Pub Date : 2026-01-26DOI: 10.1021/acsenergylett.5c04072
Seung-Joo Chang, Seong Chan Cho, Seong-Ho Cho, Sang-Uk Lee, Minh Anh Truong, Sang Uck Lee, Atsushi Wakamiya, Nam-Gyu Park
Although carbazole-based hole-collecting monolayers (HCMs) have been widely employed for achieving high-efficiency inverted perovskite solar cells (PSCs), enhancing their film uniformity remains a critical challenge. Here, we report the use of Hammett constant (σp)-engineered benzoic acid derivatives to improve the conformal coating of the tripodal triazatruxene-based 3PATAT-C3 HCM. Benzoic acid derivatives with positive σp values enhanced the power conversion efficiency (PCE), whereas those with negative σp values reduced device performance. Among the tested derivatives, 4-acetylbenzoic acid (4-AcBA), bearing an electron-withdrawing substituent that imparts a positive σp, promoted improved conformality and a favorable work function for efficient hole extraction. In contrast, 4-aminobenzoic acid (4-ABA), with an electron-donating substituent corresponding to a negative σp, led to poor conformality and an unfavorable work function. Furthermore, compared to 4-ABA, the incorporation of 4-AcBA strengthened the binding of both HCMs and the additive itself to the fluorine-doped tin oxide (FTO) surface. As a result, engineering the 3PATAT-C3 HCM with 4-AcBA increased the PCE from 23.55% to 24.43%, while also significantly enhancing operational stability compared with the untreated control device.
{"title":"Tuning Hole-Collecting Monolayers with Hammett Constant-Engineered Benzoic Acid Derivatives for Inverted Perovskite Solar Cells","authors":"Seung-Joo Chang, Seong Chan Cho, Seong-Ho Cho, Sang-Uk Lee, Minh Anh Truong, Sang Uck Lee, Atsushi Wakamiya, Nam-Gyu Park","doi":"10.1021/acsenergylett.5c04072","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04072","url":null,"abstract":"Although carbazole-based hole-collecting monolayers (HCMs) have been widely employed for achieving high-efficiency inverted perovskite solar cells (PSCs), enhancing their film uniformity remains a critical challenge. Here, we report the use of Hammett constant (σ<sub>p</sub>)-engineered benzoic acid derivatives to improve the conformal coating of the tripodal triazatruxene-based 3PATAT-C3 HCM. Benzoic acid derivatives with positive σ<sub>p</sub> values enhanced the power conversion efficiency (PCE), whereas those with negative σ<sub>p</sub> values reduced device performance. Among the tested derivatives, 4-acetylbenzoic acid (4-AcBA), bearing an electron-withdrawing substituent that imparts a positive σ<sub>p</sub>, promoted improved conformality and a favorable work function for efficient hole extraction. In contrast, 4-aminobenzoic acid (4-ABA), with an electron-donating substituent corresponding to a negative σ<sub>p</sub>, led to poor conformality and an unfavorable work function. Furthermore, compared to 4-ABA, the incorporation of 4-AcBA strengthened the binding of both HCMs and the additive itself to the fluorine-doped tin oxide (FTO) surface. As a result, engineering the 3PATAT-C3 HCM with 4-AcBA increased the PCE from 23.55% to 24.43%, while also significantly enhancing operational stability compared with the untreated control device.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044826","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 : 2026-01-26DOI: 10.1021/acsenergylett.5c02410
Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi,Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi
Despite the rapid increase in efficiency of perovskite photovoltaics, poor reproducibility remains a barrier to their commercialization. Film processing and device performance are highly sensitive to environmental factors during fabrication, yet these interactions are not well understood. Here, we present a systematic methodology to investigate the direct and coupled effects of environmental variables on the perovskite solar cell performance. To do this, we developed an integrated fabrication platform to independently control solvent partial pressure, absolute humidity, and temperature during spin-coating and thermal-annealing of perovskite films and combined it with a closed-loop Bayesian optimization framework to efficiently explore the multidimensional processing space. Efficiency maps reveal coupled nonlinear effects of these variables on device performance, validated by in situ structural characterization, which showed that humidity–solvent interactions affect film crystallization. To overcome the limitations of conventional SHapley Additive exPlanations in disentangling strongly coupled variables, we distilled the knowledge of a Gaussian teacher regressor into multiple student models within an interpretable machine learning framework that employs Shapley interaction analysis to decipher these coupled interactions. This study demonstrates active learning with interpretable machine learning as a powerful tool to explore complex processing landscapes and highlights the importance of environmental control for robust and generalizable processing protocols to accelerate scalable, high-performance, and reproducible perovskite solar cell manufacturing.
