Pub Date : 2025-03-27DOI: 10.1021/acsenergylett.5c00231
Shaorui Chen, Tianzhao Hu, Tong Yu, Xianyou Luo, Lei Zhang, Feng Li
Sodium-ion batteries are an attractive alternative to lithium-ion batteries due to the abundance and cost-effectiveness and are suitable for large-scale energy storage. Carbon materials, notable for their availability, economic viability, high capacity, and stability, stand out as potential anode materials. The sodium storage performance of carbon materials is inherently determined by their structural features. Manipulating these features is key to optimizing the storage behavior. This Perspective systematically evaluates the classification and structural distinctions of existing carbon-based materials for sodium-ion batteries, summarizing different sodium storage processes and electrochemical behaviors. Structural features are categorized into intrinsic (e.g., arrangement and distribution of carbon atoms) and extrinsic (e.g., heteroatoms). The sodium storage processes and behaviors associated with these features and the corresponding regulation strategies are explored in depth. Finally, the challenges and future directions for developing high-performance carbon anodes are proposed, aiming to provide actionable insights for advancing research and commercialization efforts.
{"title":"Structural Feature Design for Carbon Materials toward Sodium Storage: Insights and Prospects","authors":"Shaorui Chen, Tianzhao Hu, Tong Yu, Xianyou Luo, Lei Zhang, Feng Li","doi":"10.1021/acsenergylett.5c00231","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00231","url":null,"abstract":"Sodium-ion batteries are an attractive alternative to lithium-ion batteries due to the abundance and cost-effectiveness and are suitable for large-scale energy storage. Carbon materials, notable for their availability, economic viability, high capacity, and stability, stand out as potential anode materials. The sodium storage performance of carbon materials is inherently determined by their structural features. Manipulating these features is key to optimizing the storage behavior. This Perspective systematically evaluates the classification and structural distinctions of existing carbon-based materials for sodium-ion batteries, summarizing different sodium storage processes and electrochemical behaviors. Structural features are categorized into intrinsic (e.g., arrangement and distribution of carbon atoms) and extrinsic (e.g., heteroatoms). The sodium storage processes and behaviors associated with these features and the corresponding regulation strategies are explored in depth. Finally, the challenges and future directions for developing high-performance carbon anodes are proposed, aiming to provide actionable insights for advancing research and commercialization efforts.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"49 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723839","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-27DOI: 10.1021/acsenergylett.4c03602
Jie Huang, Bin Qiu, Feng Xu, Jinyu Gao, Peixin Zhang, Chuanxin He, Hongwei Mi
Solid-state lithium metal batteries (LMBs) based on polymer electrolytes have become a hot topic for next-generation energy storage owing to their high specific energy, flexibility, and simple preparation process. However, poor electrolyte–electrode interface reactions and intrinsically slow Li+ transfer kinetics limit the development of solid-state LMBs. Here, a tris(4-fluorophenyl)phosphine (T4FPP) additive with strong steric hindrance and weak coordination is introduced to remodel the Li+ coordination environment to facilitate electrolyte bulk and interface charge transfer. Furthermore, theoretical analysis combined with in situ/ex situ characterizations demonstrate that the addition of T4FPP helps to construct an anion-dominated solvation structure through molecular crowding and form a LiF/Li2O-rich SEI layer. Ultimately, the LFP|Li full cell based on the T4FPP modified electrolyte works normally even at 10 C with a reversible specific capacity of 88.9 mAh g–1. Simultaneously, the electrochemical performance at 0–60 °C further verified the wide temperature range adaptability of the electrolyte.
