ACS Materials LettersPub Date : 2024-10-08DOI: 10.1021/acsenergylett.4c0208110.1021/acsenergylett.4c02081
Xu Dong, Alexander Mayer, Zhen Chen, Stefano Passerini* and Dominic Bresser*,
{"title":"Advanced Single-Ion Conducting Block Copolymer Electrolyte for Safer and Less Costly Lithium–Metal Batteries","authors":"Xu Dong, Alexander Mayer, Zhen Chen, Stefano Passerini* and Dominic Bresser*, ","doi":"10.1021/acsenergylett.4c0208110.1021/acsenergylett.4c02081","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02081https://doi.org/10.1021/acsenergylett.4c02081","url":null,"abstract":"<p >High-performance polymer electrolyte systems for lithium–metal batteries (LMBs) commonly contain a relatively high amount of fluorine to stabilize the electrode|electrolyte interfaces, particularly that with lithium metal. Herein, we report an advanced single-ion conducting polymer electrolyte that contains less fluorine in the backbone than previous systems, enabling a significant cost reduction, while still providing highly stable cycling of LMB cells containing LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> (NCM<sub>622</sub>) and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM<sub>811</sub>) positive electrodes. Moreover, we show that the choice of the incorporated “molecular transporters”, i.e., small molecules with high mobility and a high dielectric constant to facilitate the Li<sup>+</sup> transport, is essential for achieving high-performance LMB cells. In fact, the transition from pure ethylene carbonate to a mixture with propylene carbonate allows for an extended electrochemical stability toward oxidation and higher limiting current density, resulting in enhanced rate capability and cycling stability of Li∥NCM cells─and the possibility to cycle these cells also at ambient temperature.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5279–5287 5279–5287"},"PeriodicalIF":19.3,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609459","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-07DOI: 10.1021/acsenergylett.4c0201910.1021/acsenergylett.4c02019
Saul Perez-Beltran, Dacheng Kuai and Perla B. Balbuena*,
{"title":"SEI Formation and Lithium-Ion Electrodeposition Dynamics in Lithium Metal Batteries via First-Principles Kinetic Monte Carlo Modeling","authors":"Saul Perez-Beltran, Dacheng Kuai and Perla B. Balbuena*, ","doi":"10.1021/acsenergylett.4c0201910.1021/acsenergylett.4c02019","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02019https://doi.org/10.1021/acsenergylett.4c02019","url":null,"abstract":"<p >The stabilization and enhanced performance of lithium metal batteries (LMBs) depend on the formation and evolution of the Solid Electrolyte Interphase (SEI) layer as a critical component for regulating the Li metal electrodeposition processes. This study employs a first-principles kinetic Monte Carlo (kMC) model to simulate the SEI formation and Li<sup>+</sup> electrodeposition processes on a lithium metal anode, integrating both the electrochemical electrolyte reduction reactions and the diffusion events giving place to the SEI aggregation processes during battery charge and discharge processes. The model replicates the competitive interactions between organic and inorganic SEI components, emphasizing the influence of the cycling regime. Results indicate that grain boundaries within the SEI facilitate faster lithium-ion transport compared to crystalline regions, crucial for improving the performance and stability of LMBs. The findings underscore the importance of dynamic SEI modeling for further development of next-generation high-energy-density batteries.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5268–5278 5268–5278"},"PeriodicalIF":19.3,"publicationDate":"2024-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c02019","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609561","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-03DOI: 10.1021/acsenergylett.4c0193110.1021/acsenergylett.4c01931
Suhwan Kim, Hyobin Lee, Jaejin Lim, Joonam Park and Yong Min Lee*,
