Article
Chemistry, Multidisciplinary
Philipp Stehle, Daniel Rutz, Ali M. Bazzoun, Dragoljub Vrankovic, Montaha Anjass
Summary: LiDFP has been found to improve the performance of Si-containing anodes in pouch cells, with a concentration of 1 wt% being the most optimal. Higher concentrations of LiDFP lead to the formation of a more beneficial SEI film, resulting in less degradation of electrolyte components and better maintenance of the anode microstructure.
Article
Chemistry, Physical
Ming Chen, Xiehe Huang, Ciqing Yang, Yuanxiang Zhou, Ying Yang
Summary: Lithium-ion capacitors (LICs), as promising energy storage devices, have high energy density, high power density, and long cycle life. This study demonstrates a strategy of simultaneous prelithiation and compatible modification by introducing Li2S and LiDFOB as additives, which greatly improves the performance of LICs and provides new insights for the simplified fabrication of LICs.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Haneol Kang, Hoon Kim, Chuleun Yeom, Moon Jeong Park
Summary: In this study, electrolyte additives were designed and synthesized for lithium batteries with an Si-graphite composite (SGC) anode to improve their rate performance and cycle stability. A hybrid artificial solid-electrolyte interphase (SEI) was formed on the anode surface through a combination of fluoroethylene carbonate (FEC) and dilithium vinylphosphonate (VPLi), resulting in enhanced capacity retention and rate capability.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Nanoscience & Nanotechnology
Yujun Pan, Xiaoqun Qi, Haoran Du, Yongsheng Ji, Dan Yang, Zhenglu Zhu, Ying Yang, Long Qie, Yunhui Huang
Summary: In conventional lithium-ion batteries (LIBs), the consumption of active lithium (Li) ions during the formation of the solid electrolyte interphase causes irreversible Li loss, reducing the energy density. This study proposes the use of lithium selenide (Li2Se) as a cathode prelithiation additive for LIBs, which can be irreversibly converted into selenide (Se) and supply additional Li. The addition of Li2Se to the LiFePO4 (LFP) cathodes results in an increase in specific capacity and energy density without compromising other battery performance, making it an efficient prelithiation additive for high-energy LIBs.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Leyi Guo, Feifei Huang, Muzhi Cai, Junjie Zhang, Guoqiang Ma, Shiqing Xu
Summary: By synthesizing a high-purity solid lithium difluorobis(oxalato) phosphate (LiDFOP) in an ether-based electrolyte, an outstanding organic-inorganic hybrid solid electrolyte interphase (SEI) was obtained, leading to improved cycling performance of the metallic lithium anode.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Chemistry, Analytical
Ruqian Ding, Shiyu Tian, Kaicheng Zhang, Jingrui Cao, Yi Zheng, Weichao Tian, Xiaoyan Wang, Lizhi Wen, Li Wang, Guangchuan Liang
Summary: The growing interest in electric vehicles and energy storage systems has increased the demand for lithium-ion battery technologies capable of providing high capacity and high energy density. Prelithiation of cathodes is a simpler method compared to anode prelithiation, and many studies are focused on finding suitable cathode additives to enhance the electrochemical performance of existing lithium-ion batteries. Challenges in effective cathode prelithiation additives and the development direction of prelithiation technology are discussed in the article.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2021)
Article
Nanoscience & Nanotechnology
Manoj Gautam, Govind Kumar Mishra, Aakash Ahuja, Supriya Sau, Mohammad Furquan, Sagar Mitra
Summary: Direct-contact prelithiation is a facile, practical, and scalable method for silicon anode material, and the effects of prelithiation time, pressure, and temperature on cell performance have been studied. A synchronization strategy is proposed to achieve excellent cell performance.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Nanoscience & Nanotechnology
Lin-Bo Huang, Ge Li, Zhuo-Ya Lu, Jin-Yi Li, Lu Zhao, Yu Zhang, Xu-Dong Zhang, Ke-Cheng Jiang, Quan Xu, Yu-Guo Guo
Summary: The usage of trans-difluoroethylene carbonate (DFEC) as an electrolyte additive helps maintain the structural integrity of microsized SiOx with a uniform carbon layer, resulting in improved stability and efficiency for the anode material.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Yufei Yang, Jiangyan Wang, Sang Cheol Kim, Wenbo Zhang, Yucan Peng, Pu Zhang, Rafael A. Vila, Yinxing Ma, You Kyeong Jeong, Yi Cui
Summary: This study presents an in situ prelithiation method by integrating a Li metal mesh into the cell assembly to spontaneously prelithiate Si with electrolyte addition. The prelithiation amount can be precisely controlled by using Li meshes with different porosities, and the uniformity of prelithiation is enhanced by the patterned mesh design. With optimized prelithiation amount, the in situ prelithiated Si-based full cell exhibits a constant >30% capacity improvement in 150 cycles.
