The integration of reversible photochromism and multicolor luminescence modulation in transparent glass offers significant potential for high-capacity, nonvolatile 3D optical storage. However, achieving effective multicolor luminescence modulation and 3D patterning remains a challenge. This study introduces a Mn2+/Sb5+ charge compensation mechanism to induce purple photochromism in gallium silicate glass via the Mn2+ → Mn3+ transition under 532 nm laser irradiation. The effect is fully reversible, with efficient thermal erasure. By codoping Tb3+ and Mn2+, wavelength-independent red and green luminescence modulation enables multidimensional optical encoding. Arbitrary 3D photochromic patterns are directly inscribed using a 532 nm laser and decoded via tunable luminescence. This multimodal system advances 4D optical storage by combining 3D spatial dimensions with tunable luminescence intensity multiplexing. Mn2+/Tb3+ doped gallium silicate glass represents a breakthrough for 3D information display, data encryption, and insights into photochromic mechanisms in transition-metal-doped photonic systems.
{"title":"Direct 3D Lithography of Reversible Photochromic Patterns with Tunable Luminescence in Amorphous Transparent Media","authors":"Heping Zhao, Jiayan Liao, Shasha Fu, Yingzhu Zi, Xue Bai, Yang Ci, Yueteng Zhang, Xinhao Cai, Yuewei Li, Yangke Cun, Anjun Huang, Yue Liu, Jianbei Qiu, Zhiguo Song, Guogang Li, Ji Zhou, Zhengwen Yang","doi":"10.1021/acsenergylett.5c00024","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00024","url":null,"abstract":"The integration of reversible photochromism and multicolor luminescence modulation in transparent glass offers significant potential for high-capacity, nonvolatile 3D optical storage. However, achieving effective multicolor luminescence modulation and 3D patterning remains a challenge. This study introduces a Mn<sup>2+</sup>/Sb<sup>5+</sup> charge compensation mechanism to induce purple photochromism in gallium silicate glass via the Mn<sup>2+</sup> → Mn<sup>3+</sup> transition under 532 nm laser irradiation. The effect is fully reversible, with efficient thermal erasure. By codoping Tb<sup>3+</sup> and Mn<sup>2+</sup>, wavelength-independent red and green luminescence modulation enables multidimensional optical encoding. Arbitrary 3D photochromic patterns are directly inscribed using a 532 nm laser and decoded via tunable luminescence. This multimodal system advances 4D optical storage by combining 3D spatial dimensions with tunable luminescence intensity multiplexing. Mn<sup>2+</sup>/Tb<sup>3+</sup> doped gallium silicate glass represents a breakthrough for 3D information display, data encryption, and insights into photochromic mechanisms in transition-metal-doped photonic systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"51 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495796","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 dendrite penetration has caused internal short-circuits that have limited the life of lithium metal all-solid-state batteries. Defects and pores in dry compacted solid electrolytes promote dendrite growth. This study introduces an organic molecular coating, 1-undecanethiol, that anchors strongly to the surface of Li6PS5Cl and functions as an adsorbed lubrication layer, thus reducing interparticle friction, facilitating particle rearrangement and densification. Under a compacting pressure of 375 MPa, the 1-undecanethiol coated Li6PS5Cl achieves a porosity of 1.7%, a substantial reduction from the porosity of 10.9% for Li6PS5Cl. As a result, Li symmetric cells incorporating the 1-undecanethiol densified Li6PS5Cl pellet exhibit up to a 4-fold increase in critical current density and demonstrate remarkable 4600 h cycling at a current density of 1 mA cm–2. Likewise, the Li||LiNi0.8Co0.1Mn0.1O2 full cell shows a 4-fold increase in cycling current density. This work points to the potential of organic surface engineering to enable long-life solid-state batteries.