{"title":"Steric Hindrance Manipulation in Polymer Electrolytes toward Wide-Temperature Solid-State Lithium Metal Batteries","authors":"Jie Huang, Bin Qiu, Feng Xu, Jinyu Gao, Peixin Zhang, Chuanxin He, Hongwei Mi","doi":"10.1021/acsenergylett.4c03602","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03602","url":null,"abstract":"Solid-state lithium metal batteries (LMBs) based on polymer electrolytes have become a hot topic for next-generation energy storage owing to their high specific energy, flexibility, and simple preparation process. However, poor electrolyte–electrode interface reactions and intrinsically slow Li<sup>+</sup> transfer kinetics limit the development of solid-state LMBs. Here, a tris(4-fluorophenyl)phosphine (T4FPP) additive with strong steric hindrance and weak coordination is introduced to remodel the Li<sup>+</sup> coordination environment to facilitate electrolyte bulk and interface charge transfer. Furthermore, theoretical analysis combined with <i>in situ</i>/<i>ex situ</i> characterizations demonstrate that the addition of T4FPP helps to construct an anion-dominated solvation structure through molecular crowding and form a LiF/Li<sub>2</sub>O-rich SEI layer. Ultimately, the LFP|Li full cell based on the T4FPP modified electrolyte works normally even at 10 C with a reversible specific capacity of 88.9 mAh g<sup>–1</sup>. Simultaneously, the electrochemical performance at 0–60 °C further verified the wide temperature range adaptability of the electrolyte.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"183 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143724014","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The interface between the semiconductor light absorber and the metal electrode is critical for facilitating the extraction of photogenerated charges in photoelectrodes. Achieving a lattice-matched semiconductor/electrode interface with low defect density is highly desirable but remains a challenge for Ta3N5 photoanodes. In this study, we synthesized niobium nitride thin film electrodes with controllable crystallographic phases to achieve a lattice-matched Ta3N5/Nb5N6 back contact. This results in an enhanced crystallinity of the Ta3N5 film and reduced interfacial defect density. Consequently, the photoanode with the lattice-matched back contact attains a record half-cell solar-to-hydrogen conversion efficiency of 4.1%, attributed to the bulk carrier separation efficiency of nearly 100%. This work highlights lattice-matching as an effective strategy to enhance the efficiency of thin film-based solar energy conversion devices.
{"title":"Lattice-Matched Ta3N5/Nb5N6 Interface Enables a Bulk Charge Separation Efficiency of Close to 100%","authors":"Yitong Liu, Zeyu Fan, Ronghua Li, Andraž Mavrič, Iztok Arčon, Matjaz Valant, Gregor Kapun, Beibei Zhang, Chao Feng, Zemin Zhang, Tingxi Chen, Yanning Zhang, Yanbo Li","doi":"10.1021/acsenergylett.5c00603","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00603","url":null,"abstract":"The interface between the semiconductor light absorber and the metal electrode is critical for facilitating the extraction of photogenerated charges in photoelectrodes. Achieving a lattice-matched semiconductor/electrode interface with low defect density is highly desirable but remains a challenge for Ta<sub>3</sub>N<sub>5</sub> photoanodes. In this study, we synthesized niobium nitride thin film electrodes with controllable crystallographic phases to achieve a lattice-matched Ta<sub>3</sub>N<sub>5</sub>/Nb<sub>5</sub>N<sub>6</sub> back contact. This results in an enhanced crystallinity of the Ta<sub>3</sub>N<sub>5</sub> film and reduced interfacial defect density. Consequently, the photoanode with the lattice-matched back contact attains a record half-cell solar-to-hydrogen conversion efficiency of 4.1%, attributed to the bulk carrier separation efficiency of nearly 100%. This work highlights lattice-matching as an effective strategy to enhance the efficiency of thin film-based solar energy conversion devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"72 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-27DOI: 10.1021/acsenergylett.5c00281
Xiuyu Jin, Di Huang, Qiusu Miao, Ziting Zhu, Wei Tong, Alvaro Videla, Gao Liu
Herein, we demonstrate the utility of optical microscopy as an accessible technique for the in situ visualization of dendrite growth within polymer–sulfide composite solid-state electrolytes. The composite electrolyte features in situ polymerization and cross-linking of the polymer between ceramic particles, which opens up extensive opportunities for accelerated materials discovery, given the vast array of acrylate/methacrylate monomers available. Specifically, the cross-linked polymer poly(triethylene glycol dimethacrylate) (poly(TEGDMA)) was observed to effectively fill pores and inhibit dendrite growth at the lithium metal interface, attributed to its glassy state at room temperature. This work represents the first application of optical microscopy to illustrate that the incorporation of glassy, undoped polymers such as poly(TEGDMA) can serve as a viable strategy for dendrite suppression in solid-state composite electrolytes.
