Article
Chemistry, Multidisciplinary
S. Vauthier, M. Alvarez-Tirado, G. Guzman-Gonzalez, L. C. Tome, S. Cotte, L. Castro, A. Gueguen, D. Mecerreyes, N. Casado
Summary: The role of binders is crucial to achieve high performance and long cycle lives in next-generation electrodes for lithium batteries. In this study, PDADMA poly(ionic liquid)s with fluorinated anions were used as cathode binders in Li-ion and Li-air batteries, showing improved cell performances and enhanced capacity values, rate performance, and cycling stability. The proposed fluorinated PDADMA Poly(ionic liquid)s can be a highly competitive alternative to conventional binders used nowadays in Li-ion and Li-air batteries.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Physical
Suseeladevi Asha, Deepthi Thomas, K. P. Vijayalakshmi, Benny K. George
Summary: The thermal stability and decomposition mechanisms of two pyrrolidinium based ionic liquids were investigated using Py-GC-MS and DFT, revealing different decomposition pathways and comparable activation energy parameters between experimental and computational methods.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Physical
Young Gyun Choi, Jong Chan Shin, Anseong Park, Young Min Jeon, Jin Il Kim, Sebin Kim, Seulwoo Kim, Won Bo Lee, Minjae Lee, Jong Hyeok Park
Summary: A semi-interpenetrating polymer network (semi-IPN) ion-transporting solid film using a new material named P(N)PEG is reported in this study to enhance the performance of lithium metal batteries. P(N)PEG exhibits good ability to solvate Li+ and the semi-IPN electrolyte shows excellent ionic conductivity and lithium ion transport properties.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Yichao Cai, Yunpeng Hou, Yong Lu, Qiu Zhang, Zhenhua Yan, Jun Chen
Summary: By optimizing the solvating molecule, we achieved fast Li+ transport and stable Li deposition in Li-O-2 batteries, leading to high rate capability and long cycle life. This work provides an effective electrolyte design principle for high-performance Li-O-2 batteries.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Mojtaba Eftekharnia, Robert Kerr, Maria Forsyth, Patrick C. Howlett
Summary: In order to utilize the advantages of high energy density lithium-metal batteries, their cycle life and safety need to be improved. External compression has been shown to enhance the performance of these batteries by reducing dendrite growth and improving lithium deposition morphology. This study investigates the behavior of high-capacity Li||LFP pouch cells in pyrrolidinium-based ionic liquid electrolytes under different levels of compression and discusses the mechanisms that affect the cell performance and failure. The results indicate that higher compression leads to more uniform and less dendritic lithium deposition.
JOURNAL OF POWER SOURCES
(2023)
Article
Biochemistry & Molecular Biology
Brian R. Carrick, Claire L. Seitzinger, Timothy P. Lodge
Summary: This study investigates the LCST phase behavior of poly(benzyl methacrylate) in a specific ionic liquid, showing that concentration has a strong influence on phase boundaries while molecular weight has no effect. The experimental cloud point is close to the coexistence curve, indicating thermal reversibility of the phase transitions.
Review
Chemistry, Physical
Syed Shoaib Hassan Zaidi, Xianglin Li
Summary: The search for high-energy-density battery systems has been driven by the remarkable increase in energy demand. Li-O-2 battery (LOB) and Li-air battery (LAB) have attracted extensive research due to their high theoretical energy density. However, the commercial development of LOB has faced challenges due to its components. Ionic liquids (ILs) are considered promising electrolyte solvents for LOBs and LABs due to their excellent electrochemical and thermal stability, non-flammability, low flammability, and O-2 solubility. This review summarizes the progress of IL-based LOBs and LABs since their first report in 2005, discussing the impact of ILs' physiochemical properties on the performance of the batteries under different operating conditions, and the methodologies employed to optimize these properties for rechargeable lithium batteries, enabling the design of cost-effective batteries with high safety, energy density, power density, and long-term stability.
