Korean Chemical Engineering Research

  • 제61권3호
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  • Pages.426-438
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  • 2023
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  • 0304-128X(pISSN)
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  • 2233-9558(eISSN)
한국화학공학회 (The Korean Institute of Chemical Engineers)
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고성능 리튬-황 전지를 위한 금속산화물을 첨가한 탄소나노튜브 프리스탠딩 전극

Metal Oxides Decorated Carbon Nanotube Freestanding Electrodes for High Performance of Lithium-sulfur Batteries

  • Yun Jung Shin (Department of Chemical Engineering, Chungbuk National University) ;
  • Hyeon Seo Jeong (Department of Chemical Engineering, Chungbuk National University) ;
  • Eun Mi Kim (Department of Chemical Engineering, Chungbuk National University) ;
  • Tae Yun Kim (SNPLab Co. Ltd.) ;
  • Sang Mun Jeong (Department of Chemical Engineering, Chungbuk National University)
  • 투고 : 2023.06.19
  • 심사 : 2023.07.15
  • 발행 : 2023.08.01
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초록

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(MOx, M=Ni, Mg)을 CNT/S 전극에 첨가함으로써 리튬-황 전지의 셔틀반응을 억제하였다. MOx@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. MOx@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 Ni0.7Mg0.3O@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.

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.

키워드

과제정보

본연구는 2022년도정부(산업통상자원부, 과학기술정보통신부)의 재원으로 한국에너지기술평가원(KETEP) (No. 20224000000070), 연구개발특구진흥재단-기술이전사업화 사업(R&BD) (2022-IT-RD-0106)의 지원을 받아 수행된 연구임.

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