Review
Chemistry, Multidisciplinary
Doron Aurbach, Elena Markevich, Gregory Salitra
Summary: To enhance the energy density of lithium ion batteries, the combination of lithium metal anodes with specific cathode materials and advanced electrolyte solutions is crucial. Research has shown that the use of fluorinated co-solvents can improve the cycling behavior of full cells, paving the way for developing rechargeable batteries with the highest energy density.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Neeha Gogoi, Erik Bowall, Robin Lundstrom, Nataliia Mozhzhukhina, Guiomar Hernandez, Peter Broqvist, Erik J. Berg
Summary: A recent study reveals that silyl groups not only react with fluorides but also with several common Lewis bases in Li-ion batteries. This research helps establish a simplified and universally applicable reaction mechanism, explaining how silyl groups can lower cell impedance and prolong battery lifespan.
CHEMISTRY OF MATERIALS
(2022)
Article
Energy & Fuels
Yunya Guo, Jingjing Zhang, Na Sun, Lixia Ling, Riguang Zhang, Heqin Guo, Debao Li, Baojun Wang
Summary: A halogen-free catalyst, magnesium oxide, has been investigated for the efficient cycloaddition of ethylene oxide and CO2 to generate ethylene carbonate. The catalyst exhibited low activity due to high activation energy, but a stable Li-MgO catalyst was obtained and shown to have a lower activation energy in a one-step route via the Eley-Rideal mechanism.
Article
Chemistry, Physical
Taku Sudoh, Keisuke Shigenobu, Kaoru Dokko, Masayoshi Watanabe, Kazuhide Ueno
Summary: The effects of diluents on the Li+ transference number were investigated. It was found that coordinating diluents effectively improve the Li+ transference number, while non-coordinating diluents have no effect on the ion transport mechanism.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Arihant Bhandari, Chao Peng, Jacek Dziedzic, John R. Owen, Denis Kramer, Chris-Kriton Skylaris
Summary: In this study, the nucleation and growth of Li clusters on the graphite anode in Li-ion batteries were investigated using theoretical calculations. The results showed that the growth of clusters is influenced by the applied voltage and the lithiation level of the graphite. The zigzag edge termination and lithiated graphite were found to be more prone to nucleation and growth. Additionally, the surrounding electrolyte environment plays a significant role in the nucleation process.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Mikel Arrese-Igor, Maria Martinez-Ibanez, Juan Miguel Lopez del Amo, Eduardo Sanchez-Diez, Devaraj Shanmukaraj, Erwan Dumont, Michel Armand, Frederic Aguesse, Pedro Lopez-Aranguren
Summary: Solid state lithium metal batteries based on polymer electrolytes show promising prospects in addressing the energy density and safety issues of conventional Li ion batteries. The use of different polymers can bring advantages for high-performance cells, but salt migration needs to be solved.
ENERGY STORAGE MATERIALS
(2022)
Article
Electrochemistry
Min Lin, Xuerui Yang, Xi Zheng, Jianming Zheng, Jun Cheng, Yong Yang
Summary: This study used density functional theory to investigate the oxidation reaction processes of fluoroethylene carbonate and ethylene carbonate on LixCoO2 surfaces, revealing that the oxidation of fluoroethylene carbonate is more favorable than ethylene carbonate due to stronger adsorption of the fluorinated molecular fragment on the surface.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Engineering, Chemical
Ning Rui, Rui Shi, Ramon A. Gutierrez, Rina Rosales, Jindong Kang, Mausumi Mahapatra, Pedro J. Ramirez, Sanjaya D. Senanayake, Jose A. Rodriguez
Summary: The conversion and utilization of carbon dioxide is a critical challenge for reducing greenhouse gas pollution and producing high value chemicals. ZrO2/Cu(111) is an inverse oxide/metal catalyst with high activity and stability for the hydrogenation of CO2 into methanol, affecting the reaction products significantly.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
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
Chemistry, Multidisciplinary
Junze Guo, Weidong Zhang, Zeyu Shen, Shulan Mao, Xinyang Wang, Shichao Zhang, Jiahui Zhang, Yingying Lu
Summary: Poly(ethylene oxide) (PEO) based solid-state electrolytes show potential for practical all solid-state Li-metal batteries (ASSLMBs) due to their good chemical stability. However, the use of thin PEO presents a risk of short circuit in its semi-molten state, and PEO can be oxidatively decomposed by cathodes under high voltage, hindering the practical application of PEO-based ASSLMBs. In this study, the introduction of Nanodiamonds (NDs) into PEO electrolytes is found to greatly improve the electrochemical performance of PEO-based batteries by readjusting the Li+ and e(-) conductivity at the anode/cathode interface.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Bernardine L. D. Rinkel, J. Padmanabhan Vivek, Nuria Garcia-Araez, Clare P. Grey