{"title":"Digital Twin Battery Modeling and Simulations: A New Analysis and Design Tool for Rechargeable Batteries","authors":"Suhwan Kim, Hyobin Lee, Jaejin Lim, Joonam Park and Yong Min Lee*, ","doi":"10.1021/acsenergylett.4c0193110.1021/acsenergylett.4c01931","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01931https://doi.org/10.1021/acsenergylett.4c01931","url":null,"abstract":"<p >The intricate correlation between microstructural properties and performance in lithium rechargeable batteries necessitates advanced methods to elucidate their mechanisms. In this regard, digital twin simulations have been utilized by creating virtual replicas that simulate battery behaviors and performances under various conditions. However, the relationship between microstructural parameters and battery performances is still not fully understood. This focus review aims to revisit the state of digital twin simulations, with a particular focus on its effectiveness for analyzing microstructures and unraveling the hidden parameters. For this purpose, we explore microstructure formation and validation methods as top-down and bottom-up simulation techniques and provide a comprehensive view of multiphysics approaches for understanding the electrochemical, mechanical, and thermal behaviors. Finally, we discuss the potential of artificial intelligence (AI)-driven multiscale modeling strategies and dynamic simulations, offering insights into how digital twin technology can advance battery design and optimization for enhanced performance and safety.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5225–5239 5225–5239"},"PeriodicalIF":19.3,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407456","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-03DOI: 10.1021/acsenergylett.4c0235010.1021/acsenergylett.4c02350
Michal Ronovský, Olivia Dunseath, Tomáš Hrbek, Peter Kúš, Matija Gatalo, Shlomi Polani, Jan Kubát, Daniel Götz, Hridya Nedumkulam, Andrea Sartori, Enrico Petrucco, Francisco Ruiz-Zepeda, Nejc Hodnik, Alex Martinez Bonastre, Peter Strasser and Jakub Drnec*,
{"title":"Origins of Nanoalloy Catalysts Degradation during Membrane Electrode Assembly Fabrication","authors":"Michal Ronovský, Olivia Dunseath, Tomáš Hrbek, Peter Kúš, Matija Gatalo, Shlomi Polani, Jan Kubát, Daniel Götz, Hridya Nedumkulam, Andrea Sartori, Enrico Petrucco, Francisco Ruiz-Zepeda, Nejc Hodnik, Alex Martinez Bonastre, Peter Strasser and Jakub Drnec*, ","doi":"10.1021/acsenergylett.4c0235010.1021/acsenergylett.4c02350","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02350https://doi.org/10.1021/acsenergylett.4c02350","url":null,"abstract":"<p >Despite extensive efforts to reduce the costs of high-performance electrochemical devices, incorporating catalyst materials frequently falls short of achieving performance targets. Platinum alloys, known for their high oxygen reduction activity, exemplify this challenge due to integration difficulties. Here, we introduce an in situ X-ray diffraction approach to investigate structural changes in PtCo and PtNi catalysts during ink preparation. Contrary to previous assumptions that acidity is the main factor driving catalyst dissolution, our findings demonstrate that temperature plays a more critical role. Additionally, we observe rapid structural degradation during the hot-pressing of catalyst-coated membranes (CCMs), a critical yet often unavoidable processing step. These results indicate that significant catalyst deactivation can occur before operation, emphasizing the need for optimized fabrication processes. This study highlights the importance of refining ink formulation and processing protocols to fully leverage advanced materials in CCM-based energy conversion systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5251–5258 5251–5258"},"PeriodicalIF":19.3,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407462","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-03DOI: 10.1021/acsenergylett.4c0221810.1021/acsenergylett.4c02218
Suraj Yadav, Manasi Pranav, Chandrasekhar Gangadharappa, Mathias Huss-Hansen, Matthias Schwartzkopf, Jakob Kjelstrup-Hansen, Matti Knaapila and Satish Patil*,
{"title":"Rational Third Component Choices Drive Enhanced Morphology and Efficiency in Ternary Blend Organic Solar Cells","authors":"Suraj Yadav, Manasi Pranav, Chandrasekhar Gangadharappa, Mathias Huss-Hansen, Matthias Schwartzkopf, Jakob Kjelstrup-Hansen, Matti Knaapila and Satish Patil*, ","doi":"10.1021/acsenergylett.4c0221810.1021/acsenergylett.4c02218","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02218https://doi.org/10.1021/acsenergylett.4c02218","url":null,"abstract":"<p >The impetus to add a third component in ternary blend organic solar cells (TBSCs) maximizes the light-harvesting capability of the active layer. Beyond this, the third component can perform other useful functions, such as enhancing the morphology and charge transport, and assisting in resonance energy transfer. Currently, there are no established guidelines for selecting the third component in TBSCs to optimize the organic solar cell (OSC) performance. By varying the chromophore chain length of perylene diimide (PDI) molecules, we revealed its influence on the morphology of the thin film and the efficiency of PM6:Y6 OSCs. Detailed optical and electrical characterization and morphological studies revealed that molecular size and PDIs’ chromophore chain length are pivotal to improving the performance of OSCs. The PDI monomer acts as an additive to improve the morphology and light-harvesting capability of TBSCs. This study presents several significant findings, including the dual role of the third component, the influence of the chromophore chain length on morphology, and the dynamics of excited states.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5259–5267 5259–5267"},"PeriodicalIF":19.3,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407463","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-03DOI: 10.1021/acsenergylett.4c0208610.1021/acsenergylett.4c02086