ADVANCED ENERGY MATERIALS
(2023)
Article
Physics, Applied
Zisheng Liu, Ning Zhao, Xiaohui Zhao, Chenggong Wang, Tao Zhang, Sheng Xu, Xiangxin Guo
Summary: Li-O-2 batteries based on the conversion reaction of oxygen cathodes can deliver high specific capacity. Combining Li-rich layered-oxide cathodes with oxygen cathodes improves cell performance and extends cycle life.
APPLIED PHYSICS LETTERS
(2022)
Article
Nanoscience & Nanotechnology
Ruoyao Xu, Hua Dong, Peizhou Li, Xiangrong Cao, Haomiao Li, Jingrui Li, Zhaoxin Wu
Summary: By introducing FAAc, we successfully developed a strategy for the formation of high-quality films in Sn-based PSCs, achieving improved device performance and maintaining 82% of the initial efficiency in a light aging test.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Bhabani S. Dhananjay, Bhabani S. Mallik
Summary: Mixed electrolytes consisting of dimethylacetamide (DMA)/ sulfolane (TMS) with lithium bisfluorosulfonimide (LiTFSI) show better performance in aprotic lithium-O-2 batteries compared to single solvent electrolytes. This study uses classical molecular dynamics simulations to analyze the structure and ionic dynamics of DMA/TMS hybrid electrolytes. The results indicate minimal changes in electrolyte structure with increasing DMA content and provide insights into ion-pair and ion-cage formation and their correlation with ionic conductivity.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Engineering, Chemical
Syeda Saba Fatima, Azry Borhan, Muhammad Ayoub, Noraini Abd Ghani
Summary: The serious environmental issues associated with CO2 emissions have led to the development of energy efficient processes and CO2 capture technologies. CO2 adsorption using functionalized sorbents is one suitable technique. In this study, a functionalized activated carbon material was developed via the wet impregnation technique. The researchers found that temperature has a positive impact on the CO2 adsorption capacity of functionalized activated carbon.
Article
Chemistry, Physical
Samuel T. Plunkett, Alireza Kondori, Duck Young Chung, Jianguo Wen, Mark Wolfman, Saul H. Lapidus, Yang Ren, Rachid Amine, Khalil Amine, Anil U. Mane, Mohammad Asadi, Said Al-Hallaj, Brian P. Chaplin, Kah Chun Lau, Hsien-Hau Wang, Larry A. Curtiss
Summary: The development of LiO2-based batteries using IrLi nanoparticles as cathode material can significantly reduce the charge overpotentials and stabilize the LiO2 discharge products. The formation of crystalline LiO2 on the (111) facets of IrLi nanoparticles provides a means to prevent the generation of Li2O2.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Physical
Sumana Brahma, Ramesh L. Gardas
Summary: This study provides a detailed analysis of the volumetric and acoustic properties of dilute solutions of ionic liquids and acetonitrile. The findings are important for potential engineering applications and process design, and contribute to our understanding of the intermolecular interactions between solutes and solvents.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Multidisciplinary
Yichao Cai, Qiu Zhang, Yong Lu, Zhimeng Hao, Youxuan Ni, Jun Chen
Summary: The Li+ transport ability of TFSI-IL electrolyte was greatly enhanced by introducing hydrofluoroether and optimizing electrolyte component ratios, resulting in robust Li deposition and significantly improved cycling stability of Li-O-2 batteries.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Dongxu Ouyang, Kuo Wang, Yimei Pang, Zhirong Wang
Summary: This study comprehensively investigates a fluorinated electrolyte proposed by Im et al., and finds that the electrolyte with added LFO (FF19+3LFO) can improve the cycling performance of lithium-ion batteries under high-voltage conditions. The FF19+3LFO cells also demonstrate better performance in high-temperature storage tests and accelerating rate calorimetry tests. These findings are important for achieving high-capacity and high-safety lithium-ion cells.