Summary: This study investigates the mechanism of electrolyte decomposition in lithium-ion batteries. The results indicate that the electrolyte decomposition on NMC electrodes can proceed through two distinct routes with different onset potentials. The consumption of water at the negative electrode can effectively reduce the decomposition products, thereby mitigating the degradation of NMC/graphite cells.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Minju Chung, Kyoungsuk Jin, Joy S. Zeng, Thu N. Ton, Karthish Manthiram
Summary: Selective and efficient electrocatalysts are crucial for the successful deployment of electrochemistry for synthetic applications. In this study, iridium-decorated manganese oxide nanoparticles were synthesized through galvanic replacement reactions, demonstrating high partial current density and Faradaic efficiency. Operando X-ray absorption spectroscopy results revealed that the leaching of manganese ions from the nanoparticles during the galvanic replacement process resulted in structural changes and increased presence of electrophilic oxygen atoms on the catalyst surface, enhancing the electrocatalytic activity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Natthapong Pongpichayakul, Suwaphid Themsirimongkon, Suphitsara Maturost, Kanlayawat Wangkawong, Li Fang, Burapat Inceesungvorn, Paralee Waenkaew, Surin Saipanya
Summary: Catalyst composites based on carbon loaded with Pt and CeO2 have been successfully prepared for methanol oxidation in direct-methanol fuel cells (DMFCs), showing enhanced catalytic performance and reduced CO poisoning by modifying carbon surfaces with CeO2 and Pt nanoparticles.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Review
Chemistry, Multidisciplinary
Dongfeng Du, Zhuo Zhu, Kwong-Yu Chan, Fujun Li, Jun Chen
Summary: Rechargeable lithium-oxygen batteries have high potential as energy storage devices, but their performance is hindered by slow oxygen reduction and evolution reactions at the cathodes. Introducing light into the batteries can improve reaction kinetics, but the understanding of this process is limited. This tutorial review summarizes recent findings on photoinvolved Li-O-2 batteries and discusses the challenges and prospects, considering the interdisciplinary nature of the field.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Engineering, Environmental
Yuhang Hu, Hao Li, Zidong Chen, Wanglai Cen, Qiang Wang, Yungui Chen, Ali Davoodi, Wei Liu
Summary: Researchers found that doping Li with 8.9 at% Sn can create a Li-Li22Sn5 dual-phase alloy with impressive processability, allowing the fabrication of thin foils. The textured Li-alloy exhibits stable plate-strip cycling and improved performance.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Shaked Dror, Sasha Khalfin, Noam Veber, Arad Lang, Yaron Kauffmann, Maria Koifman Khristosov, Reut Shechter, Boaz Pokroy, Ivano E. Castelli, Yehonadav Bekenstein
Summary: Double-perovskite structures with the composition of Cs2AgBiBr6 are suggested as emerging inorganic semiconductors for solar energy conversion. Colloidal synthesis provides a methodological basis for investigating single monolayer two-dimensional materials and using them as building blocks for a more stable bilayer structure and thicker nanoplates. The colloidal approach enables the use of high-resolution transmission electron microscopy to detect structural defects, which is essential for improving the properties of bismuth-based lead-free double perovskites and bringing them closer to real-life photovoltaic implementation.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jette K. Mathiesen, Jonathan Quinson, Sonja Blaseio, Emil T. S. Kjaer, Alexandra Dworzak, Susan R. Cooper, Jack K. Pedersen, Baiyu Wang, Francesco Bizzotto, Johanna Schroeder, Tiffany L. Kinnibrugh, Soren B. Simonsen, Luise Theil Kuhn, Jacob J. K. Kirkensgaard, Jan Rossmeisl, Mehtap Oezaslan, Matthias Arenz, Kirsten M. o. Jensen
Summary: In this study, a surfactant-free synthesis method was used to prepare colloidal iridium nanoparticles. The formation routes and structures of the nanoparticles were investigated using in situ X-ray total scattering experiments. It was found that the precursor salt used greatly influenced the formation process and resulting structure of the nanoparticles. This study provides valuable insights into the formation and growth of iridium nanoparticles.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Hao Wan, Xingli Wang, Lei Tan, Michael Filippi, Peter Strasser, Jan Rossmeisl, Alexander Bagger
Summary: This article reveals the possibility of producing urea through the co-reduction reaction of nitrogen oxides and carbon monoxide, and constructs a 2-D activity heatmap to describe the nitrogen conversion to urea. This work provides a clear example of using computational simulations to predict selective and active materials for urea production.
