@kist.re.kr
Korea Institute of Science and Technology (KIST)
Materials Chemistry, Energy, Electrochemistry, Organic Chemistry
Scopus Publications
Scholar Citations
Scholar h-index
Scholar i10-index
In Taek Song, Joonkoo Kang, Jongkwan Koh, Hyunju Choi, Heemyeong Yang, Eunkyung Park, Jina Lee, Woohyung Cho, Yu-mi Lee, Seokkyeong Lee,et al.
Springer Science and Business Media LLC
A‐Re Jeon, Byeol Yi Han, Minhyung Kwon, Seung‐Ho Yu, Kyung Yoon Chung, Jimin Shim, and Minah Lee
Wiley
AbstractThe intrinsic reactivity of lithium (Li) toward ambient air, combined with insufficient cycling stability in conventional electrolytes, hinders the practical adoption of Li metal anodes in rechargeable batteries. Here, a bilayer interphase for Li metal is introduced to address both its susceptibility to corrosion in ambient air and its deterioration during cycling in carbonate electrolytes. Initially, the Li metal anode is coated with a conformal bottom layer of polysiloxane bearing methacrylate, followed by further grafting with poly(vinyl ethylene carbonate) (PVEC) to enhance anti‐corrosion capability and electrochemical stability. In contrast to single‐layer applications of polysiloxane or PVEC, the bilayer design offers a highly uniform coating that effectively resists humid air and prevents dendritic Li growth. Consequently, it demonstrates stable plating/stripping behavior with only a marginal increase in overpotential over 200 cycles in carbonate electrolytes, even after exposure to ambient air with 46% relative humidity. The design concept paves the way for scalable production of high‐voltage, long‐cycling Li metal batteries.
Seungyun Jeon, Sehee lm, Inyeong Kang, Dongki Shin, Seung‐Ho Yu, Minah Lee, and Jihyun Hong
Wiley
AbstractLithium‐ion capacitors (LICs) exhibit superior power density and cyclability compared to lithium‐ion batteries. However, the low initial Coulombic efficiency (ICE) of amorphous carbon anodes (e.g., hard carbon (HC) and soft carbon (SC)) limits the energy density of LICs by underutilizing cathode capacity. Here, a solution‐based deep prelithiation strategy for carbon anodes is applied using a contact‐ion pair dominant solution, offering high energy density based on a systematic electrode balancing based on the cathode capacity increased beyond the original theoretical limit. Increasing the anode ICE to 150% over 100%, the activated carbon (AC) capacity is doubled by activating Li+ cation storage, which unleashes rocking‐chair LIC operation alongside the dual‐ion‐storage mechanism. The increased AC capacity results in an energy density of 106.6 Wh kg−1AC+SC, equivalent to 281% of that of LICs without prelithiation. Moreover, this process lowers the cathode‐anode mass ratio, reducing the cell thickness by 67% without compromising the cell capacity. This solution‐based deep chemical prelithiation promises high‐energy LICs based on transition metal‐free, earth‐abundant active materials to meet the practical demands of power‐intensive applications.
Sunghyun Ko, Jinkwan Choi, Jihyun Hong, Changsoo Kim, Uichan Hwang, Minhyung Kwon, Gukhyun Lim, Seok Su Sohn, Jinha Jang, Ung Lee,et al.
Royal Society of Chemistry (RSC)
We establish thermodynamically controlled Li-coupled electron transfer from recyclable electron donors to cathodes as a viable route for directly regenerating spent cathodes under ambient conditions.
Suyeon Oh, A-Re Jeon, Gukhyun Lim, Min Kyung Cho, Keun Hwa Chae, Seok Su Sohn, Minah Lee, Sung-Kyun Jung, and Jihyun Hong
Elsevier BV
Gukhyun Lim, Min Kyung Cho, Jaewon Choi, Ke-Jin Zhou, Dongki Shin, Seungyun Jeon, Minhyung Kwon, A-Re Jeon, Jinkwan Choi, Seok Su Sohn,et al.
Royal Society of Chemistry (RSC)
Stabilizing lattice oxygen at the electrochemical interface of Li-/Mn-rich cathodes preferentially promotes layered-to-spinel phase transition and suppresses rocksalt phase formation, offering excellent capacity retention.