JOURNAL OF POWER SOURCES
(2022)
Article
Nanoscience & Nanotechnology
Anna T. S. Freiberg, Simon Qian, Johannes Wandt, Hubert A. Gasteiger, Ethan J. Crumlin
Summary: A new operando spectro-electrochemical setup was developed to study oxygen depletion from the surface of layered transition metal oxide particles at high degrees of delithiation. By analyzing the O 1s spectra of the particles and comparing it to the Ni 2p3/2 intensity, the metal-to-oxygen ratio of the metal oxide close to the particle surface can be calculated, providing insight into the formation of an oxygen-depleted phase. This new setup enables a deeper understanding of interfacial changes of layered oxide-based cathode active materials for Li-ion batteries upon cycling.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Electrochemistry
Stefan Oswald, Hubert A. Gasteiger
Summary: The composition of layered transition metal oxides as cathode active materials is trending towards higher nickel contents for increased capacity and energy. The stability of these materials at high degrees of delithiation is determined by their composition, rather than the stability window of the electrolyte. Short-term cycling experiments and online electrochemical mass spectrometry reveal that capacity fade and lattice oxygen release are concurrent processes contributing to CAM degradation.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Clara Berg, Robert Morasch, Maximilian Graf, Hubert A. Gasteiger
Summary: A comparison is made between graphite and microsilicon anodes in terms of their temperature-dependent kinetic charge-transfer resistances and ion transport resistances. It is found that the charge-transfer resistance dominates at low temperatures, while at high temperatures, the pore resistance dominates for both electrode types. Additionally, when fast-charging, the thinner silicon electrode has lower overpotentials due to lower ion transport losses in the electrolyte phase.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Tobias Teufl, Daniel Pritzl, L. Hartmann, Sophie Solchenbach, Manuel A. Mendez, Hubert A. Gasteiger
Summary: Fluoroethylene-carbonate (FEC) is commonly used in lithium-ion batteries as a co-solvent for high-voltage cathodes and silicon-based anodes. However, its limited thermal stability when used with LiPF6 can trigger detrimental side reactions, producing vinylene-carbonate (VC) and HF at elevated temperatures. These side reactions not only increase impedance but also lead to transition metal dissolution. Comparatively, FEC has no advantage over ethylene-carbonate (EC) in high-voltage operation without lattice oxygen evolution. Extended charge/discharge cycling at 45 degrees C shows that the thermal decomposition of FEC leads to cell bulging due to the oxidation of VC above approximately 4.4-4.5 V vs. Li+/Li.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Franziska Friedrich, Alexander Kunz, Andreas Jossen, Hubert A. Gasteiger
Summary: Using isothermal micro-calorimetry, the heat generation of lithium- and manganese-rich layered oxides (LMR-NCMs) during the first cycle is investigated. It is found that irreversible structural rearrangements during activation lead to a considerable generation of heat. Only a fraction of the lost electrical work is converted into waste heat, suggesting that the heat flow profile of the first charge is unique.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Christian Sedlmeier, Robin Schuster, Carina Schramm, Hubert A. Gasteiger
Summary: Impedance measurements are a powerful tool to investigate interfaces in lithium-ion batteries. This study presents a straightforward approach to implement a micro-reference electrode (mu-RE) for electrode-resolved impedance and potential measurements in all-solid-state batteries. The mu-RE consists of an insulated gold wire sandwiched between two Li6PS5Cl/polymer separator sheets and is activated by in situ electrochemical lithiation. The results show the importance of the cell assembly configuration in providing a reservoir of cyclable lithium.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Correction
Electrochemistry
Stefan Oswald, Daniel Pritzl, Morten Wetjen, Hubert A. Gasteiger
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Ana Marija Damjanovic, Anna Theresa Sophie Freiberg, Armin Siebel, Burak Koyutuerk, Davide Menga, Kevin Krempl, Pankaj Madkikar, Olivier Proux, Hubert Andreas Gasteiger, Michele Piana
Summary: Ex situ and operando X-ray absorption spectroscopy (XAS) were used to investigate the structure and degradation mechanism of Fe-based catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). The results showed that Fe3+ was incorporated in the ZrO2 structure and significant presence of Fe-N-C-type structures was excluded in the Fe0.07Zr0.93O2-delta/C catalyst. The aging process led to the formation of oxidic Fe clusters and Fe demetalation from the ZrO2 structure. The faster aging of Fe0.07Zr0.93O2-delta compared to Fe-N-C was attributed to improved mass transport to/from active sites.