{"title":"Disentangling Environmental Effects on Perovskite Solar Cell Performance via Interpretable Machine Learning","authors":"Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi,Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi","doi":"10.1021/acsenergylett.5c02410","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c02410","url":null,"abstract":"Despite the rapid increase in efficiency of perovskite photovoltaics, poor reproducibility remains a barrier to their commercialization. Film processing and device performance are highly sensitive to environmental factors during fabrication, yet these interactions are not well understood. Here, we present a systematic methodology to investigate the direct and coupled effects of environmental variables on the perovskite solar cell performance. To do this, we developed an integrated fabrication platform to independently control solvent partial pressure, absolute humidity, and temperature during spin-coating and thermal-annealing of perovskite films and combined it with a closed-loop Bayesian optimization framework to efficiently explore the multidimensional processing space. Efficiency maps reveal coupled nonlinear effects of these variables on device performance, validated by in situ structural characterization, which showed that humidity–solvent interactions affect film crystallization. To overcome the limitations of conventional SHapley Additive exPlanations in disentangling strongly coupled variables, we distilled the knowledge of a Gaussian teacher regressor into multiple student models within an interpretable machine learning framework that employs Shapley interaction analysis to decipher these coupled interactions. This study demonstrates active learning with interpretable machine learning as a powerful tool to explore complex processing landscapes and highlights the importance of environmental control for robust and generalizable processing protocols to accelerate scalable, high-performance, and reproducible perovskite solar cell manufacturing.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"31 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044952","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 : 2026-01-26DOI: 10.1021/acsenergylett.5c03191
Abasi Abudulimu,Xiaoming Wang,Tyler Brau,Jaroslav Kuliček,Scott L. Wenner,Adam B. Phillips,Ebin Bastola,Manoj K. Jamarkattel,Vijay C. Karade,Kiran Lamichhane,Aparajita Dixit,Bohuslav Rezek,Yanfa Yan,Michael J. Heben,Randy J. Ellingson
Defect recombination limits wide-gap Se-based chalcogenide devices, yet how chloride activation reshapes radiative pathways remains unclear. Here we show that a 40 min CdCl2 anneal converts evaporated CdSe from porous nanograins into dense micrometer-scale polycrystals and sharpens the optical band edge, reducing the Urbach energy from 85 to 17 meV at 300 K. Combining temperature- and fluence-dependent photoluminescence (PL), time-resolved PL, hyperspectral mapping, and hybrid-DFT, we resolve three emissive channels and identify their mechanisms. The near-edge band is excitonic at low temperature and evolves into free-carrier emission at elevated temperature. A sub-gap band at Eg −0.45 eV requires above-gap carriers and thermally quenches with a 0.16 eV activation energy. A broad ∼1.05 eV infrared band is excited by above- and below-gap photons and retains microsecond lifetimes at room temperature; patial mapping links it to edge-rich microstructure. Calculations suggest selenium-vacancy and cadmium-vacancy–chlorine complexes, pointing to routes to suppress defect-related losses in wide-gap chalcogenide devices.