Jin Da Tan, Balamurugan Ramalingam*, Vijila Chellappan, Nipun Kumar Gupta, Laurent Dillard, Saif A. Khan, Casey Galvin and Kedar Hippalgaonkar*,
{"title":"Generative Design and Experimental Validation of Non-Fullerene Acceptors for Photovoltaics","authors":"Jin Da Tan, Balamurugan Ramalingam*, Vijila Chellappan, Nipun Kumar Gupta, Laurent Dillard, Saif A. Khan, Casey Galvin and Kedar Hippalgaonkar*, ","doi":"10.1021/acsenergylett.4c0208610.1021/acsenergylett.4c02086","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02086https://doi.org/10.1021/acsenergylett.4c02086","url":null,"abstract":"<p >The utilization of non-fullerene acceptors (NFA) in organic photovoltaic (OPV) devices offers advantages over fullerene-based acceptors, including lower costs and improved light absorption. Despite advances in small molecule generative design, experimental validation frameworks are often lacking. This study introduces a comprehensive pipeline for generating, virtual screening, and synthesizing potential NFAs for high-efficiency OPVs, integrating generative and predictive ML models with expert knowledge. Iterative refinement ensured the synthetic feasibility of the generated molecules, using the diketopyrrolopyrrole (DPP) core motif to manually generate NFA candidates meeting stringent synthetic criteria. These candidates were virtually screened using a predictive ML model based on power conversion efficiency (PCE) calculations from the modified Scharber model (PCE<sub>MS</sub>). We successfully synthesized seven NFA candidates, each requiring three or fewer steps. Experimental HOMO and LUMO measurements yielded calculated PCE<sub>MS</sub> values from 6.7% to 11.8%. This study demonstrates an effective pipeline for discovering OPV NFA candidates by integrating generative and predictive ML models.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5240–5250 5240–5250"},"PeriodicalIF":19.3,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-02DOI: 10.1021/acsenergylett.4c0251410.1021/acsenergylett.4c02514
Silver-Hamill Turren-Cruz*, Jorge Pascual, Shuaifeng Hu, Jesus Sanchez-Diaz, Sergio Galve-Lahoz, Wentao Liu, Wolfram Hempel, Vladimir S. Chirvony, Juan P. Martinez-Pastor, Pablo P. Boix, Atsushi Wakamiya* and Iván Mora-Seró*,
{"title":"Correction to “Multicomponent Approach for Stable Methylammonium-Free Tin–Lead Perovskite Solar Cells”","authors":"Silver-Hamill Turren-Cruz*, Jorge Pascual, Shuaifeng Hu, Jesus Sanchez-Diaz, Sergio Galve-Lahoz, Wentao Liu, Wolfram Hempel, Vladimir S. Chirvony, Juan P. Martinez-Pastor, Pablo P. Boix, Atsushi Wakamiya* and Iván Mora-Seró*, ","doi":"10.1021/acsenergylett.4c0251410.1021/acsenergylett.4c02514","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02514https://doi.org/10.1021/acsenergylett.4c02514","url":null,"abstract":"","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5206 5206"},"PeriodicalIF":19.3,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c02514","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-02DOI: 10.1021/acsenergylett.4c0197610.1021/acsenergylett.4c01976
Nutpaphat Jarulertwathana, Kyuwon Lee, Hyeseung Shin, Eui-Jung Ryu, In Soo Kim, Cheon Woo Moon and Jerome K. Hyun*,
{"title":"A Black State from Reversible Copper Electrodeposition without Metal Additives","authors":"Nutpaphat Jarulertwathana, Kyuwon Lee, Hyeseung Shin, Eui-Jung Ryu, In Soo Kim, Cheon Woo Moon and Jerome K. Hyun*, ","doi":"10.1021/acsenergylett.4c0197610.1021/acsenergylett.4c01976","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01976https://doi.org/10.1021/acsenergylett.4c01976","url":null,"abstract":"<p >Metal electrodeposition and dissolution on a transparent electrode enable dynamic switching between the opaque and transparent states, respectively. To be used as dynamic windows, a fully black state must be achieved while maintaining reversibility. Cu is a top candidate that meets the latter criterion but fails the former, producing its characteristic orange tint. As a result, metal additives are often