Pub Date : 2025-01-25DOI: 10.1021/acsenergylett.4c0325610.1021/acsenergylett.4c03256
Ke Zhou, Sijian Lu, Charles Mish, Yu-Ting Chen, Shijie Feng, Jiyoung Kim, Min-Sang Song, Hyunsun Alicia Kim* and Ping Liu*,
The practical application of all-solid-state batteries (ASSBs) requires reliable operation at low pressures, which remains a significant challenge. In this work, we examine the role of a cathode composite microstructure composed of solid-state electrolyte (SSE) with different particle sizes. A composite made of LiNi0.8Co0.1Mn0.1O2 (NCM811) and fine-particle Li6PS5Cl (LPSC) shows a more uniform distribution of SSE on the surface of NCM811 particles, ensuring intimate contact. Moreover, the composite features reduced tortuosity, which enhances Li ion conduction. These microstructural advantages result in significantly reduced charge transfer resistance, helping to suppress mechanical distortion and electrochemical degradation during cycling under low-pressure conditions. As a result, the fine-LPSC cathode composite exhibits enhanced cycling stability at a moderate stack pressure of 2 MPa, outperforming its coarse-LPSC counterpart. Our finding confirms the important role of microstructure design in enabling high-performance ASSBs operating under low-pressure conditions.
{"title":"Tailored Cathode Composite Microstructure Enables Long Cycle Life at Low Pressure for All-Solid-State Batteries","authors":"Ke Zhou, Sijian Lu, Charles Mish, Yu-Ting Chen, Shijie Feng, Jiyoung Kim, Min-Sang Song, Hyunsun Alicia Kim* and Ping Liu*, ","doi":"10.1021/acsenergylett.4c0325610.1021/acsenergylett.4c03256","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03256https://doi.org/10.1021/acsenergylett.4c03256","url":null,"abstract":"<p >The practical application of all-solid-state batteries (ASSBs) requires reliable operation at low pressures, which remains a significant challenge. In this work, we examine the role of a cathode composite microstructure composed of solid-state electrolyte (SSE) with different particle sizes. A composite made of LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) and fine-particle Li<sub>6</sub>PS<sub>5</sub>Cl (LPSC) shows a more uniform distribution of SSE on the surface of NCM811 particles, ensuring intimate contact. Moreover, the composite features reduced tortuosity, which enhances Li ion conduction. These microstructural advantages result in significantly reduced charge transfer resistance, helping to suppress mechanical distortion and electrochemical degradation during cycling under low-pressure conditions. As a result, the fine-LPSC cathode composite exhibits enhanced cycling stability at a moderate stack pressure of 2 MPa, outperforming its coarse-LPSC counterpart. Our finding confirms the important role of microstructure design in enabling high-performance ASSBs operating under low-pressure conditions.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"966–974 966–974"},"PeriodicalIF":19.3,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402214","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 : 2025-01-25DOI: 10.1021/acsenergylett.4c0317610.1021/acsenergylett.4c03176
Jiao Lin, Wei Li and Zheng Chen*,
Lithium-ion batteries (LIBs) are indispensable for modern technology, yet their limited lifespan contributes substantially to electronic waste. Effective recycling methods are crucial to mitigating material scarcity, enhancing sustainability, and fostering a circular economy. This perspective examines the current LIB recycling processes, with a focus on the emerging potential and challenges of direct recycling methods. Unlike traditional pyrometallurgy and hydrometallurgy, which often destroy valuable materials, direct recycling seeks to recover and restore functional components, preserving the integrity of active materials. However, this method faces significant technical hurdles, particularly due to the complex design of LIBs and the degradation of key components over time. This perspective explores the intricacies of battery structure and component degradation, examines the challenges of scaling up direct recycling for industry applications, and proposes future directions to improve the efficiency and viability of this sustainable recycling approach.