{"title":"Densifying Solid Electrolytes through Surface Lubrication to Mitigate Shorting of Solid-State Batteries","authors":"Mengchen Liu, Ershuang Lu, Shen Wang, Shijie Feng, Junwei Gao, Wenlin Yan, Jeong Woo Oh, Min-Sang Song, Jian Luo, Ping Liu","doi":"10.1021/acsenergylett.4c03387","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03387","url":null,"abstract":"Lithium dendrite penetration has caused internal short-circuits that have limited the life of lithium metal all-solid-state batteries. Defects and pores in dry compacted solid electrolytes promote dendrite growth. This study introduces an organic molecular coating, 1-undecanethiol, that anchors strongly to the surface of Li<sub>6</sub>PS<sub>5</sub>Cl and functions as an adsorbed lubrication layer, thus reducing interparticle friction, facilitating particle rearrangement and densification. Under a compacting pressure of 375 MPa, the 1-undecanethiol coated Li<sub>6</sub>PS<sub>5</sub>Cl achieves a porosity of 1.7%, a substantial reduction from the porosity of 10.9% for Li<sub>6</sub>PS<sub>5</sub>Cl. As a result, Li symmetric cells incorporating the 1-undecanethiol densified Li<sub>6</sub>PS<sub>5</sub>Cl pellet exhibit up to a 4-fold increase in critical current density and demonstrate remarkable 4600 h cycling at a current density of 1 mA cm<sup>–2</sup>. Likewise, the Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> full cell shows a 4-fold increase in cycling current density. This work points to the potential of organic surface engineering to enable long-life solid-state batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495797","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}
Tin halide perovskites are promising materials to replace lead-based materials for perovskite optoelectronics, yet their performance is limited by their high self-p-doping. To quantify the impact of p-doping on carrier dynamics, we combine terahertz spectroscopy and density functional theory calculations to investigate the coupling of charge carriers to the lattice in prototypical tin-based perovskites. Doping is shown to influence the charge-phonon interactions significantly. We identify the formation of polarons at doping densities below 1018 cm–3, while a Drude-like response is found for photogenerated carriers at higher charge density, confirming that for highly p-doped systems, the terahertz response is dominated by quasi-free charge carriers. Our study suggests that charge-phonon coupling could serve as a proxy for the self-p-doping level, offering additional insights into fundamental charge-transport properties of tin halide perovskites and their potential optimization for photovoltaic applications.
{"title":"Charge-Phonon Coupling in Tin Halide Perovskites","authors":"Lorenzo Gatto, Isabella Poli, Daniele Meggiolaro, Federico Grandi, Giulia Folpini, Antonella Treglia, Eugenio Cinquanta, Annamaria Petrozza, Filippo De Angelis, Caterina Vozzi","doi":"10.1021/acsenergylett.4c02558","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02558","url":null,"abstract":"Tin halide perovskites are promising materials to replace lead-based materials for perovskite optoelectronics, yet their performance is limited by their high self-p-doping. To quantify the impact of p-doping on carrier dynamics, we combine terahertz spectroscopy and density functional theory calculations to investigate the coupling of charge carriers to the lattice in prototypical tin-based perovskites. Doping is shown to influence the charge-phonon interactions significantly. We identify the formation of polarons at doping densities below 10<sup>18</sup> cm<sup>–3</sup>, while a Drude-like response is found for photogenerated carriers at higher charge density, confirming that for highly p-doped systems, the terahertz response is dominated by quasi-free charge carriers. Our study suggests that charge-phonon coupling could serve as a proxy for the self-p-doping level, offering additional insights into fundamental charge-transport properties of tin halide perovskites and their potential optimization for photovoltaic applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"6 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495798","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}
Li6PS5I based solid-state electrolytes (SSEs) show promising interface compatibility for all-solid-state batteries (ASSBs), but they still suffer from limited ionic conductivity. Herein, a superionic conductor lithium argyrodite sulfide, Li7–x(GeSi)(1–x)/2SbxS5I, was developed through multi-cation substitution of Ge, Si, and Sb for P, increasing configurational entropy of the Li6PS5I. This approach enhanced Li+ content and anion site disorder, leading to a low activation energy of 0.17 eV for Li+ migration, and consequently a high cold-pressed ionic conductivity of 12.7 mS cm–1, and a record value of 32.2 mS cm–1 after hot-pressing. When incorporating Li3InCl6 as the catholyte and interlayer, the LiNi0.8Co0.1Mn0.1O2@Li3InCl6|Li3InCl6|Li20/3(GeSiSb)1/3S5I|Li-In ASSBs exhibited a high capacity of 219 mAh g–1 at 0.1 C, and a notable capacity of 135 mAh g–1 with 84.4% retention at 1 C after 550 cycles. Our ASSBs demonstrated stable cycling across −20 to 60 °C and operated well at an ultrahigh cathode loading of 100 mg cm–2. These findings advance sulfide SSEs for high-performance and wide-temperature ASSBs.