{"title":"Radiative Defects in Chloride-Activated CdSe Thin Films","authors":"Abasi Abudulimu,Xiaoming Wang,Tyler Brau,Jaroslav Kuliček,Scott L. Wenner,Adam B. Phillips,Ebin Bastola,Manoj K. Jamarkattel,Vijay C. Karade,Kiran Lamichhane,Aparajita Dixit,Bohuslav Rezek,Yanfa Yan,Michael J. Heben,Randy J. Ellingson","doi":"10.1021/acsenergylett.5c03191","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03191","url":null,"abstract":"Defect recombination limits wide-gap Se-based chalcogenide devices, yet how chloride activation reshapes radiative pathways remains unclear. Here we show that a 40 min CdCl2 anneal converts evaporated CdSe from porous nanograins into dense micrometer-scale polycrystals and sharpens the optical band edge, reducing the Urbach energy from 85 to 17 meV at 300 K. Combining temperature- and fluence-dependent photoluminescence (PL), time-resolved PL, hyperspectral mapping, and hybrid-DFT, we resolve three emissive channels and identify their mechanisms. The near-edge band is excitonic at low temperature and evolves into free-carrier emission at elevated temperature. A sub-gap band at Eg −0.45 eV requires above-gap carriers and thermally quenches with a 0.16 eV activation energy. A broad ∼1.05 eV infrared band is excited by above- and below-gap photons and retains microsecond lifetimes at room temperature; patial mapping links it to edge-rich microstructure. Calculations suggest selenium-vacancy and cadmium-vacancy–chlorine complexes, pointing to routes to suppress defect-related losses in wide-gap chalcogenide devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"57 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044954","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 light emitting diodes (PeLEDs) are highly promising for next-generation displays owing to their exceptional emissive properties. However, their complex fabrication, often relying on interleaved solution processing and vacuum deposition, hinders scalable mass production. Here, we present a strategy for high-performance, all-vacuum-deposited PeLEDs. By incorporating vacuum-sublimed nitrogen-containing additives, guanidinium bromide, we effectively suppress intrinsic bulk defects in perovskite films and mitigate nonradiative recombination. Furthermore, an ultrathin, vacuum-deposited alkali metal halide top layer is introduced to heal the defective interface by compensating for the loss of bromide during thermal evaporation and improving crystallinity. Integrating these advanced perovskite films with vacuum-sublimed organic transporting layers resulted in PeLEDs demonstrating a maximum luminance exceeding 164,000 cd/m2 and external quantum efficiencies (EQEs) of 14.83%. Our EQE approaches the current vacuum-device record, while the luminance represents a more than 5-fold improvement over most of the previously reported all-vacuum-deposited devices, highlighting a significant leap toward industrially viable PeLED displays.
{"title":"Efficient and Bright All-Vacuum-Deposited Perovskite Light Emitting Diode via Guanidinium Doping and an Ultrathin Lithium Bromide Interfacial Layer","authors":"Yu-Jer Wu, Cheng-Yueh Chen, Yung-Tang Chuang, Hao-Cheng Lin, Pei-En Jan, Hung-Ming Chen, Ping-Hsun Tsai, Chun-Hao Li, Bo-Han Chen, Kai Chen, Shang-Da Yang, Jin-Wei Lu, Ming-Yen Lu, Ken-Tsung Wong, Hao-Wu Lin","doi":"10.1021/acsenergylett.5c03740","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03740","url":null,"abstract":"Perovskite light emitting diodes (PeLEDs) are highly promising for next-generation displays owing to their exceptional emissive properties. However, their complex fabrication, often relying on interleaved solution processing and vacuum deposition, hinders scalable mass production. Here, we present a strategy for high-performance, all-vacuum-deposited PeLEDs. By incorporating vacuum-sublimed nitrogen-containing additives, guanidinium bromide, we effectively suppress intrinsic bulk defects in perovskite films and mitigate nonradiative recombination. Furthermore, an ultrathin, vacuum-deposited alkali metal halide top layer is introduced to heal the defective interface by compensating for the loss of bromide during thermal evaporation and improving crystallinity. Integrating these advanced perovskite films with vacuum-sublimed organic transporting layers resulted in PeLEDs demonstrating a maximum luminance exceeding 164,000 cd/m<sup>2</sup> and external quantum efficiencies (EQEs) of 14.83%. Our EQE approaches the current vacuum-device record, while the luminance represents a more than 5-fold improvement over most of the previously reported all-vacuum-deposited devices, highlighting a significant leap toward industrially viable PeLED displays.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"16 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044825","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 incorporation of self-polymerizable additives is an effective strategy to improve both efficiency and stability of perovskite solar cells (PSCs), yet the structure-performance relationship remains unclear. Here, two self-polymerizable additives, 2,2,3,3,3-pentafluoropropyl acrylate (PFPA) and n-propyl acrylate (NPA), are systematically investigated. Both additives undergo in situ thermal polymerization during perovskite annealing. The fluorinated PFPA exhibits strong interactions with undercoordinated Pb2+, enabling effective crystallization regulation and defect passivation. Polymerized PFPA preferentially accumulates at the perovskite top surface, forming a hydrophobic dipole layer that enhances charge extraction and interfacial stability. As a result, PSCs with polymerized PFPA achieve a champion power conversion efficiency (PCE) of 26.01% and retain 90.0% of the initial efficiency after 840 h at 85 °C in nitrogen and 95.1% after 1000 h under maximum power point tracking conditions. Furthermore, minimodules with an active area of 14 cm2 deliver a PCE of 21.66%.