{"title":"Scaling Direct Recycling of Lithium-Ion Batteries toward Industrialization: Challenges and Opportunities","authors":"Jiao Lin, Wei Li and Zheng Chen*, ","doi":"10.1021/acsenergylett.4c0317610.1021/acsenergylett.4c03176","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03176https://doi.org/10.1021/acsenergylett.4c03176","url":null,"abstract":"<p >Lithium-ion batteries (LIBs) are indispensable for modern technology, yet their limited lifespan contributes substantially to electronic waste. Effective recycling methods are crucial to mitigating material scarcity, enhancing sustainability, and fostering a circular economy. This perspective examines the current LIB recycling processes, with a focus on the emerging potential and challenges of direct recycling methods. Unlike traditional pyrometallurgy and hydrometallurgy, which often destroy valuable materials, direct recycling seeks to recover and restore functional components, preserving the integrity of active materials. However, this method faces significant technical hurdles, particularly due to the complex design of LIBs and the degradation of key components over time. This perspective explores the intricacies of battery structure and component degradation, examines the challenges of scaling up direct recycling for industry applications, and proposes future directions to improve the efficiency and viability of this sustainable recycling approach.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"947–957 947–957"},"PeriodicalIF":19.3,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402212","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 : 2025-01-24DOI: 10.1021/acsenergylett.4c03046
Yiwu Zhu, Feng He
With the rapid advancements in the power conversion efficiency (PCE) of organic photovoltaic (OPV) devices, their stability has garnered increasing attention. While material innovation has played a critical role in recent years, the Q-PHJ (quasi-planar heterojunction) architecture offers an alternative approach to device optimization. This article aims to explain how the introduction of the Q-PHJ architecture can mitigate degradation under various conditions without compromising device performance. It begins by illustrating the fundamental mechanisms responsible for the degradation of OPV devices. Following this, the advantages of the Q-PHJ device and the mechanism are explained by introducing our recent work as well as highlighting other researchers’ work in this field. Different aspects and factors such as morphology, the ternary strategy, additive engineering, and vertical distribution were analyzed. The role of material innovation is also discussed. In the end, the feasibility and challenges of applying bilayer and bilayer-dominated devices to industrial manufacturing are analyzed in detail.
{"title":"Quasi-Planar Heterojunction: Enhancing Stability and Practicality in Organic Photovoltaics","authors":"Yiwu Zhu, Feng He","doi":"10.1021/acsenergylett.4c03046","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03046","url":null,"abstract":"With the rapid advancements in the power conversion efficiency (PCE) of organic photovoltaic (OPV) devices, their stability has garnered increasing attention. While material innovation has played a critical role in recent years, the Q-PHJ (quasi-planar heterojunction) architecture offers an alternative approach to device optimization. This article aims to explain how the introduction of the Q-PHJ architecture can mitigate degradation under various conditions without compromising device performance. It begins by illustrating the fundamental mechanisms responsible for the degradation of OPV devices. Following this, the advantages of the Q-PHJ device and the mechanism are explained by introducing our recent work as well as highlighting other researchers’ work in this field. Different aspects and factors such as morphology, the ternary strategy, additive engineering, and vertical distribution were analyzed. The role of material innovation is also discussed. In the end, the feasibility and challenges of applying bilayer and bilayer-dominated devices to industrial manufacturing are analyzed in detail.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"38 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026801","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 : 2025-01-24DOI: 10.1021/acsenergylett.4c0304610.1021/acsenergylett.4c03046
Yiwu Zhu, and , Feng He*,
With the rapid advancements in the power conversion efficiency (PCE) of organic photovoltaic (OPV) devices, their stability has garnered increasing attention. While material innovation has played a critical role in recent years, the Q-PHJ (quasi-planar heterojunction) architecture offers an alternative approach to device optimization. This article aims to explain how the introduction of the Q-PHJ architecture can mitigate degradation under various conditions without compromising device performance. It begins by illustrating the fundamental mechanisms responsible for the degradation of OPV devices. Following this, the advantages of the Q-PHJ device and the mechanism are explained by introducing our recent work as well as highlighting other researchers’ work in this field. Different aspects and factors such as morphology, the ternary strategy, additive engineering, and vertical distribution were analyzed. The role of material innovation is also discussed. In the end, the feasibility and challenges of applying bilayer and bilayer-dominated devices to industrial manufacturing are analyzed in detail.