Article
Chemistry, Physical
Mads K. K. Plenge, Jack K. K. Pedersen, Vladislav A. A. Mints, Matthias Arenz, Jan Rossmeisl
Summary: The search for better and cheaper electrocatalysts is crucial in the global transition to renewable energy resources. High-entropy alloys (HEAs) provide a wide range of alloys with continuous catalytic activity. This study demonstrates that the catalytic activity of an Ag-Ir-Pd-Pt-Ru HEA can be optimized by following ridges in a landscape model, leading to a potential new strategy for designing new catalysts.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Jay T. Bender, Amanda S. Petersen, Frederik C. ostergaard, Mikayla A. Wood, Sean M. J. Heffernan, Delia J. Milliron, Jan Rossmeisl, Joaquin Resasco
Summary: Alkali metal cations have no systematic effect on the hydrogen evolution reaction (HER) in acidic electrolytes, but do influence the HER in alkaline electrolytes. In alkaline media, HER rates decrease with increasing cation size for Ir, Pd, and Pt (Li+ > Na+ > K+ > Cs+), while they increase with cation size for Cu, Ag, and Au (Li+ < Na+ < K+ < Cs+).
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Maurizia Palummo, Michele Re Fiorentin, Koichi Yamashita, Ivano E. Castelli, Giacomo Giorgi
Summary: In this paper, we discuss the optoelectronic features and potential applicability of the tin-based oxynitride material InSnO2N for photo-conversion processes. Through the use of Density Functional and Many-Body Perturbation Theory, we calculate the electronic and optical properties and analyze their variations between the nonpolar and polar phases. Additionally, we determine the Spectroscopic Limited Maximum Efficiency of InSnO2N, further highlighting its relevance for solar energy conversion processes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Hongyu Zhang, Jijiang He, Weike Zhang, Ivano E. Castelli, Martin Saunders, Jeffrey M. Gordon, Hui Tong Chua
Summary: The generation of boron nitride nano-onions (BNNOs) from hexagonal-BN crystallite powder via a one-pot, non-toxic, catalyst-free, rapid hightemperature lamp ablation procedure is reported. Characterization procedures revealed the shapes, sizes, and composition of the nanoparticles, and a formation mechanism for BNNOs is proposed. Temperature measurements also showed the viable temperature range for BNNO generation.
Article
Chemistry, Physical
Ritums Cepitis, Nadezda Kongi, Jan Rossmeisl, Vladislav Ivanistsev
Summary: Improved oxygen electrocatalysis is crucial for meeting the increasing energy demand. Metal-nitrogen-carbon (M-N-C) materials show promise as catalysts due to their tunable activity through variations in electronic and geometric properties, including surface curvature. However, the influence of surface curvature on M-N-Cs has not been extensively explored. In this study, a realistic in-pore dual-atom site M-N-C model was developed, and density functional theory was used to investigate the effect of surface curvature on oxygen reduction and evolution reactions. The findings suggest that adjusting the surface curvature can enhance the catalytic activity for mono- and bifunctional oxygen electrocatalysis.