{"title":"Operando Optical Microscopy for Visualization of Dendrite Growth in an Argyrodite LPSCl–Polymer Composite Electrolyte","authors":"Xiuyu Jin, Di Huang, Qiusu Miao, Ziting Zhu, Wei Tong, Alvaro Videla, Gao Liu","doi":"10.1021/acsenergylett.5c00281","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00281","url":null,"abstract":"Herein, we demonstrate the utility of optical microscopy as an accessible technique for the in situ visualization of dendrite growth within polymer–sulfide composite solid-state electrolytes. The composite electrolyte features in situ polymerization and cross-linking of the polymer between ceramic particles, which opens up extensive opportunities for accelerated materials discovery, given the vast array of acrylate/methacrylate monomers available. Specifically, the cross-linked polymer poly(triethylene glycol dimethacrylate) (poly(TEGDMA)) was observed to effectively fill pores and inhibit dendrite growth at the lithium metal interface, attributed to its glassy state at room temperature. This work represents the first application of optical microscopy to illustrate that the incorporation of glassy, undoped polymers such as poly(TEGDMA) can serve as a viable strategy for dendrite suppression in solid-state composite electrolytes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"18 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723840","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-27DOI: 10.1021/acsenergylett.5c00373
Apu Saha, Rupam Sahoo, Shyam Chand Pal, Sayaka Uchida, Madhab C. Das
The development of solid-state proton conductors (SSPCs) is of significant interest for their deployment as proton exchange membranes in fuel cell (PEMFC) technology. The aqueous medium synthesis with ample intrinsic proton sources has made crystalline polyoxometalates (POMs) promising SSPCs over others. Herein, we aim to showcase the solitary POMs and their hybrids (with polymers and MOFs/COFs) as SSPCs by organizing them based on the approaches taken up (intrinsic or extrinsic) to install various protonic sources while positioning them within specific components of the POM frameworks. Particular attention is paid with a critical discussion on whether the conductivity is purely protonic or a combination of protonic and other ionic conductivity (majorly originating from charge balancing counterions) and thus recommend the terminology to be used. The “Critical Discussion” section provides in-depth insights which are often overlooked, while the future recommendations are made in “Future Outlook”.
{"title":"Polyoxometalates (POMs) as Proton Conductors","authors":"Apu Saha, Rupam Sahoo, Shyam Chand Pal, Sayaka Uchida, Madhab C. Das","doi":"10.1021/acsenergylett.5c00373","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00373","url":null,"abstract":"The development of solid-state proton conductors (SSPCs) is of significant interest for their deployment as proton exchange membranes in fuel cell (PEMFC) technology. The <i>aqueous medium</i> synthesis with ample <i>intrinsic</i> proton sources has made crystalline polyoxometalates (POMs) promising SSPCs over others. Herein, we aim to showcase the solitary POMs and their hybrids (with polymers and MOFs/COFs) as SSPCs by organizing them based on the approaches taken up (<i>intrinsic</i> or <i>extrinsic</i>) to install various protonic sources while positioning them within specific components of the POM frameworks. Particular attention is paid with a critical discussion on whether the conductivity is purely protonic or a combination of protonic and other ionic conductivity (majorly originating from charge balancing counterions) and thus recommend the terminology to be used. The “Critical Discussion” section provides in-depth insights which are often overlooked, while the future recommendations are made in “Future Outlook”.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143724015","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Perovskite microstructure is one of the key factors limiting the effectiveness of current machine learning (ML) approaches for designing perovskite solar cells (PSCs) with high power conversion efficiency (PCE). This work develops a multimodal convolutional neural network to extract microstructural features from scanning electron microscopy (SEM) images of perovskite thin films. The model dynamically adjusts the weights of different modal information, including material composition, processing techniques, and microstructure, to enhance predictive accuracy. The model achieves an impressive coefficient of determination (R2) of 0.79 on the 1,583 SEM images data set. By introducing six SEM image features to describe the grain size of PSCs, we found that a grain boundary length density (GBLD) below 5.96 and an equivalent circular diameter (ECD) above 0.83 significantly enhance the PCE. Additional experiments confirmed the effectiveness of the results, and by improving these parameters to alter the crystallization, the PCE was increased to 24.61%, and the consistency of the results demonstrated the effectiveness and rationality of the multimodal model.
