYREAN), field emission-scanning electron microscopy (FE-SEM, SU8220, Hitachi, Tokyo, Japan), X-ray photoelectron spectroscopy (XPS, JEM-ARM200F, JEOL, Tokyo, Japan) and their surface areas were measured using a BET method (BELSORP-MAX, MicrotracBEL Corp, Tokyo, Japan).
The stability tests of LCO and LCNx for continuous cycles were conducted at current of 20 mA/cm² for 2 hours of ORR & OER, respectively. As shown in Fig.

대상 데이터

The working electrode was cut into a round shape which area is 1 cm². The counter and reference electrodes were used a Pt mesh (Alfa Aesar, Haverhill, MA, USA) and a Zn wire (a diameter of 1 mm, Aldrich), respectively. In the three-elec- trode system, KOH solution was contact with the catalytic layer and the air went to catalytic layer through the gas diffusion layer (carbon paper).

이론/모형

The surface areas and pore size distributions were estimated by N₂ adsorption-desorption isotherms and calculated based on the Brunauer-Emmett-Teller (BET) method, as shown in Fig. 5 and listed in Table 1. The BET specific surface area of LCNx synthesized using porous template are much larger than traditional synthesized perovskite oxides.

참고문헌 (34)

Y. Li, H. Dai, "Recent advances in zinc-air batteries", Chem. Soc. Rev., Vol. 43, No. 15, 2014, pp. 5257-5275, doi: https://doi.org/10.1039/C4CS00015C.

상세보기
J. Jiang, Y. Li, J. Liu, X. Huang, C. Yuan, and X. W. Lou, "Recent advances in metal oxidebased electrode architecture design for electrochemical energy storage", Adv. Mater. Vol. 24, No. 38, 2012, pp. 5166-5180, doi: https://doi.org/10.1002/adma.201202146.

상세보기
S. Guo, S. Zhang, and S. Sun, "Tuning nanoparticle catalysis for the oxygen reduction reaction", Angew. Chem. Int. Ed., Vol. 52, No. 33, 2013, pp. 8526-8544, doi: https://doi.org/10.1002/anie.201207186.

상세보기
J. H. Yang, H. J. Sun, G. Park, J. C. An, and J. Shim. "Synthesis of highly porous LaCoO 3 catalyst by nanocasting and its performance for oxygen reduction and evolution reactions in alkaline solution", J. Electroceram., Vol. 41, 2018, pp. 80-87, doi: https://doi.org/10.1007/s10832-018-0165-7.

상세보기
V. Elayappan, R. Shanmugam, S. Chinnusamy, D. J. Yoo, G. Mayakrishnan, K. Kim, H. S. Noh, M. K. Kim, and H. Lee, "Three-dimensional bimetal TMO supported carbon based electrocatalyst developed via dry synthesis for hydrogen and oxygen evolution", Appl. Surf. Sci., Vol. 505, 2020, pp. 144642, doi: https://doi.org/10.1016/j.apsusc.2019.144642.

상세보기
R. Kannan, A. R. Kim, K. S. Nahm, H. K. Lee, and D. J. Yoo, "Synchronized synthesis of Pd@C-RGO carbocatalyst for improved anode and cathode performance for direct ethylene glycol fuel cell", Chem. Commun., Vol. 50, No. 93, 2014, pp. 14623-14626, doi: https://doi.org/10.1039/C4CC06879C.

상세보기
S. Ramakrishnan, M. Karuppannan, M. Vinothkannan, K. Ramachandran, O. J. Kwon, and D. J. Yoo, "Ultrafine Pt nanoparticles stabilized by MoS2/N-doped reduced graphene oxide as a durable electrocatalyst for alcohol oxidation and oxygen reduction reactions", ACS Appl. Mater. Interfaces, Vol. 11, No. 13, 2019, pp. 12504-12515, doi: https://doi.org/10.1021/acsami.9b00192.

상세보기
S. Ramakrishnan, J. Balamurugan, M. Vinothkannan, A. R. Kim, S. Sengodan, and D. J. Yoo, "Nitrogen-doped graphene encapsulated FeCoMoS nanoparticles as advanced trifunctional catalyst for water splitting devices and zinc-air batteries", Appl. Cat. B: Environ., Vol. 279, 2020, pp. 119381, doi: https://doi.org/10.1016/j.apcatb.2020.119381.

상세보기
Z. Chen, A. Yu, D. Higgins, H. Li, H. Wang, and Z. Chen, "Highly active and durable core-corona structured bifunctional catalyst for rechargeable metal-air battery application", Nano Lett., Vol. 12, No. 4, 2012, pp. 1946-1952, doi: https://doi.org/10.1021/nl2044327.

