Article
Chemistry, Multidisciplinary
Daniel Martin-Yerga, David C. Milan, Xiangdong Xu, Julia Fernandez-Vidal, Laura Whalley, Alexander J. Cowan, Laurence J. Hardwick, Patrick R. Unwin
Summary: In this study, correlative scanning electrochemical cell microscopy (SECCM) and shell-isolated nanoparticles for enhanced Raman spectroscopy (SHINERS) were used to screen the formation of solid-electrolyte interphase (SEI) on Si electrodes. The results revealed the heterogeneous and dynamic nature of SEI, showing characteristic evolution as a function of cycle number. This correlative technique has the potential to accelerate the optimization of SEI formation methods in lithium-ion batteries.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Zachary T. Gossage, Nanako Ito, Tomooki Hosaka, Ryoichi Tatara, Shinichi Komaba
Summary: This study provides a deeper understanding of the solid-electrolyte interphase (SEI) that occurs in highly concentrated water-insalt electrolytes (WISEs). The research shows that SEI in aqueous batteries exhibits similar passivating structures and slow electron transfer rates to that found in lithium-ion batteries. Additionally, the properties of SEI change when the electrolyte becomes more concentrated.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xiangdong Xu, Daniel Martin-Yerga, Nicholas E. Grant, Geoff West, Sophie L. Pain, Minkyung Kang, Marc Walker, John D. Murphy, Patrick R. Unwin
Summary: Understanding the formation of SEI and (de)lithiation phenomena at silicon electrodes is crucial for improving the performance and longevity of Si-based lithium-ion batteries. However, these processes are still elusive, particularly the role of Si surface termination.
Article
Chemistry, Multidisciplinary
Carla S. Santos, Alexander Botz, Aliaksandr S. Bandarenka, Edgar Ventosa, Wolfgang Schuhmann
Summary: The solid-electrolyte interphase (SEI) provides a protective layer in lithium-ion batteries, preventing degradation of the electrolyte at the anode. This study used scanning electrochemical microscopy (SECM) to quantitatively assess the local electronic and ionic properties of SEI in Li-ion batteries, and found that the formation conditions and electrolyte type have a significant impact on its conductivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Electrochemistry
Shinji Kondou, Yoshifumi Watanabe, Kaoru Dokko, Masayoshi Watanabe, Kazuhide Ueno
Summary: This study demonstrates a significant improvement in the cycle performance of a Li4Ti5O12 electrode by using a Li-Ca binary salt hydrate electrolyte and an optimized electrochemical pretreatment process to form a thick SEI layer. This approach offers a promising route for the practical use of low-potential anode materials in aqueous rechargeable lithium-ion batteries.
Article
Chemistry, Physical
Jiahao Chen, Hong Zhang, Hongzhu Chen, Enjie Xia, Yanmei Wu, Zhicheng Li
Summary: Solid-state Li-ion batteries have gained significant attention for their high safety and energy density. Polyvinylidene fluoride (PVDF) has shown potential as an electrolyte due to its high permittivity, wide voltage window, and excellent thermal stability. This study successfully prepared Y3+-doped Li29Zr9Nb3O40 (LZNO) Li-ionic conductor and fabricated LZNO-decorated PVDF-based composite solid electrolytes. Addition of LZNO powder improved the interface resistance and greatly enhanced the specific discharge capacity of the cells at high rates.
JOURNAL OF POWER SOURCES
(2022)
Article
Materials Science, Ceramics
Fugang Lu, Ce Wang, Jiujie Xu, Zhanguo Liu, Panpan Lin, Tiesong Lin, Jincheng Lin, Xinfei Zhang, Xinyue Li, Peng He
Summary: Excess Li compensation powder (ECP) can be used as a covering powder in the pressureless sintering of Li-garnet solid electrolytes, optimizing the microstructure and improving the density and ionic conductivity.