{"title":"A Superionic Conductor Lithium Argyrodite Sulfide of Li7–x(GeSi)(1–x)/2SbxS5I toward All-Solid-State Lithium-Ion Batteries","authors":"Yuxin Ma, Daokuan Jin, Haodong Shi, Rui Li, Yutao Niu, Yunyun Xu, Cong Dong, Yangyang Liu, Rui Yang, Guiming Zhong, Chunyang Wang, Zhizhen Zhang, Zhangquan Peng, Zhong-Shuai Wu","doi":"10.1021/acsenergylett.4c03115","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03115","url":null,"abstract":"Li<sub>6</sub>PS<sub>5</sub>I based solid-state electrolytes (SSEs) show promising interface compatibility for all-solid-state batteries (ASSBs), but they still suffer from limited ionic conductivity. Herein, a superionic conductor lithium argyrodite sulfide, Li<sub>7–<i>x</i></sub>(GeSi)<sub>(1–<i>x</i>)/2</sub>Sb<sub><i>x</i></sub>S<sub>5</sub>I, was developed through multi-cation substitution of Ge, Si, and Sb for P, increasing configurational entropy of the Li<sub>6</sub>PS<sub>5</sub>I. This approach enhanced Li<sup>+</sup> content and anion site disorder, leading to a low activation energy of 0.17 eV for Li<sup>+</sup> migration, and consequently a high cold-pressed ionic conductivity of 12.7 mS cm<sup>–1</sup>, and a record value of 32.2 mS cm<sup>–1</sup> after hot-pressing. When incorporating Li<sub>3</sub>InCl<sub>6</sub> as the catholyte and interlayer, the LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>@Li<sub>3</sub>InCl<sub>6</sub>|Li<sub>3</sub>InCl<sub>6</sub>|Li<sub>20/3</sub>(GeSiSb)<sub>1/3</sub>S<sub>5</sub>I|Li-In ASSBs exhibited a high capacity of 219 mAh g<sup>–1</sup> at 0.1 C, and a notable capacity of 135 mAh g<sup>–1</sup> with 84.4% retention at 1 C after 550 cycles. Our ASSBs demonstrated stable cycling across −20 to 60 °C and operated well at an ultrahigh cathode loading of 100 mg cm<sup>–2</sup>. These findings advance sulfide SSEs for high-performance and wide-temperature ASSBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486432","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 : 2025-02-24DOI: 10.1021/acsenergylett.5c00349
Qiong Yuan, Wei Gao, Jingbo L. Liu
The Presidential Symposium (PRES) at the Fall Meeting, hosted by the American Chemical Society (ACS) in Denver, CO, brought together a diverse group of professionals and experts from chemistry, chemical engineering, and other fields. They presented their research discoveries and convened a panel of interdisciplinary researchers to discuss innovative and practical solutions to energy sustainability challenges and the advancement of smart materials. This PRES event, organized by leaders from the Chinese American Chemical Society (CACS) under guidance from the ACS President’s Office, focused on “Achievements in Elevating the Chemistry Enterprise: Advancing Energy Transition and Smart Materials.” The symposium focused on variable-property materials and energy systems, aiming for net-zero emissions and a circular economy. Presentations and discussions highlighted leading-edge research in energy consumption, materials development, and climate change. The event promoted community building and identified new opportunities, facilitating dialogue and knowledge exchange among academia, industry, government laboratories, and nonprofits. Topics included hydrogen production, carbon capture and conversion, sustainable biofuels, natural polymers, energy storage and conversion, and entrepreneurship in energy transition. Discussions addressed tuning nanosystem dimensionality, enhancing material electrochemical properties, and advancing nanomaterial manufacturing from lab to market. Machine-learning methods for self-regulating nanomaterials and innovative applications in sustainable energy were also featured. This PRES event laid a foundation for future research directions, emphasizing collaborative efforts and strategic planning for energy sustainability and intelligent materials innovation. It provided key insights and practical solutions, promoting innovative advancements in the field. The leadership of the ACS, including Drs. Mary Carroll, Marinda Wu, and H. N. Cheng, provided comprehensive guidance to ensure the smooth operation of the PRES events (Figure 1). Their expertise and strategic direction were instrumental in addressing key challenges and facilitating successful outcomes. Their leadership was critical for the event to proceed seamlessly, promoting valuable discussions and fostering a collaborative atmosphere. Dr. Mary K. Carroll (Figure 1a), the Dwane W. Crichton Professor of Chemistry at Union College and the 2024 ACS president, provided strategic guidelines for the event. Her goals include promoting research dissemination, valuing science communication, encouraging outreach activities, and increasing ACS’s diversity. With extensive experience and dedication, Dr. Carroll aims to enhance ACS’s global impact and effectively communicate the benefits of chemistry. With over 40 years of experience in the chemical industry, Dr. Marinda Li Wu (Figure 1b) has held critical research and senior management roles. A staunch advocate for STEM education and chemi