상세보기
W. G. Hardin, D. A. Slanac, X. Wang, S. Dai, K. P. Johnston, and K. J. Stevenson, "Highly active, nonprecious metal perovskite electrocatalysts for bifunctional metal-air battery electrodes", J. Phys. Chem. Lett., Vol. 4, 2013, pp. 1254-1259, doi: https://doi.org/10.1021/jz400595z.

상세보기
Y. Xue, S. Sun, Q. Wang, Z. Donga and Z. Liu, "Transition metal oxide-based oxygen reduction reaction electrocatalysts for energy conversion systems with aqueous electrolytes", J. Mater. Chem. A, Vol. 23, 2018, pp. 10595-10626, doi: https://doi.org/10.1039/c7ta10569j.

상세보기
Z. Shao and S. M. Haile, "A high-performance cathode for the next generation of solid-oxide fuel cells", Nature, Vol. 431, 2004, pp. 170-173, doi: https://doi.org/10.1038/nature02863.

상세보기
D. Zhang, Y. Song, Z. Du, L. Wang, Y. Li, and J. B. Goodenough, "Active LaNi 1-x FexO 3 bifunctional catalysts for air cathodes in alkaline media", J. Mater. Chem. A, Vol. 3, No. 18, 2015, pp. 9421-9426, doi: https://doi.org/10.1039/C5TA01005E.

상세보기
W. Zhou, R. Ran, and Z. Shao, "Progress in understanding and development of Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 3-δ -based cathodes for intermediate-temperature solid-oxide fuel cells: a review", J. Power Sources, Vol. 192, No. 2, 2009, pp. 231-246, doi: https://doi.org/10.1016/j.jpowsour.2009.02.069.

상세보기
K. Lopez, G. Park, H. J. Sun, J. C. An, S. Eom, and J. Shim, "Electrochemical characterizations of LaMO 3 (M Co, Mn, Fe, and Ni) and partially substituted LaNi x M 1-x O 3 (x 0.25 or 0.5) for oxygen reduction and evolution in alkaline solution", J. Appl. Electrochem., Vol. 45, 2015, pp. 313-323, doi: https://doi.org/10.1007/s10800-015-0798-z.

상세보기
S. W. Eom, C. W. Lee, M. S. Yun, and Y. K. Sun, "The roles and electrochemical characterizations of activated carbon in zinc air battery cathodes", Electrochim. Acta, Vol. 52, No. 4, 2006, pp. 1592-1595, doi: https://doi.org/10.1016/j.electacta.2006.02.067.

상세보기
J. J. Xu, D. Xu, Z. L. Wang, H. G. Wang, L. L. Zhang, and X. B. Zhang, "Synthesis of perovskitebased porous La 0.75 Sr 0.25 MnO 3 nanotubes as a highly efficient electrocatalyst for rechargeable lithium-oxygen batteries", Angew. Chem. Int. Ed., Vol. 52, No. 14, 2013, pp. 3887-3890, doi: https://doi.org/10.1002/anie.201210057.

상세보기
J. Deng, L. Zhang, H. Dai, and C. T. Au, "In situ hydrothermally synthesized mesoporous LaCoO 3 /SBA-15 catalysts: high activity for the complete oxidation of toluene and ethyl acetate", Appl. Cat. A: General, Vol. 352, No. 1-2, 2009, pp. 43-49, doi: https://doi.org/10.1016/j.apcata.2008.09.037.

상세보기
K. Kim, K. Lopez, H. J. Sun, J. C. An, G. Park, and J. Shim, "Electrochemical performance of bifunctional Co/graphitic carbon catalysts prepared from metal-organic frameworks for oxygen reduction and evolution reactions in alkaline solution", J. Appl. Electrochem., Vol. 48, 2018, pp. 1231-1241, doi: https://doi.org/10.1007/s10800-018-1245-8.

상세보기
J. Shim, K. J. Lopez, H. J. Sun, G. Park, J. C. An, S. Eom, S. Shimpalee, and J. W. Weidner, "Preparation and characterization of electrospun LaCoO 3 fibers for oxygen reduction and evolution in rechargeable Zn-air batteries", J. Appl. Electrochem., Vol. 45, 2015, pp. 1005-1012, doi: https://doi.org/10.1007/s10800-015-0868-2.

상세보기
R. Robert, L. Bocher, B. Sipos, M. Dobeli, and A. Weidenkaff, "Ni-doped cobaltates as potential materials for high temperature solar thermoelectric converters", Prog. Solid State Chem., Vol. 35, No. 2-4, 2007, pp. 447-455, doi: https://doi.org/10.1016/j.progsolidstchem.2007.01.020.

상세보기
S. Q. Chen and Y. Liu, "LaFe y Ni 1-y O 3 supported nickel catalysts used for steam reforming of ethanol", Int. J. Hydrogen Energy, Vol. 34, No. 11, 2009, pp. 4735-4746, doi: https://doi.org/10.1016/j.ijhydene.2009.03.048.