{"title":"Integration of Microstructural Image Data into Machine Learning Models for Advancing High-Performance Perovskite Solar Cell Design","authors":"Haotian Liu, Antai Yang, Chengquan Zhong, Xu Zhu, Hao Meng, Zhuo Feng, Jixin Tang, Chen Yang, Jingzi Zhang, Jiakai Liu, Kailong Hu, Xi Lin","doi":"10.1021/acsenergylett.5c00626","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00626","url":null,"abstract":"Perovskite microstructure is one of the key factors limiting the effectiveness of current machine learning (ML) approaches for designing perovskite solar cells (PSCs) with high power conversion efficiency (PCE). This work develops a multimodal convolutional neural network to extract microstructural features from scanning electron microscopy (SEM) images of perovskite thin films. The model dynamically adjusts the weights of different modal information, including material composition, processing techniques, and microstructure, to enhance predictive accuracy. The model achieves an impressive coefficient of determination (<i>R</i><sup>2</sup>) of 0.79 on the 1,583 SEM images data set. By introducing six SEM image features to describe the grain size of PSCs, we found that a grain boundary length density (GBLD) below 5.96 and an equivalent circular diameter (ECD) above 0.83 significantly enhance the PCE. Additional experiments confirmed the effectiveness of the results, and by improving these parameters to alter the crystallization, the PCE was increased to 24.61%, and the consistency of the results demonstrated the effectiveness and rationality of the multimodal model.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"59 1","pages":"1884-1891"},"PeriodicalIF":22.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713429","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-26DOI: 10.1021/acsenergylett.5c00271
Jiguo Tu, Bokun Zhang, Yan Li, Xiaoyun Wang, Shuqiang Jiao
High-voltage Co-free LiNi0.5Mn1.5O4 (LNMO) is considered a promising candidate for next-generation high-performance lithium-ion batteries. However, there is a significant absence of full understanding of elaborate evolution of crystal structures. This review article aims to thoroughly examine the latest advancements in state-of-the-art LNMO and establish a systematic framework that outlines the varied phase evolution mechanisms under different synthesis conditions and during cycling from the perspective of the crystal structure. First, an analysis of the intrinsic structural properties of LNMO is conducted for optimizing the synthesis process, including crystal orientation, oxygen deficiency, disorder–order transition, and surface phase reconstruction under various synthesis conditions. Then, the phase transformation mechanisms during cycling have been systematically elucidated to develop strategies to mitigate any detrimental effects and improve the electrochemical performance. Finally, the insights into further development directions in LNMO are offered at relevant length scales from the crystal structure level to the electrode level.