{"title":"Achievements in Elevating the Chemistry Enterprise: Advancing Energy Transition and Smart Materials","authors":"Qiong Yuan, Wei Gao, Jingbo L. Liu","doi":"10.1021/acsenergylett.5c00349","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00349","url":null,"abstract":"The Presidential Symposium (PRES) at the Fall Meeting, hosted by the American Chemical Society (ACS) in Denver, CO, brought together a diverse group of professionals and experts from chemistry, chemical engineering, and other fields. They presented their research discoveries and convened a panel of interdisciplinary researchers to discuss innovative and practical solutions to energy sustainability challenges and the advancement of smart materials. This PRES event, organized by leaders from the Chinese American Chemical Society (CACS) under guidance from the ACS President’s Office, focused on “Achievements in Elevating the Chemistry Enterprise: Advancing Energy Transition and Smart Materials.” The symposium focused on variable-property materials and energy systems, aiming for net-zero emissions and a circular economy. Presentations and discussions highlighted leading-edge research in energy consumption, materials development, and climate change. The event promoted community building and identified new opportunities, facilitating dialogue and knowledge exchange among academia, industry, government laboratories, and nonprofits. Topics included hydrogen production, carbon capture and conversion, sustainable biofuels, natural polymers, energy storage and conversion, and entrepreneurship in energy transition. Discussions addressed tuning nanosystem dimensionality, enhancing material electrochemical properties, and advancing nanomaterial manufacturing from lab to market. Machine-learning methods for self-regulating nanomaterials and innovative applications in sustainable energy were also featured. This PRES event laid a foundation for future research directions, emphasizing collaborative efforts and strategic planning for energy sustainability and intelligent materials innovation. It provided key insights and practical solutions, promoting innovative advancements in the field. The leadership of the ACS, including Drs. Mary Carroll, Marinda Wu, and H. N. Cheng, provided comprehensive guidance to ensure the smooth operation of the PRES events (Figure 1). Their expertise and strategic direction were instrumental in addressing key challenges and facilitating successful outcomes. Their leadership was critical for the event to proceed seamlessly, promoting valuable discussions and fostering a collaborative atmosphere. Dr. Mary K. Carroll (Figure 1a), the Dwane W. Crichton Professor of Chemistry at Union College and the 2024 ACS president, provided strategic guidelines for the event. Her goals include promoting research dissemination, valuing science communication, encouraging outreach activities, and increasing ACS’s diversity. With extensive experience and dedication, Dr. Carroll aims to enhance ACS’s global impact and effectively communicate the benefits of chemistry. With over 40 years of experience in the chemical industry, Dr. Marinda Li Wu (Figure 1b) has held critical research and senior management roles. A staunch advocate for STEM education and chemi","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"16 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486418","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 : 2025-02-24DOI: 10.1021/acsenergylett.5c00034
Miao Zeng, Zhongliang Yan, Xinyu Ye, Yu Lou, Tao Sheng, Xianyuan Jiang, Yulin Mao, Arui Huang, Xueying Yang, Zhaojin Wang, Yuanmiao Sun, Yang Bai, Hui-Ming Cheng, Guichuan Xing
The efficiency and lifetime of tin halide perovskite solar cells (THPSCs) lag far behind those of their lead counterparts, which is mainly attributed to the low-quality of tin perovskite films as a result of their poorly controlled crystallization. Here, we introduce 3D polydentate methyl-β-cyclodextrin (CD) on top of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), and such a supramolecular interlayer leads to well-regulated crystallization. The attenuate coordination between CD and ammonium at the supramolecular interface facilitates the nucleation rate, and the multisite interaction in different spatial directions retards their crystal growth, resulting in denser and defect-less tin perovskite films. Moreover, such a supramolecular interlayer not only enables better energy alignment but also weakens the acidity of PEDOT:PSS. As a result, the efficiency of THPSCs with a tailored supramolecular interface is increased to 14.94% with a new record-high VOC of up to 1.017 V, and the unencapsulated devices exhibit an outstanding stability after nearly 4000 h of storage.