상세보기
M. Mousavi and A. N. Pour, "Performance and structural features of LaNi 0.5 Co 0.5 O 3 perovskite oxides for the dry reforming of methane: influence of the preparation method", New J. Chem., Vol. 43, No. 27, 2019, pp. 10763-10773, doi: https://doi.org/10.1039/C9NJ01805K.

상세보기
M. Mao, J. Xu, M. Zhu, Y. Li, and Z. Liu, "Highly efficient catalytic hydrogen production of Co(OH) 2 -modified rare-earth perovskite LaNiO 3 composite under visible light", Appl Nanosci, Vol. 10, 2020, pp. 4361-4374, doi: https://doi.org/10.1007/s13204-020-01343-9.

상세보기
J. A. Villoria, M. C. Alvarez-Galvan, S. M. Al-Zahrani, P. Palmisano, S. Specchia, V. Specchia, J. L. G. Fierro, and R. M. Navarro, "Oxidative reforming of diesel fuel over LaCoO 3 perovskite derived catalysts: influence of perovskite synthesis method on catalyst properties and performance", Appl. Catalysis B: Environmental, Vol. 105, No. 3-4, 2011, pp. 276-288, doi: https://doi.org/10.1016/j.apcatb.2011.04.010.

상세보기
M. C. Biesinger, B. P. Payne, A. P. Grosvenor, L. W. M. Lau, A. R. Gerson, and R. St. C. Smart, "Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Cr, Mn, Fe, Co and Ni", Appl. Surf. Sci., Vol. 257, No. 7, 2011, pp. 2717-2730, doi: https://doi.org/10.1016/j.apsusc.2010.10.051.

상세보기
J. F. Moulder, W. F. Stickle, P. E'Sobol, and K. D. Bomben, "Handbook of X-ray photoelectron spectroscopy", PerkinElmer Corporation, USA, 1992.
H. Wang, W. Xu, S. Richins, K. Liaw, L. Yan, M. Zhou, and H. Luo, "Polymer-assisted approach to LaCo 1-x Ni x O 3 network nanostructures as bifunctional oxygen electrocatalysts", Electrochim. Acta, Vol. 296, 2019, pp. 945-953, doi: https://doi.org/10.1016/j.electacta.2018.11.075.

상세보기
J. Yang and T. Sasaki, "Synthesis of CoOOH hierarchically hollow spheres by nanorod self-assembly through bubble templating", Chem. Mater., Vol. 20, No. 5, 2008, pp. 2049-2056, doi: https://doi.org/10.1021/cm702868u.

상세보기
P. T. Babar, A. C. Lokhande, M. G. Gang, B. S. Pawar, S. M. Pawar, and J. H. Kim, "Thermally oxidized porous NiO as an efficient oxygen evolution reaction (OER) electrocatalyst for electrochemical water splitting application", J. Ind. Eng. Chem., Vol. 60, 2018, pp. 493-497, doi: https://doi.org/10.1016/j.jiec.2017.11.037.

상세보기
J. Zhou, Y. Wang, X. Su, S. Gu, R. Liu, Y. Huang, S. Yan, J. Li, and S. Zhang, "Electrochemically accessing ultrathin Co (oxy)-hydroxide nanosheets and operando identifying their active phase for the oxygen evolution reaction", Energy Environ. Sci., Vol. 12, No. 2, 2019, pp. 739-746, doi: https://doi.org/10.1039/C8EE03208D.

상세보기
A. Bergmann, T. E. Jones, E. M. Moreno, D. Teschner, P. Chernev, M. Gliech, T. Reier, H. Dau, and P. Strasser, "Unified structural motifs of the catalytically active state of Co(oxyhydr)oxides during the electrochemical oxygen evolution reaction", Nature Cat., Vol. 1, 2018, pp. 711-719, doi: https://doi.org/10.1038/s41929-018-0141-2.

상세보기
A. Moysiadou, S. Lee, C. S. Hsu, H. M. Chen, and X. Hu, "Mechanism of oxygen evolution catalyzed by cobalt oxyhydroxide: cobalt superoxide species as a key intermediate and dioxygen release as a rate-determining step", J. Am. Chem. Soc., Vol. 142, No. 27, 2020, pp. 11901-11914, doi: https://doi.org/10.1021/jacs.0c04867.

상세보기
J. Huang, J. Chen, T. Yao, J. He, S. Jiang, Z. Sun, Q. Liu, W. Cheng, F. Hu, Y. Jiang, Z. Pan, and S. Wei, "CoOOH nanosheets with high mass activity for water oxidation", Angew. Chem., Vol. 54, No. 30, 2015, pp. 8722-8727, doi: https://doi.org/10.1002/anie.201502836.

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