{"title":"Comprehensive Crystal Structural Insights into Phase Evolution of Spinel Co-Free Lithium Nickel Manganese Oxide","authors":"Jiguo Tu, Bokun Zhang, Yan Li, Xiaoyun Wang, Shuqiang Jiao","doi":"10.1021/acsenergylett.5c00271","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00271","url":null,"abstract":"High-voltage Co-free LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> (LNMO) is considered a promising candidate for next-generation high-performance lithium-ion batteries. However, there is a significant absence of full understanding of elaborate evolution of crystal structures. This review article aims to thoroughly examine the latest advancements in state-of-the-art LNMO and establish a systematic framework that outlines the varied phase evolution mechanisms under different synthesis conditions and during cycling from the perspective of the crystal structure. First, an analysis of the intrinsic structural properties of LNMO is conducted for optimizing the synthesis process, including crystal orientation, oxygen deficiency, disorder–order transition, and surface phase reconstruction under various synthesis conditions. Then, the phase transformation mechanisms during cycling have been systematically elucidated to develop strategies to mitigate any detrimental effects and improve the electrochemical performance. Finally, the insights into further development directions in LNMO are offered at relevant length scales from the crystal structure level to the electrode level.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":"1892-1910"},"PeriodicalIF":22.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-25DOI: 10.1021/acsenergylett.4c03562
Xirui Zhang, Yangsen Xu, Kang Xu, Liyan Chen, Feng Zhu, Fan He, Zhiwei Du, Wei Yuan, Yu Chen
Developing air electrode materials with high catalytic activity and durability of oxygen reduction/evolution reactions is an important solution to address the performance and stability problems of reversible protonic ceramic electrochemical cells (R-PCECs). This work reports an active and durable misfit-layered air electrode with a chemical formula of Ca3Co3.8Mo0.2O9+δ. A low area-specific resistance of 0.13 Ω cm2 with reasonable operation stability over 100 h is achieved in the air with 30% steam at 650 °C, likely attributed to the fast surface exchange kinetics and bulk diffusion processes. A single cell with this electrode demonstrates outstanding performance in fuel cell and electrolysis modes, with a peak power density of 1.62 W cm–2 and an electrolysis current density of −2.98 A cm–2 at 650 °C. Most notably, Mo ions doped in air electrodes significantly enhance the cell’s operational reversibility stability, with no observed performance degradation after 52 reversible cycles and over 200 h in dual modes of fuel and electrolysis cell tests.
{"title":"An Active and Durable Misfit-Layered Air Electrode for Reversible Protonic Ceramic Electrochemical Cells","authors":"Xirui Zhang, Yangsen Xu, Kang Xu, Liyan Chen, Feng Zhu, Fan He, Zhiwei Du, Wei Yuan, Yu Chen","doi":"10.1021/acsenergylett.4c03562","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03562","url":null,"abstract":"Developing air electrode materials with high catalytic activity and durability of oxygen reduction/evolution reactions is an important solution to address the performance and stability problems of reversible protonic ceramic electrochemical cells (R-PCECs). This work reports an active and durable misfit-layered air electrode with a chemical formula of Ca<sub>3</sub>Co<sub>3.8</sub>Mo<sub>0.2</sub>O<sub>9+δ</sub>. A low area-specific resistance of 0.13 Ω cm<sup>2</sup> with reasonable operation stability over 100 h is achieved in the air with 30% steam at 650 °C, likely attributed to the fast surface exchange kinetics and bulk diffusion processes. A single cell with this electrode demonstrates outstanding performance in fuel cell and electrolysis modes, with a peak power density of 1.62 W cm<sup>–2</sup> and an electrolysis current density of −2.98 A cm<sup>–2</sup> at 650 °C. Most notably, Mo ions doped in air electrodes significantly enhance the cell’s operational reversibility stability, with no observed performance degradation after 52 reversible cycles and over 200 h in dual modes of fuel and electrolysis cell tests.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"20 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695828","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-24DOI: 10.1021/acsenergylett.5c00490
Abdullah Al Shafe, Saqlain Raza, Reece Henry, Jun Liu, Brendan T. O’Connor
Self-assembled monolayers (SAMs) are promising interface layers in organic photovoltaic (OPV) cells. Phosphonic acid-based SAMs, such as 2PACz, have shown improved efficiency over the commonly used PEDOT:PSS hole transport layer. This study examines the impact of 2PACz and its variants (MeO-2PACz, Cl-2PACz, Br-2PACz) on not only device performance but also interfacial adhesion. T-peel and shear strength tests show that 2PACz increases interfacial peel and shear strength more than 3-fold compared to PEDOT:PSS, whereas the halogenated SAMs do not enhance adhesion significantly. Molecular dynamic simulations of the photoactive molecules on the SAMs reveal that 2PACz exhibits stronger interaction energy with PM6 than the halogenated SAMs, consistent with adhesion measurements. The improved adhesion when using 2PACz relative to the other SAMs is attributed to greater conformational freedom allowing for more intimate packing with the polymer semiconductor. These findings demonstrate the potential of SAM interlayers to enhance OPV efficiency and mechanical reliability and that adhesion is sensitive to small variations of the SAM structure.