{"title":"Tailored Supramolecular Interface Enables Efficient and Stable Tin Halide Perovskite Photovoltaics","authors":"Miao Zeng, Zhongliang Yan, Xinyu Ye, Yu Lou, Tao Sheng, Xianyuan Jiang, Yulin Mao, Arui Huang, Xueying Yang, Zhaojin Wang, Yuanmiao Sun, Yang Bai, Hui-Ming Cheng, Guichuan Xing","doi":"10.1021/acsenergylett.5c00034","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00034","url":null,"abstract":"The efficiency and lifetime of tin halide perovskite solar cells (THPSCs) lag far behind those of their lead counterparts, which is mainly attributed to the low-quality of tin perovskite films as a result of their poorly controlled crystallization. Here, we introduce 3D polydentate methyl-β-cyclodextrin (CD) on top of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), and such a supramolecular interlayer leads to well-regulated crystallization. The attenuate coordination between CD and ammonium at the supramolecular interface facilitates the nucleation rate, and the multisite interaction in different spatial directions retards their crystal growth, resulting in denser and defect-less tin perovskite films. Moreover, such a supramolecular interlayer not only enables better energy alignment but also weakens the acidity of PEDOT:PSS. As a result, the efficiency of THPSCs with a tailored supramolecular interface is increased to 14.94% with a new record-high <i>V</i><sub>OC</sub> of up to 1.017 V, and the unencapsulated devices exhibit an outstanding stability after nearly 4000 h of storage.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"15 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477628","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}
Plasmonic metal/semiconductor hetero-nanostructures have attracted tremendous research interests in optoelectronic devices, photocatalysis and photothermal therapy, and related fields. Among various mechanisms of localized surface plasmon resonance (LSPR) induced enhancements, the mechanism of LSPR-induced hot carrier injection has emerged as a particularly powerful and efficient process for modulating charge dynamics, especially in photocatalysis. The efficiency of these hot carrier injections relies on robust metal–semiconductor interfaces, with performance heavily influenced by the composition, crystallinity, and atomic structure of the multi-interfaces involved. This letter explores the mechanisms of LSPR-induced hot carrier injection, highlighting recent advances with emphasis on multi-interfacial engineering to optimize charge dynamics and utilization. These interface-regulated hot carrier processes, combined with enhanced photocatalytic performance, provide new opportunities for further advanced photocatalysis and a wide range of photoelectric conversion applications.