Min-Gi Jeong, Hyun Ho Lee, Hyeon-Ji Shin, Yeseul Jeong, Jang-Yeon Hwang, Won-Jin Kwak, Gwangseok Oh, Wonkeun Kim, Kyounghan Ryu, Seungho Yu,et al.
Royal Society of Chemistry (RSC)
The introduction of CF3(CF2)2I into the electrolyte leads to the simultaneous formation of LiI as a redox mediator and LiF as a protective layer. This enables long cycle life and high reversibility even at high areal capacity (∼5 mA h cm−2).
A-Re Jeon, Seungyun Jeon, Gukhyun Lim, Juyoung Jang, Woo Joo No, Si Hyoung Oh, Jihyun Hong, Seung-Ho Yu, and Minah Lee
American Chemical Society (ACS)
Rechargeable magnesium (Mg) batteries can offer higher volumetric energy densities and be safer than their conventional counterparts, lithium-ion batteries. However, their practical implementation is impeded due to the passivation of the Mg metal anode or the severe corrosion of the cell parts in conventional electrolyte systems. Here, we present a chemical activation strategy to facilitate the Mg deposition/stripping process in additive-free simple salt electrolytes. By exploiting the simple immersion-triggered spontaneous chemical reaction between reactive organic halides and Mg metal, the activated Mg anode exhibited an overpotential below 0.2 V and a Coulombic efficiency as high as 99.5% in a Mg(TFSI)2 electrolyte. Comprehensive analyses reveal simultaneous evolution of morphology and interphasial chemistry during the activation process, through which stable Mg cycling over 990 cycles was attained. Our activation strategy enabled the efficient cycling of Mg full-cell candidates using commercially available electrolytes, thereby offering possibilities of building practical Mg batteries.
Jina Lee, A-Re Jeon, Hye Jin Lee, Ukseon Shin, Yiseul Yoo, Hee-Dae Lim, Cheolhee Han, Hochun Lee, Yong Jin Kim, Jayeon Baek,et al.
Royal Society of Chemistry (RSC)
Concurrent modification of linear carbonates combining alkyl-chain extension and alkoxy substitution enables thermally stable high-performance batteries by decreasing volatility and increasing solvation ability simultaneously.
Sanghyuk Gong, Yeongje Lee, Jinkwan Choi, Minah Lee, Kyung Yoon Chung, Hun‐Gi Jung, Sunho Jeong, and Hyung‐Seok Kim
Wiley
AbstractSiOx is a promising next‐generation anode material for lithium‐ion batteries. However, its commercial adoption faces challenges such as low electrical conductivity, large volume expansion during cycling, and low initial Coulombic efficiency. Herein, to overcome these limitations, an eco‐friendly in situ methodology for synthesizing carbon‐containing mesoporous SiOx nanoparticles wrapped in another carbon layers is developed. The chemical reactions of vinyl‐terminated silanes are designed to be confined inside the cationic surfactant‐derived emulsion droplets. The polyvinylpyrrolidone‐based chemical functionalization of organically modified SiO2 nanoparticles leads to excellent dispersion stability and allows for intact hybridization with graphene oxide sheets. The formation of a chemically reinforced heterointerface enables the spontaneous generation of mesopores inside the thermally reduced SiOx nanoparticles. The resulting mesoporous SiOx‐based nanocomposite anodes exhibit superior cycling stability (≈100% after 500 cycles at 0.5 A g−1) and rate capability (554 mAh g−1 at 2 A g−1), elucidating characteristic synergetic effects in mesoporous SiOx‐based nanocomposite anodes. The practical commercialization potential with a significant enhancement in initial Coulombic efficiency through a chemical prelithiation reaction is also presented. The full cell employing the prelithiated anode demonstrated more than 2 times higher Coulombic efficiency and discharge capacity compared to the full cell with a pristine anode.
