[논문]고성능 리튬-황 전지를 위한 금속산화물을 첨가한 탄소나노튜브 프리스탠딩 전극

신윤정; 정현서; 김은미; 김태윤; 정상문

doi:10.9713/kcer.2023.61.3.426

고성능 리튬-황 전지를 위한 금속산화물을 첨가한 탄소나노튜브 프리스탠딩 전극
Metal Oxides Decorated Carbon Nanotube Freestanding Electrodes for High Performance of Lithium-sulfur Batteries 원문보기

Korean chemical engineering research = 화학공학, v.61 no.3, 2023년, pp.426 - 438

신윤정 (충북대학교 화학공학과) , 정현서 (충북대학교 화학공학과) , 김은미 (충북대학교 화학공학과) , 김태윤 (에스엔피랩(주)) , 정상문 (충북대학교 화학공학과)

초록
AI-Helper

차세대 전지로 주목받는 리튬-황 전지는 높은 에너지 밀도를 갖는 반면, 황의 절연 특성, 셔틀 현상 그리고 부피팽창으로 인하여 상용화에 어려움이 있다. 본 연구에서는 경제적이고 간단한 진공여과 방법으로 바인더와 집전체가 없는 프리스탠딩 전극을 제조하였고 탄소나노튜브(CNT)를 황의 전기전도도 향상을 위하여 사용하였다. 여기서 CNT는 집전체와 도전재 역할을 동시에 수행하였다. 추가로 리튬폴리설파이드의 흡착에 용이한 금속산화물(MO_x, M=Ni, Mg)을 CNT/S 전극에 첨가함으로써 리튬-황 전지의 셔틀반응을 억제하였다. MO_x@CNT/S 전극은 금속산화물을 도입하지 않은 CNT/S 전극에 비해 높은 용량 특성과 사이클 안정성을 나타내었으며, 이는 금속산화물의 우수한 리튬폴리설파이드 흡착 특성으로 인하여 황 활물질의 손실을 억제한 결과이다. MO_x@CNT/S 전극 중에서 NiO를 도입한 NiO@CNT/S 전극은 1 C에서 780 mAh g^-1의 높은 방전용량을 나타내었고 200 사이클 후 134 mAh g^-1으로 극심한 용량 감소가 나타났다. MgO@CNT/S 전극은 비록 초기 사이클에 544 mAh g^-1의 낮은 방전용량을 나타냈지만, 200 사이클까지 용량을 90% 유지하는 우수한 사이클 안정성을 나타내었다. 고용량과 사이클 안정성 확보를 위하여 Ni:Mg를 0.7:0.3의 비율로 혼합한 Ni_0.7Mg_0.3O@CNT/S 전극은 755 mAh g^-1 (1 C)의 초기 방전용량과 200 사이클 후에도 90% 이상의 용량 유지율을 나타내었다. 따라서 이원 금속산화물의 CNT/S 프리스탠딩으로의 적용은 고용량 특성뿐만 아니라 가장 큰 문제인 리튬폴리설파이드의 용출을 효과적으로 개선하여 경제적이고 고성능 리튬-황 전지의 개발이 가능함을 시사한다.

Abstract ▼ AI-Helper

Lithium-sulfur batteries, recently attracting attention as next-generation batteries, have high energy density but are limited in application due to sulfur's insulating properties, shuttle phenomenon, and volume expansion. This study used an economical and simple vacuum filtration method to prepare a freestanding electrode without a binder and collector. Carbon nanotubes (CNTs) are used to improve the electrical conductivity of sulfur, where CNT also acts as both collector and conductor. In addition, metal oxides (MOx, M=Ni, Mg), which are easy to adsorb lithium polysulfide, are added to the CNT/S electrode to suppress the shuttle reaction in lithium-sulfur batteries, which is a result of suppressing the loss of active sulfur material due to the excellent adsorption of lithium polysulfide by metal oxides. The MOx@CNT/S electrode exhibited higher capacity characteristics and cycle stability than the CNT/S electrode without metal oxides. Among the MOx@CNT/S electrodes, the NiO@CNT/S electrode displayed a high discharge capacity of 780 mAh g-1 at 1 C and an extreme capacity decrease to 134 mAh g-1 after 200 cycles. Although the MgO@CNT/S electrode exhibited a low discharge rate of 544 mAh g-1 in the initial cycle, it showed good cycle stability with 90% of capacity retention up to 200 cycles. Further, to achieve high capacity and cycle stability, the Ni0.7Mg0.3O@CNT/S electrode, mixed with Ni:Mg in the ratio of 0.7:0.3, manifested an initial discharge rate of 755 mAh g-1 (1 C) and a capacity retention rate of more than 90% after 200 cycles. Therefore, applying binary metal oxides to CNT/S provides a freestanding electrode for developing economical and high-performance Li-S batteries, effectively improving lithium polysulfide's high capacity characteristics and dissolution.