{"title":"Plasmon Mediated Photocatalysis: Engineering Interfaces for Effective Hot Carrier Utilization","authors":"Xinyuan Li, Bohan Wu, Xurui Zhang, Akang Chen, Jiale Wang, Honglei Wang, Artur Ciesielski, Jia Liu, Jiatao Zhang","doi":"10.1021/acsenergylett.5c00090","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00090","url":null,"abstract":"Plasmonic metal/semiconductor hetero-nanostructures have attracted tremendous research interests in optoelectronic devices, photocatalysis and photothermal therapy, and related fields. Among various mechanisms of localized surface plasmon resonance (LSPR) induced enhancements, the mechanism of LSPR-induced hot carrier injection has emerged as a particularly powerful and efficient process for modulating charge dynamics, especially in photocatalysis. The efficiency of these hot carrier injections relies on robust metal–semiconductor interfaces, with performance heavily influenced by the composition, crystallinity, and atomic structure of the multi-interfaces involved. This letter explores the mechanisms of LSPR-induced hot carrier injection, highlighting recent advances with emphasis on multi-interfacial engineering to optimize charge dynamics and utilization. These interface-regulated hot carrier processes, combined with enhanced photocatalytic performance, provide new opportunities for further advanced photocatalysis and a wide range of photoelectric conversion applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"26 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477669","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 : 2025-02-22DOI: 10.1021/acsenergylett.5c00004
Se Hwan Park, Abhinand Ayyaswamy, Jonathan Gjerde, W. Beck Andrews, Bairav S. Vishnugopi, Michael Drakopoulos, Nghia T. Vo, Zhong Zhong, Katsuyo Thornton, Partha P. Mukherjee, Kelsey B. Hatzell
Lithium-reservoir-free solid-state batteries can fail due to electrical shorting as a result of fracture and lithium metal filament formation. Mechanical stress at the solid electrolyte surface can induce fractures, which promote lithium filament growth. This stress arises from both electrochemical sources, due to lithium electrodeposition, and mechanical sources, such as external stack pressure. Solid electrolyte surface roughness and the applied stack pressure together affect stress development. This study combines electrochemical experiments, 3D synchrotron imaging, and mesoscale modeling to explore how stack pressure influences failure mechanisms in lithium free solid-state batteries. At low stack pressure, irregular lithium plating and the resulting high local current density drive failure. At higher stack pressure, uniform lithium plating is favored; however, notch-like features in the surface of the solid electrolyte experience high tensile stress, leading to fractures that cause premature short-circuiting.
{"title":"Filament-Induced Failure in Lithium-Reservoir-Free Solid-State Batteries","authors":"Se Hwan Park, Abhinand Ayyaswamy, Jonathan Gjerde, W. Beck Andrews, Bairav S. Vishnugopi, Michael Drakopoulos, Nghia T. Vo, Zhong Zhong, Katsuyo Thornton, Partha P. Mukherjee, Kelsey B. Hatzell","doi":"10.1021/acsenergylett.5c00004","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00004","url":null,"abstract":"Lithium-reservoir-free solid-state batteries can fail due to electrical shorting as a result of fracture and lithium metal filament formation. Mechanical stress at the solid electrolyte surface can induce fractures, which promote lithium filament growth. This stress arises from both electrochemical sources, due to lithium electrodeposition, and mechanical sources, such as external stack pressure. Solid electrolyte surface roughness and the applied stack pressure together affect stress development. This study combines electrochemical experiments, 3D synchrotron imaging, and mesoscale modeling to explore how stack pressure influences failure mechanisms in lithium free solid-state batteries. At low stack pressure, irregular lithium plating and the resulting high local current density drive failure. At higher stack pressure, uniform lithium plating is favored; however, notch-like features in the surface of the solid electrolyte experience high tensile stress, leading to fractures that cause premature short-circuiting.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470448","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 : 2025-02-21DOI: 10.1021/acsenergylett.5c00078
Xiaochen Yang, Yu Chen, Grace Wei, Mouhamad Said Diallo, Maxim Avdeev, Han-Ming Hau, Hao Qiu, Huiwen Ji, Gerbrand Ceder
Halides are promising solid-state electrolytes for all-solid-state lithium batteries due to their exceptional oxidation stability, high Li-ion conductivity, and mechanical deformability. However, their practicality is limited by the reliance on rare and expensive metals. This study investigates the Li2MgCl4 inverse spinel system as a cost-effective alternative. Molecular dynamics simulations reveal that lithium disordering at elevated temperatures significantly reduces the activation energy in Li2MgCl4. To stabilize this disorder at lower temperatures, we experimentally explored the LixZr1–x/2Mgx/2Cl4 system and found that Zr doping induces both Zr and Li disorder at the 16c site at room temperature (RT). This leads to a 2 order-of-magnitude increase in ionic conductivity for the Li1.25Zr0.375Mg0.625Cl4 composition, achieving 1.4 × 10–5 S cm–1 at RT, compared to pristine Li2MgCl4. By deconvoluting the role of lithium vacancies and dopants, we reveal that cation disordering to the 16c site predominantly enhances ionic conductivity, whereas lithium vacancy concentration has a very limited effect.