{"title":"Quasi-Planar Heterojunction: Enhancing Stability and Practicality in Organic Photovoltaics","authors":"Yiwu Zhu, and , Feng He*, ","doi":"10.1021/acsenergylett.4c0304610.1021/acsenergylett.4c03046","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03046https://doi.org/10.1021/acsenergylett.4c03046","url":null,"abstract":"<p >With the rapid advancements in the power conversion efficiency (PCE) of organic photovoltaic (OPV) devices, their stability has garnered increasing attention. While material innovation has played a critical role in recent years, the Q-PHJ (quasi-planar heterojunction) architecture offers an alternative approach to device optimization. This article aims to explain how the introduction of the Q-PHJ architecture can mitigate degradation under various conditions without compromising device performance. It begins by illustrating the fundamental mechanisms responsible for the degradation of OPV devices. Following this, the advantages of the Q-PHJ device and the mechanism are explained by introducing our recent work as well as highlighting other researchers’ work in this field. Different aspects and factors such as morphology, the ternary strategy, additive engineering, and vertical distribution were analyzed. The role of material innovation is also discussed. In the end, the feasibility and challenges of applying bilayer and bilayer-dominated devices to industrial manufacturing are analyzed in detail.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"935–946 935–946"},"PeriodicalIF":19.3,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402202","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 : 2025-01-23DOI: 10.1021/acsenergylett.4c0323310.1021/acsenergylett.4c03233
Mengde Zhai, Kaihuai Du, Chengyang Liu, Cheng Chen, Guixiang Li*, Haoxin Wang, Ziyang Xia, Jinman Yang, Hui Xu, Aili Wang*, Toshinori Matsushima, Zhanglin Guo, Meng Li, Antonio Abate, Paul J. Dyson, Mohammad Khaja Nazeeruddin and Ming Cheng*,
Spiro-OMeTAD is a widely used hole transport material (HTM) in perovskite solar cells (PSCs), but its inherent low hole mobility and poor thermal stability affect the overall performance of PSCs. To overcome these limitations, we develop a series of fluorene-terminated Spiro-type HTMs, engineered by modulating the fluorene substitution site and π-conjugated intensity. Among these, the p-BM material exhibits high energetic ordering in film, appropriate energy levels, and efficient carrier extraction, enabling PSCs to achieve power conversion efficiencies (PCEs) of 25.5% and 24.03% for aperture areas of 0.0625 and 1 cm2, respectively. Additionally, a perovskite solar mini-module (size 16 cm2) based on p-BM HTM achieved a PCE of 22.4%. More importantly, p-BM exhibits a high glass transition temperature and enhanced film hydrophobicity, significantly improving the stability of devices in relation to heat and humidity. Our findings provide a promising alternative HTM for developing efficient and stable perovskite photovoltaic devices.