CERAMICS INTERNATIONAL
(2023)
Review
Chemistry, Multidisciplinary
Yating Li, Zuhao Yu, Jianhang Huang, Yonggang Wang, Yongyao Xia
Summary: The problems of zinc anode, such as dendrite growth and hydrogen evolution, significantly impair the performance of zinc batteries. The solid electrolyte interphase (SEI), crucial for achieving high reversibility of lithium anode in non-aqueous organic solvents, also contributes to the improvement of zinc anode performance in aqueous electrolytes. However, current research on the interphase for zinc electrodes is fragmented, lacking a deep understanding of the underlying causes or general design rules for SEI construction. The high reactivity of water molecules poses a serious challenge for effective SEI formation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Jialong Fu, Zhuo Li, Xiaoyan Zhou, Zhiyong Li, Xin Guo
Summary: A fluorinated quasi-solid polymer electrolyte is synthesized to stabilize Li metal, effectively suppressing Li dendrites and Li pulverization. The lithium metal battery with the fluorinated quasi-solid polymer electrolyte exhibits stable cycling performance owing to the enriched C-F/LiF solid electrolyte interphase and lithophilic C-F-guided ion plating/stripping and rapid Li+ transportation.
Article
Materials Science, Ceramics
Young Seon Park, Kangsanin Kim, Jong-Won Lee, Ji-Woong Moon, Hyung-Ho Park, Haejin Hwang
Summary: In this study, a specially designed cell assembly is proposed to adjust to the changes in volume that occur during cycling while maintaining a constant cell pressure. The evaluations indicate that using a spring-equipped assembly effectively reduces stress and capacity fading in all-solid-state cells. Focused ion beam-scanning electron microscope observations confirm the absence of cracks and delamination in the electrode materials.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
John Holoubek, Haodong Liu, Qizhang Yan, Zhaohui Wu, Bao Qiu, Minghao Zhang, Sicen Yu, Shen Wang, Jianbin Zhou, Tod A. Pascal, Jian Luo, Zhaoping Liu, Ying Shirley Meng, Ping Liu
Summary: This study demonstrates the reversible performance of a localized-high-concentration electrolyte (LHCE) based on ether solvents for Li||LMR batteries, improving the cycling performance and cathode-electrolyte interphase chemistry.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Le Anh Ma, Andrew J. Naylor, Leif Nyholm, Reza Younesi
Summary: This study investigates the impact of electrolyte chemistry on the dissolution of the solid electrolyte interphase (SEI) in sodium-ion batteries, using beta-alumina as a sodium-conductive membrane to prevent crosstalk. The research found that the solubility of SEI species in the electrolyte can reach up to 30% after a 50-hour pause, and saturation of the electrolyte with these SEI species can counteract aging due to SEI dissolution.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Sheng Chen, Yunping Wu, Shuwen Niu, Zhengyu Wei, Youshen Wu, Wei Wei
Summary: By exploiting the advantages of solid polymer electrolytes (SPEs) including light weight, flexibility, and flame retardancy, this study addresses the safety concerns and energy density improvement for lithium-ion batteries (LIBs). The development of SPEs is still hindered by their low ionic conductivity, which can be overcome by a hierarchical structure of flower-like Co3O4 microspheres and a multifunctional coating of polydopamine (PDA) used as a lithiophilic backbone. The interphase characterizations and their effects on Li+ conductivity and mechanical/electrochemical stability are investigated, and the potential application of Co3O4@PDA-based composite solid polymer electrolytes (CPEs) in all-solid-state LIBs is demonstrated.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Jimin Oh, Gun Park, Hongjun Kim, Sujung Kim, Dong Ok Shin, Kwang Man Kim, Hye Ryung Byon, Young-Gi Lee, Seungbum Hong
Summary: In this study, we investigate the relationship between the content of solid electrolytes and irreversible capacity in composite electrodes. We analyze the variations of chemical composition and morphology in the solid electrolyte interphase (SEI) layer on the electrodes using electrochemical strain microscopy (ESM) and X-ray photoelectron spectroscopy (XPS). The results show that the solid electrolyte content affects the thickness of the SEI layer and the chemical distributions of Li and F ions, which in turn affect the Coulombic efficiency.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Engineering, Multidisciplinary
Falco Schneider, Jochen Zausch, Jan Lammel, Heiko Andra
Summary: The growth of the solid electrolyte interphase (SEI) is a major degradation process in Li-ion batteries, leading to increased cell resistance and reduced capacity. This study proposes a semi-implicit solution approach to handle the dynamics of SEI growth and evaluates its performance compared to the traditional monolithic solver. The results show that the semi-implicit solver significantly improves performance while maintaining convergence behavior.