{"title":"Harnessing Cation Disorder for Enhancing Ionic Conductivity in Lithium Inverse Spinel Halides","authors":"Xiaochen Yang, Yu Chen, Grace Wei, Mouhamad Said Diallo, Maxim Avdeev, Han-Ming Hau, Hao Qiu, Huiwen Ji, Gerbrand Ceder","doi":"10.1021/acsenergylett.5c00078","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00078","url":null,"abstract":"Halides are promising solid-state electrolytes for all-solid-state lithium batteries due to their exceptional oxidation stability, high Li-ion conductivity, and mechanical deformability. However, their practicality is limited by the reliance on rare and expensive metals. This study investigates the Li<sub>2</sub>MgCl<sub>4</sub> inverse spinel system as a cost-effective alternative. Molecular dynamics simulations reveal that lithium disordering at elevated temperatures significantly reduces the activation energy in Li<sub>2</sub>MgCl<sub>4</sub>. To stabilize this disorder at lower temperatures, we experimentally explored the Li<sub><i>x</i></sub>Zr<sub>1–<i>x</i>/2</sub>Mg<sub><i>x</i>/2</sub>Cl<sub>4</sub> system and found that Zr doping induces both Zr and Li disorder at the 16c site at room temperature (RT). This leads to a 2 order-of-magnitude increase in ionic conductivity for the Li<sub>1.25</sub>Zr<sub>0.375</sub>Mg<sub>0.625</sub>Cl<sub>4</sub> composition, achieving 1.4 × 10<sup>–5</sup> S cm<sup>–1</sup> at RT, compared to pristine Li<sub>2</sub>MgCl<sub>4</sub>. By deconvoluting the role of lithium vacancies and dopants, we reveal that cation disordering to the 16c site predominantly enhances ionic conductivity, whereas lithium vacancy concentration has a very limited effect.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"20 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470451","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 : 2025-02-20DOI: 10.1021/acsenergylett.4c02285
David Garcia Romero, Lorenzo Di Mario, Maria Antonietta Loi
Organic solar cells (OSCs) are one of the most promising emerging photovoltaic technologies due to the rapid increase in efficiency in recent years. While efficiencies over 20% have been reported in laboratory scale devices using the conventional (p-i-n) structure, OSCs with inverted (n-i-p) structures still underperform, reaching values around 18%. Tin oxide (SnO2) has recently emerged as a promising transport layer for OSCs. Yet, some reproducibility challenges shown by the literature have hindered the full adaptation of this electron transport layer (ETL) by the organic solar cell community. This Perspective evaluates the current status of investigation for SnO2 as the transport layer for OSCs, focusing on its integration into state-of-the-art systems and highlighting the challenges toward its implementation. We examine which strategies lead to the most efficient and stable devices using SnO2 and give a critical view of whether this material can soon become the next benchmark electron transport layer for OSCs.
{"title":"Tin Oxide: The Next Benchmark Transport Material for Organic Solar Cells?","authors":"David Garcia Romero, Lorenzo Di Mario, Maria Antonietta Loi","doi":"10.1021/acsenergylett.4c02285","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02285","url":null,"abstract":"Organic solar cells (OSCs) are one of the most promising emerging photovoltaic technologies due to the rapid increase in efficiency in recent years. While efficiencies over 20% have been reported in laboratory scale devices using the conventional (p-i-n) structure, OSCs with inverted (n-i-p) structures still underperform, reaching values around 18%. Tin oxide (SnO<sub>2</sub>) has recently emerged as a promising transport layer for OSCs. Yet, some reproducibility challenges shown by the literature have hindered the full adaptation of this electron transport layer (ETL) by the organic solar cell community. This Perspective evaluates the current status of investigation for SnO<sub>2</sub> as the transport layer for OSCs, focusing on its integration into state-of-the-art systems and highlighting the challenges toward its implementation. We examine which strategies lead to the most efficient and stable devices using SnO<sub>2</sub> and give a critical view of whether this material can soon become the next benchmark electron transport layer for OSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"6 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462344","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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