{"title":"Fluorene-Terminated π-Conjugated Spiro-Type Hole Transport Materials for Perovskite Solar Cells","authors":"Mengde Zhai, Kaihuai Du, Chengyang Liu, Cheng Chen, Guixiang Li*, Haoxin Wang, Ziyang Xia, Jinman Yang, Hui Xu, Aili Wang*, Toshinori Matsushima, Zhanglin Guo, Meng Li, Antonio Abate, Paul J. Dyson, Mohammad Khaja Nazeeruddin and Ming Cheng*, ","doi":"10.1021/acsenergylett.4c0323310.1021/acsenergylett.4c03233","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03233https://doi.org/10.1021/acsenergylett.4c03233","url":null,"abstract":"<p >Spiro-OMeTAD is a widely used hole transport material (HTM) in perovskite solar cells (PSCs), but its inherent low hole mobility and poor thermal stability affect the overall performance of PSCs. To overcome these limitations, we develop a series of fluorene-terminated Spiro-type HTMs, engineered by modulating the fluorene substitution site and π-conjugated intensity. Among these, the <i>p</i>-BM material exhibits high energetic ordering in film, appropriate energy levels, and efficient carrier extraction, enabling PSCs to achieve power conversion efficiencies (PCEs) of 25.5% and 24.03% for aperture areas of 0.0625 and 1 cm<sup>2</sup>, respectively. Additionally, a perovskite solar mini-module (size 16 cm<sup>2</sup>) based on <i>p</i>-BM HTM achieved a PCE of 22.4%. More importantly, <i>p</i>-BM exhibits a high glass transition temperature and enhanced film hydrophobicity, significantly improving the stability of devices in relation to heat and humidity. Our findings provide a promising alternative HTM for developing efficient and stable perovskite photovoltaic devices.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"915–924 915–924"},"PeriodicalIF":19.3,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c03233","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402082","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-23DOI: 10.1021/acsenergylett.4c0336910.1021/acsenergylett.4c03369
Shixuan Liu, Di Wu, Minghua Kong, Wu Wang, Lin Xie and Jiaqing He*,
Thermoelectric conversion technology can realize direct conversion between heat and electricity, providing a promising approach to relieve the energy crisis. The application of thermoelectric technology is closely related to materials’ thermoelectric and mechanical properties. However, the strong coupling of key parameters involving charge carriers and phonon transport hinders the substantial improvements in overall thermoelectric performance. In recent years, a high-entropy strategy promoted remarkable progress in the field of thermoelectric materials by leveraging the four core effects. In this review, we first discuss the theoretical basis for how a high-entropy strategy synergistically optimizes thermoelectric performance. We then classify the examples where high-entropy effects can optimize electrical, thermal, and mechanical properties in thermoelectric materials. Following this, we summarize the overall advances that the high-entropy strategy has brought to thermoelectric materials and devices. Finally, we point out the remaining challenges in high-entropy thermoelectrics and offer perspectives on future research directions in this field.
{"title":"High-Entropy Thermoelectric Materials: Advances, Challenges, and Future Opportunities","authors":"Shixuan Liu, Di Wu, Minghua Kong, Wu Wang, Lin Xie and Jiaqing He*, ","doi":"10.1021/acsenergylett.4c0336910.1021/acsenergylett.4c03369","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03369https://doi.org/10.1021/acsenergylett.4c03369","url":null,"abstract":"<p >Thermoelectric conversion technology can realize direct conversion between heat and electricity, providing a promising approach to relieve the energy crisis. The application of thermoelectric technology is closely related to materials’ thermoelectric and mechanical properties. However, the strong coupling of key parameters involving charge carriers and phonon transport hinders the substantial improvements in overall thermoelectric performance. In recent years, a high-entropy strategy promoted remarkable progress in the field of thermoelectric materials by leveraging the four core effects. In this review, we first discuss the theoretical basis for how a high-entropy strategy synergistically optimizes thermoelectric performance. We then classify the examples where high-entropy effects can optimize electrical, thermal, and mechanical properties in thermoelectric materials. Following this, we summarize the overall advances that the high-entropy strategy has brought to thermoelectric materials and devices. Finally, we point out the remaining challenges in high-entropy thermoelectrics and offer perspectives on future research directions in this field.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 2","pages":"925–934 925–934"},"PeriodicalIF":19.3,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143402198","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 : 2025-01-23DOI: 10.1021/acsenergylett.4c03233
Mengde Zhai, Kaihuai Du, Chengyang Liu, Cheng Chen, Guixiang Li, Haoxin Wang, Ziyang Xia, Jinman Yang, Hui Xu, Aili Wang, Toshinori Matsushima, Zhanglin Guo, Meng Li, Antonio Abate, Paul J. Dyson, Mohammad Khaja Nazeeruddin, Ming Cheng
Spiro-OMeTAD is a widely used hole transport material (HTM) in perovskite solar cells (PSCs), but its inherent low hole mobility and poor thermal stability affect the overall performance of PSCs. To overcome these limitations, we develop a series of fluorene-terminated Spiro-type HTMs, engineered by modulating the fluorene substitution site and π-conjugated intensity. Among these, the p-BM material exhibits high energetic ordering in film, appropriate energy levels, and efficient carrier extraction, enabling PSCs to achieve power conversion efficiencies (PCEs) of 25.5% and 24.03% for aperture areas of 0.0625 and 1 cm2, respectively. Additionally, a perovskite solar mini-module (size 16 cm2) based on p-BM HTM achieved a PCE of 22.4%. More importantly, p-BM exhibits a high glass transition temperature and enhanced film hydrophobicity, significantly improving the stability of devices in relation to heat and humidity. Our findings provide a promising alternative HTM for developing efficient and stable perovskite photovoltaic devices.