APPLIED MATHEMATICAL MODELLING
(2022)
Review
Chemistry, Multidisciplinary
Si-Xuan Guo, Cameron L. Bentley, Minkyung Kang, Alan M. Bond, Patrick R. Unwin, Jie Zhang
Summary: This article introduces two advanced spatiotemporal voltammetric techniques for electrocatalytic studies, which provide important insights into the electrochemical reduction of CO2. Fourier transformed large-amplitude alternating current voltammetry allows the resolution of rapid electron-transfer processes, while scanning electrochemical cell microscopy provides high-resolution activity maps and potentiodynamic movies of catalyst surfaces.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Electrochemistry
Jai White, Athira Anil, Daniel Martin-Yerga, German Salazar-Alvarez, Gunnar Henriksson, Ann Cornell
Summary: The study investigates the challenges faced by the development of alcohol-based electrolysis for concurrent hydrogen production and low electricity consumption. It identifies significant parameters affecting glycerol electrooxidation reaction (GEOR) and proposes a catalyst reactivation method for prolonged use and stability.
ELECTROCHIMICA ACTA
(2022)
Article
Chemistry, Physical
Zhen Qiu, Daniel Martin-Yerga, Par A. Linden, Gunnar Henriksson, Ann Cornell
Summary: In this study, two different catalytic materials, PdNi and NiO, were investigated for the oxidation reaction of carbohydrate degradation products. The results showed that the PdNi catalyst could catalyze the products at low potential requirements but had limited current density. On the other hand, the NiO catalyst could operate at high current densities but required relatively higher potentials. Compared to Pd-based catalysts, this non-noble metal catalyst exhibited better performance at high conversion rates, indicating its potential for sustainable hydrogen production using waste streams.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Multidisciplinary
Cameron L. Bentley, Minkyung Kang, Saheed Bukola, Stephen E. Creager, Patrick R. Unwin
Summary: In this study, local ion-flux imaging was performed on chemical vapor deposition (CVD) graphene vertical bar Nafion membranes using an electrochemical ion (proton) pump cell mode of scanning electrochemical cell microscopy (SECCM). The results show that most of the CVD graphene vertical bar Nafion membrane is impermeable to proton transport, with transmission occurring at localized sites across a small area of the membrane. This suggests that rare atomic defects are responsible for proton conductance.