Gukhyun Lim, Dongki Shin, Keun Hwa Chae, Min Kyung Cho, Chan Kim, Seok Su Sohn, Minah Lee, and Jihyun Hong
Wiley
AbstractThe exploding electric‐vehicle market requires cost‐effective high‐energy materials for rechargeable lithium batteries. The manganese‐rich spinel oxide LiNi0.5Mn1.5O4 (LNMO) can store a capacity greater than 200 mAh g−1 based on the multi‐cation (Ni2+/Ni4+ and Mn3+/Mn4+) redox centers. However, its practical capacity is limited to Ni2+/Ni4+ redox (135 mAh g−1) due to the poor reversibility of Mn3+/Mn4+ redox. This instability is generally attributed to the Jahn–Teller distortion of Mn3+ and its disproportionation, which leads to severe Mn dissolution. Herein, for the first time, the excellent reversibility of Mn3+/Mn4+ redox within 2.3–4.3 V is demonstrated, requiring revisiting the previous theory. LNMO loses capacity only within a wide voltage range of 2.3–4.9 V. It is revealed that a dynamic evolution of the electrochemical interface, for example, potential‐driven rocksalt phase formation and decomposition, repeatedly occurs during cycling. The interfacial evolution induces electrolyte degradation and surface passivation, impeding the charge‐transfer reactions. It is further demonstrated that stabilizing the interface by electrolyte modification extends the cycle life of LNMO while using the multi‐cation redox, enabling 71.5% capacity retention of LNMO after 500 cycles. The unveiled dynamic oxide interface will propose a new guideline for developing Mn‐rich cathodes by realizing the reversible Mn redox.
Sunghyun Ko, Yiseul Yoo, Jinkwan Choi, Hee-Dae Lim, Chan Beum Park, and Minah Lee
Royal Society of Chemistry (RSC)
We present a series of organic redox mediators (RMs) for ambient air operational LABs. The selected RMs capable of decomposing Li2O2 can not only facilitate Li2CO3 oxidation but also inhibit 1O2 generation during the charging process.
Minseok Lee, Minji Jeong, Youn Shin Nam, Janghyuk Moon, Minah Lee, Hee-Dae Lim, Dongjin Byun, Taeeun Yim, and Si Hyoung Oh
Elsevier BV
Minhyung Kwon, Jina Lee, Sunghyun Ko, Gukhyun Lim, Seung-Ho Yu, Jihyun Hong, and Minah Lee
Royal Society of Chemistry (RSC)
A synthetic method to construct a highly stable, densely packed Zn anode is presented by provoking the unusual Cu–Zn alloying alongside Zn plating. The compact Zn anode retains its morphology over repeated plating/stripping cycles in aqueous media.
Jinkwan Choi, Hyangsoo Jeong, Juyoung Jang, A-Re Jeon, Inyeong Kang, Minhyung Kwon, Jihyun Hong, and Minah Lee
American Chemical Society (ACS)
Although often overlooked in anode research, the anode's initial Coulombic efficiency (ICE) is a crucial factor dictating the energy density of a practical Li-ion battery. For next-generation anodes, a blend of graphite and Si/SiOx represents the most practical way to balance capacity and cycle life, but its low ICE limits its commercial viability. Here, we develop a chemical prelithiation method to maximize the ICE of the blend anodes using a reductive Li-arene complex solution of regulated solvation power, which enables a full cell to exhibit a near-ideal energy density. To prevent structural degradation of the blend during prelithiation, we investigate a solvation rule to direct the Li+ intercalation mechanism. Combined spectroscopy and density functional theory calculations reveal that in weakly solvating solutions, where the Li+-anion interaction is enhanced, free solvated-ion formation is inhibited during Li+ desolvation, thereby mitigating solvated-ion intercalation into graphite and allowing stable prelithiation of the blend. Given the ideal ICE of the prelithiated blend anode, a full cell exhibits an energy density of 506 Wh kg-1 (98.6% of the ideal value), with a capacity retention after 250 cycles of 87.3%. This work highlights the promise of adopting chemical prelithiation for high-capacity anodes to achieve practical high-energy batteries.
Tan Tan Bui, Boseon Yun, Kwabena Darko, Seung Beom Shin, Jaehyun Kim, Jongin Hong, Minah Lee, Sung Kyu Park, and Myung‐Gil Kim
Wiley
AbstractLithium‐rich amorphous Li‐La‐Zr‐O (a‐Li‐La‐Zr‐O) electrolyte is successfully synthesized using sol–gel processing method. With unlimited compositions of the amorphous structure, lithium‐rich compositions are systematically investigated to determine optimal composition and optimized processing conditions of a‐Li‐La‐Zr‐O coatings. There is an improvement in ionic conductivity of a‐Li‐La‐Zr‐O with Li content increasing, specifically from 3.0 × 10−8 S cm−1 (Li8La2Zr2O11) to 1.18 × 10−6 S cm−1 (Li18La2Zr2O16), thereby resulting in low activation energy. The high‐ionic‐conductivity a‐Li‐La‐Zr‐O is implemented as an artificial solid electrolyte interface coating layer on cathode materials. The a‐Li‐La‐Zr‐O‐coated LiCoO2 (LCO) and LiNi0.8Mn0.1Co0.1O2 (NMC 811) coin cells exhibit better cycling performance than the bare coin cell at the optimum compositional ratio of a‐Li‐La‐Zr‐O. A‐Li‐La‐Zr‐O can be a promising material for solid electrolyte battery and a potential coating layer for the modification of cathode surface.