주제어

표/그림 (12)

그림 Fig. 1. Scheme illustration of the synthesis of (a) metal oxides, and (b) freestanding MO_x@CNT/S electrodes.
그림 Fig. 2. TGA curves of hydrothermal materials as metal precursors at air atmospheric conditions.
$Fig. 3. X-ray diffraction patterns of (a) various materials before and after calcination, and (b) partially enlarged XRD patterns between 60º and 65º.$ 그림 Fig. 3. X-ray diffraction patterns of (a) various materials before and after calcination, and (b) partially enlarged XRD patterns between 60º and 65º.
그림 Fig. 4. FE-SEM images of (a) hydrothermal Ni precursor, (b) NiO, (c) MgO, (d) Ni_0.7Mg_0.3O powders, and EDS mapping images of (e) NiO, (f) MgO, and (g) Ni_0.7Mg_0.3O powders.
그림 Fig. 5. Chemical interaction and adsorption of metal oxides with lithium polysulfides (Li₂S₄). (a) Visual observation of lithium polysulfides (Li₂S₄) adsorption test, (b) UV-Vis spectra of Li₂S₄ solution upon adsorption by CNT and different metal oxides, XPS spectra for S 2p of (c) CNT, (d) NiO, (e) MgO, and (f) Ni_0.7Mg_0.3O adsorbed on Li₂S₄.
그림 Fig. 6. First-four cycle CV curves of the (a) CNT/S, (b) NiO@CNT/S, (c) MgO@CNT/S, and (d) Ni_0.7Mg_0.3O@CNT/S electrodes at a scan rate of 0.1 mV s^-1.
그림 Fig. 7. CV curves and peak current (I_p) versus square root of scan rates (ν^0.5) and linear fits of current peaks (a, a', b, and b') dependence on the scan rates for (a, b) CNT/S, (c, d) NiO@CNT/S, (e, f) MgO@CNT/S, and (g, h) Ni_0.7Mg_0.3O electrodes at different scan rates from 0.2 to 0.5 mV s^-1.
그림 Fig. 8. Charge-discharge curves of (a) CNT/S, (b) NiO@CNT/S, (c) MgO@CNT/S, and (d) Ni_0.7Mg_0.3O@CNT/S electrode based Li-S batteries.
그림 Fig. 9. Electrochemical performance of Li-S batteries. (a) cycling performance at 1 C rate and (b) rate capability of the CNT/S, NiO@CNT/S, MgO@CNT/S, and Ni_0.7Mg_0.3O@CNT/S electrode used Li-S batteries.
그림 Fig. 10. (a) Equivalent circuit model for electrochemical impedance spectroscopy (EIS) analysis. Nyquist plots of Li-S batteries with CNT/S and Ni_0.7Mg_0.3O@CNT/S electrodes at (b) fresh state and (c) after 10 cycles. (d) Relationship between imaginary resistance (Z') and inverse square root of angular speed (at ω^-0.5) for CNT/S and Ni_0.7Mg_0.3O@CNT/S electrodes.
그림 Fig. 11. Electrochemical properties of freestanding flexible Ni_0.7Mg_0.3O@CNT/S electrodes in flat state, folded state and 10 times folded state at a current density of 1 C. (a) cycling performance and (b) charge-discharge curves.
표 Table 1. EIS results and lithium ion diffusion coefficient (D_Li) of Li-S batteries with CNT/S and Ni_0.7Mg_0.3O@CNT/S electrodes

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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].

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