{"title":"Fluorene-Terminated π-Conjugated Spiro-Type Hole Transport Materials for Perovskite Solar Cells","authors":"Mengde Zhai, Kaihuai Du, Chengyang Liu, Cheng Chen, Guixiang Li, Haoxin Wang, Ziyang Xia, Jinman Yang, Hui Xu, Aili Wang, Toshinori Matsushima, Zhanglin Guo, Meng Li, Antonio Abate, Paul J. Dyson, Mohammad Khaja Nazeeruddin, Ming Cheng","doi":"10.1021/acsenergylett.4c03233","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03233","url":null,"abstract":"Spiro-OMeTAD is a widely used hole transport material (HTM) in perovskite solar cells (PSCs), but its inherent low hole mobility and poor thermal stability affect the overall performance of PSCs. To overcome these limitations, we develop a series of fluorene-terminated Spiro-type HTMs, engineered by modulating the fluorene substitution site and π-conjugated intensity. Among these, the <i>p</i>-BM material exhibits high energetic ordering in film, appropriate energy levels, and efficient carrier extraction, enabling PSCs to achieve power conversion efficiencies (PCEs) of 25.5% and 24.03% for aperture areas of 0.0625 and 1 cm<sup>2</sup>, respectively. Additionally, a perovskite solar mini-module (size 16 cm<sup>2</sup>) based on <i>p</i>-BM HTM achieved a PCE of 22.4%. More importantly, <i>p</i>-BM exhibits a high glass transition temperature and enhanced film hydrophobicity, significantly improving the stability of devices in relation to heat and humidity. Our findings provide a promising alternative HTM for developing efficient and stable perovskite photovoltaic devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"39 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019992","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 : 2025-01-23DOI: 10.1021/acsenergylett.4c03369
Shixuan Liu, Di Wu, Minghua Kong, Wu Wang, Lin Xie, Jiaqing He
Thermoelectric conversion technology can realize direct conversion between heat and electricity, providing a promising approach to relieve the energy crisis. The application of thermoelectric technology is closely related to materials’ thermoelectric and mechanical properties. However, the strong coupling of key parameters involving charge carriers and phonon transport hinders the substantial improvements in overall thermoelectric performance. In recent years, a high-entropy strategy promoted remarkable progress in the field of thermoelectric materials by leveraging the four core effects. In this review, we first discuss the theoretical basis for how a high-entropy strategy synergistically optimizes thermoelectric performance. We then classify the examples where high-entropy effects can optimize electrical, thermal, and mechanical properties in thermoelectric materials. Following this, we summarize the overall advances that the high-entropy strategy has brought to thermoelectric materials and devices. Finally, we point out the remaining challenges in high-entropy thermoelectrics and offer perspectives on future research directions in this field.