Article
Chemistry, Multidisciplinary
Yeyoung Ha, Maxwell C. Schulze, Sarah Frisco, Stephen E. Trask, Glenn Teeter, Nathan R. Neale, Gabriel M. Veith, Christopher S. Johnson
Summary: In this study, lithium oxide was added to a cathode to compensate for initial lithium loss at the anode, and Co3O4 was introduced to activate the lithium oxide. The additives successfully increased the capacity of the cells using Si anodes.
APPLIED SCIENCES-BASEL
(2021)
Article
Chemistry, Multidisciplinary
Xin-Yang Yue, Yu-Xing Yao, Jing Zhang, Zeheng Li, Si-Yu Yang, Xun-Lu Li, Chong Yan, Qiang Zhang
Summary: Mono-solvent DMC electrolyte is used for the first time in contact prelithiation, and the low-organic-content REI formed by this electrolyte is found to be a mixed ion/electron conductor. As a result, electron channels can be maintained even when the Li source is completely wrapped by the DMC-derived REI, leading to outstanding Li source utilization and negligible dead Li yield.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Yuke Wang, Jia Lu, Yan Qiao, Wangqi Dai, Heyi Xia, Changrong Yu, Yiwen Hu, Ziqiang Ma, Zhengwen Fu
Summary: To improve the initial coulombic efficiency and prelithiation efficiency in the prelithiation method using metal lithium, we propose a solid electrochemical corrosion (SEC) of lithium using solid electrolyte LiPON instead of liquid electrolyte. However, the low prelithiation rate of SEC with LiPON interlayer hinders its large-scale application. By introducing an ultrathin film of Bi2O3 as an interface layer, we successfully improve the prelithiation rate of SEC and demonstrate its effectiveness in enhancing the capacity and cycling performance of lithium-ion batteries.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Zijin Yang, Xianying Qin, Kui Lin, Qiuchan Cai, Yongzhu Fu, Baohua Li
Summary: In recent years, prelithiation has been considered one of the most promising schemes for improving the initial Coulombic efficiency (ICE) of lithium-ion batteries (LIBs). This study reports a modified LixSi material with high lithium reserves and great environmental adaptability as a prelithiation reagent, which can compensate for the capacity loss of the negative electrode in the first cycle. The synthesized material, which forms a protective layer consisting of LixAlySiOz/Li2O, provides a new idea for actual industrial production of prelithiation.
ELECTROCHEMISTRY COMMUNICATIONS
(2022)
Review
Materials Science, Multidisciplinary
Xiaomei Liu, Ze Wu, Leqiong Xie, Li Sheng, Jianhong Liu, Li Wang, Kai Wu, Xiangming He
Summary: In the past decade, the rapid development of lithium-ion battery (LIB) energy storage systems has supported the efficient operation of renewable energy stations. However, the current LIB falls short of meeting the demand for a longer service life. Prelithiation technology has been widely studied to improve the service life of LIBs, and this review summarizes different prelithiation methods. It also analyzes the challenges and potential of large-scale industrialization of prelithiation technology based on industry compatibility, prelithiation efficiency, and energy density. Furthermore, the future trends of LIB improvement using overlithiated cathode materials are discussed.