Juyoung Jang, Inyeong Kang, Jinkwan Choi, Hyangsoo Jeong, Kyung‐Woo Yi, Jihyun Hong, and Minah Lee
Wiley
AbstractPrelithiation is of great interest to Li‐ion battery manufacturers as a strategy for compensating for the loss of active Li during initial cycling of a battery, which would otherwise degrade its available energy density. Solution‐based chemical prelithiation using a reductive chemical promises unparalleled reaction homogeneity and simplicity. However, the chemicals applied so far cannot dope active Li in Si‐based high‐capacity anodes but merely form solid–electrolyte interphases, leading to only partial mitigation of the cycle irreversibility. Herein, we show that a molecularly engineered Li–arene complex with a sufficiently low redox potential drives active Li accommodation in Si‐based anodes to provide an ideal Li content in a full cell. Fine control over the prelithiation degree and spatial uniformity of active Li throughout the electrodes are achieved by managing time and temperature during immersion, promising both fidelity and low cost of the process for large‐scale integration.
Zhiao Yu, David G. Mackanic, Wesley Michaels, Minah Lee, Allen Pei, Dawei Feng, Qiuhong Zhang, Yuchi Tsao, Chibueze V. Amanchukwu, Xuzhou Yan,et al.
Elsevier BV
Vivian Rachel Feig, Helen Tran, Minah Lee, Kathy Liu, Zhuojun Huang, Levent Beker, David G. Mackanic, and Zhenan Bao
Wiley
AbstractDue to their high water content and macroscopic connectivity, hydrogels made from the conducting polymer PEDOT:PSS are a promising platform from which to fabricate a wide range of porous conductive materials that are increasingly of interest in applications as varied as bioelectronics, regenerative medicine, and energy storage. Despite the promising properties of PEDOT:PSS‐based porous materials, the ability to pattern PEDOT:PSS hydrogels is still required to enable their integration with multifunctional and multichannel electronic devices. In this work, a novel electrochemical gelation (“electrogelation”) method is presented for rapidly patterning PEDOT:PSS hydrogels on any conductive template, including curved and 3D surfaces. High spatial resolution is achieved through use of a sacrificial metal layer to generate the hydrogel pattern, thereby enabling high‐performance conducting hydrogels and aerogels with desirable material properties to be introduced into increasingly complex device architectures.
Yuchi Tsao, Minah Lee, Elizabeth C. Miller, Guoping Gao, Jihye Park, Shucheng Chen, Toru Katsumata, Helen Tran, Lin-Wang Wang, Michael F. Toney,et al.
Elsevier BV
Vivian R. Feig, Helen Tran, Minah Lee, and Zhenan Bao
Springer Science and Business Media LLC
The original version of this Article contained an error in the second sentence of the ‘Materials’ section of the Methods, which incorrectly read ‘PEDOT:PSS synthesized by Orgacon (739324 Aldrich, MDL MFCD07371079) was purchased as a surfactant-free aqueous dispersion with 1.1 wt% solid content.’ The correct version replaces this sentence with ‘PEDOT:PSS Orgacon ICP 1050 was provided by Agfa as a surfactant-free aqueous dispersion with 1.1 wt% solid content.’ This has been corrected in both the PDF and HTML versions of the Article.
Vivian R. Feig, Helen Tran, Minah Lee, and Zhenan Bao
Springer Science and Business Media LLC
AbstractConductive and stretchable materials that match the elastic moduli of biological tissue (0.5–500 kPa) are desired for enhanced interfacial and mechanical stability. Compared with inorganic and dry polymeric conductors, hydrogels made with conducting polymers are promising soft electrode materials due to their high water content. Nevertheless, most conducting polymer-based hydrogels sacrifice electronic performance to obtain useful mechanical properties. Here we report a method that overcomes this limitation using two interpenetrating hydrogel networks, one of which is formed by the gelation of the conducting polymer PEDOT:PSS. Due to the connectivity of the PEDOT:PSS network, conductivities up to 23 S m−1 are achieved, a record for stretchable PEDOT:PSS-based hydrogels. Meanwhile, the low concentration of PEDOT:PSS enables orthogonal control over the composite mechanical properties using a secondary polymer network. We demonstrate tunability of the elastic modulus over three biologically relevant orders of magnitude without compromising stretchability ( > 100%) or conductivity ( > 10 S m−1).