ACS ENERGY LETTERS
(2023)
Correction
Chemistry, Multidisciplinary
Olivia Westhead, Jesus Barrio, Alexander Bagger, James W. Murray, Jan Rossmeisl, Maria-Magdalena Titirici, Rhodri Jervis, Andrea Fantuzzi, Andrew Ashley, Ifan E. L. Stephens
NATURE REVIEWS CHEMISTRY
(2023)
Article
Electrochemistry
Benjamin H. H. Sjolin, Peter B. B. Jorgensen, Andrea Fedrigucci, Tejs Vegge, Arghya Bhowmik, Ivano E. E. Castelli
Summary: We developed a multi-target multi-fidelity workflow to search for stable high-performance solid state electrolytes for all-solid state batteries. The workflow utilizes thermodynamic and kinetic properties calculations, including phase and electrochemical stability, semiconducting behavior, and ionic diffusivity. By using a surrogate model to predict the transition state structure, the calculation of kinetic properties is greatly accelerated without significant loss of accuracy.
BATTERIES & SUPERCAPS
(2023)
Editorial Material
Electrochemistry
Benjamin H. H. Sjolin, Peter B. B. Jorgensen, Andrea Fedrigucci, Tejs Vegge, Arghya Bhowmik, Ivano E. E. Castelli
Summary: We developed and implemented a multi-target multi-fidelity workflow to explore the chemical space of antiperovskite materials as solid state electrolytes for all-solid state batteries. The workflow includes calculations of thermodynamic and kinetic properties, and uses a surrogate model to predict the transition state structure during ionic diffusion, significantly reducing calculation cost. This approach identified 14 materials that agree with experimental results as promising solid state electrolytes.
BATTERIES & SUPERCAPS
(2023)
Article
Chemistry, Physical
Milena Martins, Dominik Haering, Justin G. Connell, Hao Wan, Katrine L. Svane, Bostjan Genorio, Pedro Farinazzo Bergamo Dias Martins, Pietro P. Lopes, Brian Gould, Filippo Maglia, Roland Jung, Vojislav Stamenkovic, Ivano E. Castelli, Nenad M. Markovic, Jan Rossmeisl, Dusan Strmcnik
Summary: Compared to aqueous electrolytes, the understanding of chemical and electrochemical processes in non-aqueous electrolytes, particularly in Li-ion battery electrolytes, is limited. In this study, a comprehensive investigation of the electrochemistry of ethylene carbonate (EC) and its interaction with trace amounts of water and HF is conducted across various electrode materials. The electrocatalytic nature of EC, HF, and water electroreductions at different interfaces is revealed, and the catalytic role of water in EC electroreduction is also discovered. The composition of the solid-electrolyte interphase (SEI) is found to depend primarily on the balance between the (electro)chemistry of EC, water, and HF.
Article
Chemistry, Multidisciplinary
Wen Ju, Alexander Bagger, Nastaran Ranjbar Saharie, Sebastian Moehle, Jingyi Wang, Frederic Jaouen, Jan Rossmeisl, Peter Strasser
Summary: This study provides mechanistic insights into electrochemical carbonyl hydrogenation and can guide the development of efficient and sustainable electrocatalytic valorization of biomass-derived compounds.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Physical
Jette K. Mathiesen, Sofie Colding-Fagerholt, Kim D. Jensen, Jack K. Pedersen, Tom Vosch, Jan Rossmeisl, Stig Helveg, Kirsten M. o. Jensen
Summary: Bimetallic nanocrystals exhibit different behaviors compared to monometallic nanocrystals under gas environments. Under oxygen exposure, bimetallic nanocrystals lose metallic Cu and form metal oxide phases, but can reappear and reincorporate into the crystalline phase under a reducing atmosphere. Cu mobility promotes segregation and formation of CuO along with the formation of a monometallic phase, altering the active surface sites of the nanocatalyst.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Hao Wan, Xingli Wang, Lei Tan, Michael Filippi, Peter Strasser, Jan Rossmeisl, Alexander Bagger
Summary: Electrocatalytic conversion is a promising technology for storing renewable electricity in the chemical form, such as urea production. This study investigated the urea formation mechanism on Cu metal using density functional theory calculations. It was found that Cu can bind with NO and CO but not with H, and through NO and CO coreduction, two possible C-N coupling reactions and subsequent hydrogenation lead to urea formation. This work demonstrates the use of computational simulations in predicting selective and active materials for urea production.