ENERGY & ENVIRONMENTAL MATERIALS
(2023)
Article
Chemistry, Analytical
Yu-Ke Wang, Si-Yu Yang, Yangyuchen Yang, Xiang Hong, Zheng-Wen Fu
Summary: Developing a prelithiation additive with high capacity and minimal side effects is crucial for improving the energy density and cycle life of lithium-ion batteries. In this study, an in-situ synthesized LixCrSSe layer was used as a prelithiation additive, with a maximum capacity of 555 mAh/g, to compensate for the initial capacity loss of lithium-ion batteries. The results demonstrate that the in-situ synthesized LixCrSSe is an effective cathode prelithiation additive.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Joseph W. Stiles, Anna L. Soltys, Xiaoyu Song, Saul H. Lapidus, Craig B. Arnold, Leslie M. Schoop
Summary: This study presents a new material, HxCrS2, formed by proton-exchange of NaCrS2, with a measured capacity of 728 mAh g(-1) and significant improvements to capacity retention, sustaining over 700 mAh g(-1) during cycling experiments. HxCrS2 exhibits a biphasic structure featuring alternating crystalline and amorphous lamella on the scale of a few nanometers, enabling reversible access to Cr redox in the material resulting in higher capacities than seen in the parent structure. Pretreatment by proton-exchange offers a route to materials such as HxCrS2 which provide fast diffusion and high capacities for sodium-ion batteries.
ADVANCED MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Khryslyn G. Arano, Beth L. Armstrong, Ethan Boeding, Guang Yang, Harry M. Meyer III, Evelyna Wang, Rachel Korkosz, Katie L. Browning, Thomas Malkowski, Baris Key, Gabriel M. Veith
Summary: Vinylene carbonate (VC) and polyethylene oxide (PEO) are used as functional agents to mimic the solid electrolyte interphase (SEI) chemistry of silicon. Covalent surface functionalization of silicon particles was achieved through ball-milling with sacrificial VC and PEO. The additives are strongly bound to silicon, resulting in improved stability and dispersion of the functionalized particles. Raman mapping and capacity measurements show that VC-milled silicon exhibits higher capacity and improved electrode processing compared to neat silicon.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Sanghyeon Kim, Nathan T. Hahn, Timothy T. Fister, Noel J. Leon, Xiao-Min Lin, Haesun Park, Peter Zapol, Saul H. Lapidus, Chen Liao, John T. Vaughey
Summary: Calcium-ion batteries (CIBs) have potential for next-generation energy storage due to the low redox potential and abundance of calcium compounds. This study reports the use of elemental Se as a high-capacity cathode material for CIBs operating via a conversion mechanism in a Ca metal battery at room temperature. The Se electrodes exhibit reversible specific capacity and a discharge plateau near 2.0 V (vs Ca2+/Ca). The electrochemical reaction between calcium and selenium is investigated using operando synchrotron-based techniques and discussed.
CHEMISTRY OF MATERIALS
(2023)
Article
Electrochemistry
Ritesh Uppuluri, Saul H. Lapidus, Yunya Zhang, John T. Vaughey, Fulya Dogan, Baris Key
Summary: The reactivity of lithium silicides can be suppressed by substituting a multivalent cation for lithium, leading to the formation of new ternary and quaternary lithium silicides through room temperature electrochemical synthesis. This method enhances the cycling and calendar life performance of the materials.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Yeyoung Ha, Stephen E. Trask, Yicheng Zhang, Andrew N. Jansen, Anthony Burrell
Summary: The LTO/LMO system shows promise for behind-the-meter storage applications due to its critical-material-free chemistry, offering good safety and long lifetime. By designing the LTO/LMO cells with different loadings and electrolyte properties, their capacity retention and performance can be enhanced.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Zhenzhen Yang, Stephen E. Trask, Xianyang Wu, Brian J. Ingram
Summary: Commercial Li-ion batteries commonly incorporate silicon materials in the graphite anode to increase the energy density. This study examines the effect of silicon-to-graphite ratio in the composite anode on fast-charging behavior. The results show that the addition of silicon improves rate capability and capacity retention, but leads to cell degradation in the long term due to silicon-electrolyte interactions and nonuniform distribution of decomposition products.