Jihye Park, Allison C. Hinckley, Zhehao Huang, Dawei Feng, Andrey A. Yakovenko, Minah Lee, Shucheng Chen, Xiaodong Zou, and Zhenan Bao
American Chemical Society (ACS)
Conductive metal-organic frameworks (c-MOFs) have shown outstanding performance in energy storage and electrocatalysis. Varying the bridging metal species and the coordinating atom are versatile approaches to tune their intrinsic electronic properties in c-MOFs. Herein we report the first synthesis of the oxygen analog of M3(C6X6)2 (X = NH, S) family using Cu(II) and hexahydroxybenzene (HHB), namely Cu-HHB [Cu3(C6O6)2], through a kinetically controlled approach with a competing coordination reagent. We also successfully demonstrate an economical synthetic approach using tetrahydroxyquinone as the starting material. Cu-HHB was found to have a partially eclipsed packing between adjacent 2D layers and a bandgap of approximately 1 eV. The addition of Cu-HHB to the family of synthetically realized M3(C6X6)2 c-MOFs will enable greater understanding of the influence of the organic linkers and metals, and further broadens the range of applications for these materials.
Jeffrey Lopez, Yongming Sun, David G. Mackanic, Minah Lee, Amir M. Foudeh, Min‐Sang Song, Yi Cui, and Zhenan Bao
Wiley
AbstractSolid‐state electrolyte materials are attractive options for meeting the safety and performance needs of advanced lithium‐based rechargeable battery technologies because of their improved mechanical and thermal stability compared to liquid electrolytes. However, there is typically a tradeoff between mechanical and electrochemical performance. Here an elastic Li‐ion conductor with dual covalent and dynamic hydrogen bonding crosslinks is described to provide high mechanical resilience without sacrificing the room‐temperature ionic conductivity. A solid‐state lithium‐metal/LiFePO4 cell with this resilient electrolyte can operate at room temperature with a high cathode capacity of 152 mAh g−1 for 300 cycles and can maintain operation even after being subjected to intense mechanical impact testing. This new dual crosslinking design provides robust mechanical properties while maintaining ionic conductivity similar to state‐of‐the‐art polymer‐based electrolytes. This approach opens a route toward stable, high‐performance operation of solid‐state batteries even under extreme abuse.
David G. Mackanic, Wesley Michaels, Minah Lee, Dawei Feng, Jeffrey Lopez, Jian Qin, Yi Cui, and Zhenan Bao
Wiley
AbstractSolid polymer electrolytes (SPEs) promise to improve the safety and performance of lithium ion batteries (LIBs). However, the low ionic conductivity and transference number of conventional poly(ethylene oxide) (PEO)‐based SPEs preclude their widespread implementation. Herein, crosslinked poly(tetrahydrofuran) (xPTHF) is introduced as a promising polymer matrix for “beyond PEO” SPEs. The crosslinking procedure creates thermally stable, mechanically robust membranes for use in LIBs. Molecular dynamics and density functional theory (DFT) simulations accompanied by 7Li NMR measurements show that the lower spatial concentration of oxygen atoms in the xPTHF backbone leads to loosened O–Li+ coordination. This weakened interaction enhances ion transport; xPTHF has a high lithium transference number of 0.53 and higher lithium conductivity than a xPEO SPE of the same length at room temperature. It is demonstrated that organic additives further weaken the O–Li+ interaction, enabling room temperature ionic conductivity of 1.2 × 10−4 S cm−1 with 18 wt% N,N‐dimethylformamide in xPTHF. In a solid‐state LIB application, neat xPTHF SPEs cycle with near theoretical capacity for 100 cycles at 70 °C, with rate capability up to 1 C. The plasticized xPTHF SPEs operate at room temperature while maintaining respectable rate capability and capacity. The novel PTHF system demonstrated here represents an exciting platform for future studies involving SPEs.