{"title":"High-Entropy Thermoelectric Materials: Advances, Challenges, and Future Opportunities","authors":"Shixuan Liu, Di Wu, Minghua Kong, Wu Wang, Lin Xie, Jiaqing He","doi":"10.1021/acsenergylett.4c03369","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03369","url":null,"abstract":"Thermoelectric conversion technology can realize direct conversion between heat and electricity, providing a promising approach to relieve the energy crisis. The application of thermoelectric technology is closely related to materials’ thermoelectric and mechanical properties. However, the strong coupling of key parameters involving charge carriers and phonon transport hinders the substantial improvements in overall thermoelectric performance. In recent years, a high-entropy strategy promoted remarkable progress in the field of thermoelectric materials by leveraging the four core effects. In this review, we first discuss the theoretical basis for how a high-entropy strategy synergistically optimizes thermoelectric performance. We then classify the examples where high-entropy effects can optimize electrical, thermal, and mechanical properties in thermoelectric materials. Following this, we summarize the overall advances that the high-entropy strategy has brought to thermoelectric materials and devices. Finally, we point out the remaining challenges in high-entropy thermoelectrics and offer perspectives on future research directions in this field.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"82 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019994","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 : 2025-01-22DOI: 10.1021/acsenergylett.4c03073
Nuerbiya Aihemaiti, Siying Peng
Lead halide perovskites are one of the most promising materials as active layers of optoelectronic devices. Phase segregation under illumination in mixed halide perovskites is one of the major issues in stable device operation. Herein, we rationalize illumination power dependent phase segregation phenomena, including two thresholds between which phase segregation occurs, and the reversal of phase segregation. Our experimental observation combining confocal photoluminescence mapping with in situ Raman spectroscopy supports the halide oxidation model. We observed phase segregation beyond the illuminated area, while the illuminated area remained mixed. Reversal of phase segregation under illumination was also observed. We propose that the spatial distribution of phase segregation is driven by halide oxidation and diffusion of the products through mass flow, as verified by light- and spatial-dependent lattice halide vibrations. Our insights into phase segregation may provide new perspectives for manipulating phase segregation by local light intensity for dynamically tunable optoelectronics.
{"title":"Rationalizing Light-Induced Phase Segregation Reversal by Halide Oxidation and Diffusion in Mixed Halide Perovskites","authors":"Nuerbiya Aihemaiti, Siying Peng","doi":"10.1021/acsenergylett.4c03073","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03073","url":null,"abstract":"Lead halide perovskites are one of the most promising materials as active layers of optoelectronic devices. Phase segregation under illumination in mixed halide perovskites is one of the major issues in stable device operation. Herein, we rationalize illumination power dependent phase segregation phenomena, including two thresholds between which phase segregation occurs, and the reversal of phase segregation. Our experimental observation combining confocal photoluminescence mapping with in situ Raman spectroscopy supports the halide oxidation model. We observed phase segregation beyond the illuminated area, while the illuminated area remained mixed. Reversal of phase segregation under illumination was also observed. We propose that the spatial distribution of phase segregation is driven by halide oxidation and diffusion of the products through mass flow, as verified by light- and spatial-dependent lattice halide vibrations. Our insights into phase segregation may provide new perspectives for manipulating phase segregation by local light intensity for dynamically tunable optoelectronics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"28 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019995","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}
Lithium–aluminum (LixAl, x = the molar ratio of Li to Al), an important alloy anode with a specific capacity over 2 times higher than that of the carbon anode used in commercial liquid electrolyte lithium-ion batteries (LELIBs), has been proven to be a failure in LELIBs due to the notorious pulverization phenomenon. However, whether or not such pulverization persists in all solid state lithium batteries (ASSLBs) remains unclear. Herein, we show that pulverization of the LixAl anode is mitigated in ASSLBs due to the applied external stack pressure, thus preventing the mechanical failure of the LixAl anode in ASSLBs. Moreover, electron microscopy investigation reveals that, instead of pulverization, electrochemomechanical stress induces 2 orders of magnitude grain size reduction from a few tens of microns to a few hundred nanometers. The grain-refined LixAl anode facilitates lithium ion transport, which improves the rate performance and specific capacity of the LixAl anode. Consequently, the assembled single-crystal LiNi0.83Co0.12Mn0.05O2|Li10Si0.3PS6.7Cl1.8|Li0.4Al ASSLBs reach 2000 cycles with a capacity retention of 100% at 3C (13.9 mA/cm2, room temperature), at a high areal capacity of 2.1 mAh/cm2. The all-solid pouch cell with a LixAl anode can reach an energy density of 219 Wh kg–1 based on the total mass of the cell. These results demonstrate the prospect of implementing the Al-based anode in ASSLBs for practical energy storage applications.