Editorial Material
Chemistry, Multidisciplinary
Laura Trapiella-Alfonso, Mariana Tasso, Gonzalo Ramirez Garcia, Daniel Martin-Yerga, Antonio R. Montoro Bustos
FRONTIERS IN CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Daniel Martin-Yerga, David C. Milan, Xiangdong Xu, Julia Fernandez-Vidal, Laura Whalley, Alexander J. Cowan, Laurence J. Hardwick, Patrick R. Unwin
Summary: In this study, correlative scanning electrochemical cell microscopy (SECCM) and shell-isolated nanoparticles for enhanced Raman spectroscopy (SHINERS) were used to screen the formation of solid-electrolyte interphase (SEI) on Si electrodes. The results revealed the heterogeneous and dynamic nature of SEI, showing characteristic evolution as a function of cycle number. This correlative technique has the potential to accelerate the optimization of SEI formation methods in lithium-ion batteries.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Emmanuel Batsa Tetteh, Dimitrios Valavanis, Enrico Daviddi, Xiangdong Xu, Carla Santana Santos, Edgar Ventosa, Daniel Martin-Yerga, Wolfgang Schuhmann, Patrick R. Unwin
Summary: The study focuses on the material for Li-ion batteries and develops a combination method of scanning electrochemical cell microscopy and in situ optical microscopy for high-throughput charge/discharge analysis of single TiO2 nanoparticle clusters. The research reveals that TiO2 with a size of approximately 50 nm can store over 30% of the theoretical capacity at an extremely fast charge/discharge rate. This finding strengthens the potential of TiO2 for fast-charging batteries and the research method can be widely applied for electrochemical screening of nanostructured materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Cameron L. Bentley, Lachlan F. Gaudin, Minkyung Kang
Summary: Local voltammetric analysis with a scanning electrochemical droplet cell technique, in combination with a new data processing protocol, is used to directly identify previously unseen regions of elevated electrocatalytic activity on the basal plane of molybdenum disulfide. Understanding the nature of these microscopic catalytic active sites is crucial for the rational design of renewable fuel production materials.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Xiangdong Xu, Daniel Martin-Yerga, Nicholas E. Grant, Geoff West, Sophie L. Pain, Minkyung Kang, Marc Walker, John D. Murphy, Patrick R. Unwin
Summary: Understanding the formation of SEI and (de)lithiation phenomena at silicon electrodes is crucial for improving the performance and longevity of Si-based lithium-ion batteries. However, these processes are still elusive, particularly the role of Si surface termination.
Article
Chemistry, Multidisciplinary
Minkyung Kang, Cameron L. Bentley, J. Tyler Mefford, William C. Chueh, Patrick R. Unwin
Summary: This study investigates the variations in electrochemical properties of nanostructured electrocatalysts at different length scales, particularly focusing on the oxygen evolution reaction (OER) activity of beta-Co(OH)(2) platelet particles. The results reveal the significance of heterogeneous activity at the single-particle level, as well as the importance of factors such as particle structure, particle-support interaction, and presence of defects, in governing the electrochemical activities of these materials. The study suggests a roadmap for the rational design and optimization of nanostructured electrocatalysts for alkaline water electrolysis.
Review
Chemistry, Physical
Daniel Martin-Yerga, Patrick R. Unwin, Dimitrios Valavanis, Xiangdong Xu
Summary: Correlative co-located electrochemical multi-microscopy is revolutionizing our understanding of property-function relationships in electrode materials, providing high spatial resolution. This review explores recent advancements in this approach and showcases its applications in diverse electrochemical fields.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Electrochemistry
Dalia L. Swinya, Daniel Martin-Yerga, Marc Walker, Patrick R. Unwin
Summary: Surface activation through anodization in alkaline media can enhance dopamine adsorption and electron transfer kinetics on glassy carbon electrodes. Short anodization times rapidly achieve nearly complete monolayer coverage of dopamine, while longer anodization induces changes in electrochemical surface area resulting in increased dopamine concentration based on geometric area but decreased based on specific surface area.
Article
Chemistry, Physical
Oluwasegun J. Wahab, Minkyung Kang, Enrico Daviddi, Marc Walker, Patrick R. Unwin
Summary: This study investigates the influence of crystallographic orientation on the electrocatalytic performance of polycrystalline copper (Cu) in CO2 electroreduction. The results demonstrate a correlation between step and kink density of secondary surface facets and electroreduction activity. Additionally, the ease of oxide removal on low-index facets is found to follow the order of (100) > (111) > (110).
Article
Chemistry, Physical
Dalia L. Swinya, Daniel Martin-Yerga, Marc Walker, Patrick R. Unwin
Summary: The adsorption and electron-transfer kinetics of dopamine on carbon electrodes were investigated in this study. It was found that anodization of glassy carbon electrodes improves the electron-transfer kinetics and provides more adsorption sites for dopamine. However, adsorption takes longer to reach completion on the anodized surface and the extent of adsorption is less compared to the unmodified surface. Additionally, lower graphitic and higher oxygen content on the anodized electrodes suggest that oxygen-containing functional groups may not enhance dopamine adsorption.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)