{"title":"Improving Adhesion in Organic Photovoltaic Cells with Self-Assembled Monolayers","authors":"Abdullah Al Shafe, Saqlain Raza, Reece Henry, Jun Liu, Brendan T. O’Connor","doi":"10.1021/acsenergylett.5c00490","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00490","url":null,"abstract":"Self-assembled monolayers (SAMs) are promising interface layers in organic photovoltaic (OPV) cells. Phosphonic acid-based SAMs, such as 2PACz, have shown improved efficiency over the commonly used PEDOT:PSS hole transport layer. This study examines the impact of 2PACz and its variants (MeO-2PACz, Cl-2PACz, Br-2PACz) on not only device performance but also interfacial adhesion. T-peel and shear strength tests show that 2PACz increases interfacial peel and shear strength more than 3-fold compared to PEDOT:PSS, whereas the halogenated SAMs do not enhance adhesion significantly. Molecular dynamic simulations of the photoactive molecules on the SAMs reveal that 2PACz exhibits stronger interaction energy with PM6 than the halogenated SAMs, consistent with adhesion measurements. The improved adhesion when using 2PACz relative to the other SAMs is attributed to greater conformational freedom allowing for more intimate packing with the polymer semiconductor. These findings demonstrate the potential of SAM interlayers to enhance OPV efficiency and mechanical reliability and that adhesion is sensitive to small variations of the SAM structure.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695830","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-03-24DOI: 10.1021/acsenergylett.5c00117
Xiaoming Liu, Zhengwu Fang, Yubin Zhang, Yan Wang, W. Beck Andrews, Katsuyo Thornton, Neil P. Dasgupta, Miaofang Chi
Realizing solid electrolytes with low grain-boundary (GB) resistance is critical for advancing all-solid-state batteries. High GB resistance in SEs is often attributed to deficiencies in mobile ions at these boundaries; yet, when and how these deficiencies form during synthesis remain unclear. Here, we use a unique in situ scanning transmission electron microscopy setup to guide solid electrolyte crystallization during annealing, enabling real-time observation of GB formation at the atomic scale, with Li0.33La0.56TiO3 as a model SE. We reveal an ultrathin, less than 1.5 nm thick, lithium-deficient layer that emerges at the crystallization front upon crystallization and persists as two adjacent crystals fuse to form a GB. We offer two hypotheses for the origin of the lithium-deficient layer, one based on thermodynamic stabilization and the other on kinetic constraints. Our results provide guidelines for designing synthesis strategies to reduce GB resistance in solid electrolytes.
{"title":"Unraveling the Origin of Grain Boundary Lithium Deficiency in Ceramic Solid Electrolytes","authors":"Xiaoming Liu, Zhengwu Fang, Yubin Zhang, Yan Wang, W. Beck Andrews, Katsuyo Thornton, Neil P. Dasgupta, Miaofang Chi","doi":"10.1021/acsenergylett.5c00117","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00117","url":null,"abstract":"Realizing solid electrolytes with low grain-boundary (GB) resistance is critical for advancing all-solid-state batteries. High GB resistance in SEs is often attributed to deficiencies in mobile ions at these boundaries; yet, when and how these deficiencies form during synthesis remain unclear. Here, we use a unique in situ scanning transmission electron microscopy setup to guide solid electrolyte crystallization during annealing, enabling real-time observation of GB formation at the atomic scale, with Li<sub>0.33</sub>La<sub>0.56</sub>TiO<sub>3</sub> as a model SE. We reveal an ultrathin, less than 1.5 nm thick, lithium-deficient layer that emerges at the crystallization front upon crystallization and persists as two adjacent crystals fuse to form a GB. We offer two hypotheses for the origin of the lithium-deficient layer, one based on thermodynamic stabilization and the other on kinetic constraints. Our results provide guidelines for designing synthesis strategies to reduce GB resistance in solid electrolytes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"21 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695829","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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