锂铝(LixAl, x = Li to Al的摩尔比)是一种重要的合金阳极,其比容量比商用液态电解质锂离子电池(LELIBs)中使用的碳阳极高出2倍以上,但由于其臭名昭著的粉状现象,已被证明在LELIBs中是失败的。然而,这种粉末化是否在所有固态锂电池(asslb)中持续存在尚不清楚。本文表明,由于施加了外部堆叠压力,asslb中LixAl阳极的粉碎化得到了缓解,从而防止了asslb中LixAl阳极的机械失效。此外,电子显微镜研究表明,电化学力学应力导致晶粒尺寸减小2个数量级,从几十微米到几百纳米。晶粒细化的LixAl阳极有利于锂离子的输运,提高了LixAl阳极的倍率性能和比容量。因此,组装的单晶LiNi0.83Co0.12Mn0.05O2|Li10Si0.3PS6.7Cl1.8|Li0.4Al asslb在3C (13.9 mA/cm2,室温)下可达到2000次循环,容量保持率为100%,面积容量高达2.1 mAh/cm2。基于电池总质量,采用LixAl阳极的全固体袋状电池可以达到219 Wh kg-1的能量密度。这些结果显示了在asslb中实现铝基阳极用于实际储能应用的前景。
{"title":"Electrochemical Grain Refinement Enables High-Performance Lithium–Aluminum-Anode-Based All-Solid-State Batteries","authors":"Lun Zhang, Xuedong Zhang, Baiyu Guo, Zhaoyu Rong, Zhihao Yan, Bo Wang, Menglin Li, Zhenyu Wang, Lingyun Zhu, Qiao Huang, Yongfu Tang, Jianyu Huang","doi":"10.1021/acsenergylett.4c03250","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03250","url":null,"abstract":"Lithium–aluminum (Li<sub><i>x</i></sub>Al, <i>x</i> = the molar ratio of Li to Al), an important alloy anode with a specific capacity over 2 times higher than that of the carbon anode used in commercial liquid electrolyte lithium-ion batteries (LELIBs), has been proven to be a failure in LELIBs due to the notorious pulverization phenomenon. However, whether or not such pulverization persists in all solid state lithium batteries (ASSLBs) remains unclear. Herein, we show that pulverization of the Li<sub><i>x</i></sub>Al anode is mitigated in ASSLBs due to the applied external stack pressure, thus preventing the mechanical failure of the Li<sub><i>x</i></sub>Al anode in ASSLBs. Moreover, electron microscopy investigation reveals that, instead of pulverization, electrochemomechanical stress induces 2 orders of magnitude grain size reduction from a few tens of microns to a few hundred nanometers. The grain-refined Li<sub><i>x</i></sub>Al anode facilitates lithium ion transport, which improves the rate performance and specific capacity of the Li<sub><i>x</i></sub>Al anode. Consequently, the assembled single-crystal LiNi<sub>0.83</sub>Co<sub>0.12</sub>Mn<sub>0.05</sub>O<sub>2</sub>|Li<sub>10</sub>Si<sub>0.3</sub>PS<sub>6.7</sub>Cl<sub>1.8</sub>|Li<sub>0.4</sub>Al ASSLBs reach 2000 cycles with a capacity retention of 100% at 3C (13.9 mA/cm<sup>2</sup>, room temperature), at a high areal capacity of 2.1 mAh/cm<sup>2</sup>. The all-solid pouch cell with a Li<sub><i>x</i></sub>Al anode can reach an energy density of 219 Wh kg<sup>–1</sup> based on the total mass of the cell. These results demonstrate the prospect of implementing the Al-based anode in ASSLBs for practical energy storage applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"49 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019996","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}