Article
Nanoscience & Nanotechnology
Jiyu Cai, Xinwei Zhou, Tianyi Li, Hoai T. Nguyen, Gabriel M. Veith, Yan Qin, Wenquan Lu, Stephen E. Trask, Marco-Tulio Fonseca Rodrigues, Yuzi Liu, Wenqian Xu, Maxwell C. Schulze, Anthony K. Burrell, Zonghai Chen
Summary: This study identifies the issues with silicon-based lithium-ion batteries during calendar aging and proposes strategies to improve battery life by suppressing parasitic reactions.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Zhenzhen Yang, Tanvir R. Tanim, Haoyu Liu, Ira Bloom, Eric J. Dufek, Baris Key, Brian J. Ingram
Summary: During XFC of lithium-ion batteries, LLI and reaction mechanisms at the anode/electrolyte interface are crucial factors. The causes of LLI and their quantification are still challenging. This study investigates the evolution and interactions of aging mechanisms at the anode/electrolyte interface. The results provide a comprehensive analytical framework for understanding anodic degradation mechanisms and assessing XFC lithium-ion battery capacity fade.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Alec S. Ho, Dilworth Y. Parkinson, Stephen E. Trask, Andrew N. Jansen, Nitash P. Balsara
Summary: The spatial distribution of internal ionic currents during fast charging and in resting state after charging can affect battery safety.
Article
Chemistry, Physical
Kira E. Wyckoff, Linus Kautzsch, Jonas L. Kaufman, Brenden R. Ortiz, Anna Kallistova, Ganesh Pokharel, Jue Liu, Keith M. Taddei, Kamila M. Wiaderek, Saul H. Lapidus, Stephen D. Wilson, Anton van der Ven, Ram Seshadri
Summary: Controlling the magnetic properties of functional inorganic materials with a kagome-derived network is achieved by electrochemically controlling the lithium content. The electronic occupancy and consequent magnetic properties are varied by inserting up to two additional lithium ions into LiScMo3O8. The measurements and calculations reveal the evolution from a diamagnetic band insulator to a geometrically frustrated magnet and back to a diamagnetic insulator as the lithium content changes.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Sathish Rajendran, Haoyu Liu, Stephen E. Trask, Baris Key, Andrew N. Jansen, Marco-T F. Rodrigues
Summary: Development of new polymeric binders can help enable the use of silicon-rich anodes in Li-ion batteries. These polymers can improve interfacial interactions and mechanical properties, but may also accelerate cell degradation. Our work demonstrates that redox-active conductive binders can be detrimental to cell performance, and careful experimental validation under realistic conditions is necessary for evaluating new polymers.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Multidisciplinary
Yanming Sun, Yili Cao, Shixin Hu, Maxim Avdeev, Chin-Wei Wang, Sergii Khmelevskyi, Yang Ren, Saul H. Lapidus, Xin Chen, Qiang Li, Jinxia Deng, Jun Miao, Kun Lin, Xiaojun Kuang, Xianran Xing
Summary: By high-temperature synthesis, researchers have achieved tunable thermal expansion in the kagome cubic (Fd-3m) intermetallic (Zr,Nb)Fe-2 materials. By magnetic doping, they have obtained a near-zero thermal expansion coefficient, which has significant applications in advanced technologies.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Ankit Verma, Maxwell C. Schulze, Andrew Colclasure, Marco-Tulio Fonseca Rodrigues, Stephen E. Trask, Krzysztof Pupek, Christopher S. Johnson, Daniel P. Abraham
Summary: The impact of electrolyte fluorination on the calendar fade of blended silicon-graphite anodes is explored. Unfluorinated electrolyte shows higher cell resistance compared to fluorinated electrolyte, with slower rate of parasitic capacity loss for the LiBOB system. The results suggest that fluorinated electrolyte performs better in calendar life.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Inorganic & Nuclear
Callista M. Skaggs, Dong-Choon Ryu, Hari Bhandari, Yan Xin, Chang-Jong Kang, Saul H. Lapidus, Peter E. Siegfried, Nirmal J. Ghimire, Xiaoyan Tan
Summary: Polycrystalline IrGe4 with a chiral crystal structure is synthesized and exhibits metallic behavior and non-saturating magnetoresistance under an applied magnetic field.
INORGANIC CHEMISTRY
(2023)