Article
Electrochemistry
Robert Morasch, Hubert A. Gasteiger, Bharatkumar Suthar
Summary: The proposed expression for the exchange current density has been widely used for modeling Li-ion battery materials, but its applicability needs validation. In this study, the kinetic behavior of NCM 111 was analyzed using EIS and compared with the proposed theory. The results show that the charge transfer kinetics follow the proposed theory for lower concentrated electrolytes, but deviate at higher salt concentrations.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Rafael B. Berk, Thorsten Beierling, Lukas Metzger, Hubert A. Gasteiger
Summary: This study investigates the influence of the hydroxide precursor on the physical properties of cathode active material (CAM) for lithium-ion batteries during industrial production. The evolution of secondary particle size and morphology of Ni0.8Co0.1Mn0.1(OH)2 during coprecipitation is observed, revealing a two-stage particle formation mechanism: seeding phase and growth phase. The degree of turbulence in the seeding phase affects the size and number of seeds, which subsequently influences the growth rate and morphology of the secondary particles.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Secil Unsal, Michele Bozzetti, Yen-Chun Chen, Robin Girod, Anne Berger, Justus S. Diercks, Sofia Gialamoidou, Jike Lyu, Marisa Medarde, Hubert A. Gasteiger, Vasiliki Tileli, Thomas J. Schmidt, Juan Herranz
Summary: Non-noble metal catalysts (NNMCs) are a promising alternative to expensive Pt-based materials for catalyzing the oxygen reduction reaction (ORR) in proton exchange membrane fuel cell (PEMFC) cathodes. By studying catalysts with different particle sizes and porosities, it was found that smaller aggregate size and higher porosity lead to improved mass transport properties and peak power density.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Yan-Sheng Li, Davide Menga, Hubert A. Gasteiger, Bharatkumar Suthar
Summary: In this study, the impact of electronic resistance on the performance of PGM-free CCLs in PEMFCs was investigated. It was found that adding carbon additives can significantly improve fuel cell performance. Four-point probe measurements revealed a significant difference in resistance between the in-plane and through-plane direction of the CCLs, attributed to the anisotropic morphology of the CCLs.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Anne Berger, Yen-Chun Chen, Jacqueline Gatzemeier, Thomas J. Schmidt, Felix N. Buechi, Hubert A. Gasteiger
Summary: This study aims to analyze the impact of fabricating a GDL with an MPL that intrudes into the GDL-S on the structure of GDL-S and PEMFC performance. The results provide design guidelines for improved GDLs.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Timo Imhof, Roberta K. F. Della Bella, Bjoern M. Stuehmeier, Hubert A. Gasteiger, Marc Ledendecker
Summary: Liquid half-cell measurements are useful for determining parameters of electro-catalysts, but their applicability to real-world systems is uncertain. This study conducted a voltage cycling accelerated stress test (AST) and found that the loss of electrochemically active surface area (ECSA) is enhanced at higher temperatures and with a high ionomer/carbon mass ratio. The results suggest that liquid half-cell based ASTs can provide application-relevant predictions of catalyst durability.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Electrochemistry
Rafael B. Berk, Thorsten Beierling, Lukas Metzger, Hubert A. Gasteiger
Summary: This study investigates the relationship between residual sulfur content, crystallinity, and the pH value during the synthesis of Ni0.8Co0.1Mn0.1(OH)2, as well as the inhibition of crystallite growth due to sulfate adsorption. Adsorption/desorption experiments demonstrate the possibility to decouple secondary particle morphology and residual impurity content.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)