mixed with Cu ions but at the expense of some degree of reversibility. Here, a truly black state is achieved without metal additives by enhancing the dissipative interaction between light and Cu. A galvanic etching method is used to transform a flat ITO surface into an array of nanopillars, forming a gradually varying index across the ITO interface. This elongates the light absorption path length over all wavelengths once Cu is electrodeposited. The electrode is demonstrated in dynamically tunable devices including one that transitions between mirror-like and opaque states with a coloration efficiency of 20.3 cm<sup>2</sup> C<sup>–1</sup>. These results highlight the potential of our strategy in light management devices, particularly for energy-conserving dynamic windows.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5207–5214 5207–5214"},"PeriodicalIF":19.3,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407550","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Materials LettersPub Date : 2024-10-02DOI: 10.1021/acsenergylett.4c0240310.1021/acsenergylett.4c02403
Borong Li, Weicheng Zhang, Kang Yang, Long Li, Jing Luo, Qingqing Lin, Yichen Li, Zheyuan Liu*, Lingyun Li*, Yan Yu* and Chengkai Yang*,
{"title":"Bridging Atomic and Macroscopic Perspectives on Heteroepitaxial Growth in Lithium Metal Anodes","authors":"Borong Li, Weicheng Zhang, Kang Yang, Long Li, Jing Luo, Qingqing Lin, Yichen Li, Zheyuan Liu*, Lingyun Li*, Yan Yu* and Chengkai Yang*, ","doi":"10.1021/acsenergylett.4c0240310.1021/acsenergylett.4c02403","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02403https://doi.org/10.1021/acsenergylett.4c02403","url":null,"abstract":"<p >Studying lithium growth on diverse substrates with unique crystal structures is crucial for linking atomic and macroscopic views, which ensures a long cycle life and safety in lithium metal batteries. This work provides explanations on (1) the stages of nucleation, which are influenced by the adsorption-relaxation mechanism, (2) acquiring evolved traits of dendritic morphology from the embryo, and (3) the integration of the atomic and macroscopic perspectives through a variety of techniques at different scales to validate dendrite evolution. The heteroepitaxial growth process of the embryos is divided into two principal stages: nucleation and growth. The adsorption-type substrates exhibit characteristics of relatively lower average interaction energy and specific stress energy during the nucleation stage. At the growth stage, the adsorption-type substrate tends to facilitate multilayer growth. This work provides potential to design and material selection for lithium metal batteries, contributing to the development of safer, more efficient, and longer-lasting energy storage systems.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5215–5224 5215–5224"},"PeriodicalIF":19.3,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407649","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Effects of Solvation and Temperature on the Energetics of BiVO4 Surfaces with Varying Composition for Solar Water Splitting","authors":"Giacomo Melani, Wennie Wang, Francois Gygi, Kyoung-Shin Choi and Giulia Galli*, ","doi":"10.1021/acsenergylett.4c0191310.1021/acsenergylett.4c01913","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01913https://doi.org/10.1021/acsenergylett.4c01913","url":null,"abstract":"<p >Photoelectrodes used in solar water splitting must operate in aqueous media. However, computational studies that explicitly compare the dry and solvated photoelectrode energetics at finite temperature and the impact of the photoelectrode surface composition and surface defects are lacking. Here, we used first-principles molecular dynamics simulations to investigate the solvation and thermal effects on the energetics of the BiVO<sub>4</sub>(010) surface with different surface compositions and oxygen vacancies, a common defect responsible for the intrinsic n-type behavior of BiVO<sub>4</sub>. We find that the alignment of the photoelectrode electronic bands with the water redox potentials is modified in the presence of water and that solvation effects and thermal fluctuations are more prominent for Bi-rich surfaces, especially so in the presence of oxygen vacancies. Our results provide a detailed understanding of the behavior of BiVO<sub>4</sub> photoanodes operating in aqueous media, as a function of surface composition, and are directly comparable with experiments.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 10","pages":"5166–5171 5166–5171"},"PeriodicalIF":19.3,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142407820","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}