{"title":"Multifunctional Fluorinated Self-Polymerizable Additive Improves the Performance of Perovskite Photovoltaics","authors":"Na Shi,Hao Tian,Guangyue Yang,Panyu Wang,Yu Lei,Wei Li,Jingfu Jiang,Xiaoqing Jiang,Zhongjin Shen,Marina Freitag,Xin Guo,Shuping Pang,Na Shi,Hao Tian,Guangyue Yang,Panyu Wang,Yu Lei,Wei Li,Jingfu Jiang,Xiaoqing Jiang,Zhongjin Shen,Marina Freitag,Xin Guo,Shuping Pang","doi":"10.1021/acsenergylett.5c03901","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03901","url":null,"abstract":"The incorporation of self-polymerizable additives is an effective strategy to improve both efficiency and stability of perovskite solar cells (PSCs), yet the structure-performance relationship remains unclear. Here, two self-polymerizable additives, 2,2,3,3,3-pentafluoropropyl acrylate (PFPA) and n-propyl acrylate (NPA), are systematically investigated. Both additives undergo in situ thermal polymerization during perovskite annealing. The fluorinated PFPA exhibits strong interactions with undercoordinated Pb2+, enabling effective crystallization regulation and defect passivation. Polymerized PFPA preferentially accumulates at the perovskite top surface, forming a hydrophobic dipole layer that enhances charge extraction and interfacial stability. As a result, PSCs with polymerized PFPA achieve a champion power conversion efficiency (PCE) of 26.01% and retain 90.0% of the initial efficiency after 840 h at 85 °C in nitrogen and 95.1% after 1000 h under maximum power point tracking conditions. Furthermore, minimodules with an active area of 14 cm2 deliver a PCE of 21.66%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"87 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044949","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 : 2026-01-26DOI: 10.1021/acsenergylett.5c02410
Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi,Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi
Despite the rapid increase in efficiency of perovskite photovoltaics, poor reproducibility remains a barrier to their commercialization. Film processing and device performance are highly sensitive to environmental factors during fabrication, yet these interactions are not well understood. Here, we present a systematic methodology to investigate the direct and coupled effects of environmental variables on the perovskite solar cell performance. To do this, we developed an integrated fabrication platform to independently control solvent partial pressure, absolute humidity, and temperature during spin-coating and thermal-annealing of perovskite films and combined it with a closed-loop Bayesian optimization framework to efficiently explore the multidimensional processing space. Efficiency maps reveal coupled nonlinear effects of these variables on device performance, validated by in situ structural characterization, which showed that humidity–solvent interactions affect film crystallization. To overcome the limitations of conventional SHapley Additive exPlanations in disentangling strongly coupled variables, we distilled the knowledge of a Gaussian teacher regressor into multiple student models within an interpretable machine learning framework that employs Shapley interaction analysis to decipher these coupled interactions. This study demonstrates active learning with interpretable machine learning as a powerful tool to explore complex processing landscapes and highlights the importance of environmental control for robust and generalizable processing protocols to accelerate scalable, high-performance, and reproducible perovskite solar cell manufacturing.
{"title":"Disentangling Environmental Effects on Perovskite Solar Cell Performance via Interpretable Machine Learning","authors":"Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi,Tianran Liu,Nicky Evans,Kangyu Ji,Ronaldo Lee,Aaron Zhu,Vinn Nguyen,James Serdy,Elizabeth M. Wall,Yongli Lu,Florian A. Formica,Moungi G. Bawendi,Quinn C. Burlingame,Yueh-Lin Loo,Vladimir Bulović,Tonio Buonassisi","doi":"10.1021/acsenergylett.5c02410","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c02410","url":null,"abstract":"Despite the rapid increase in efficiency of perovskite photovoltaics, poor reproducibility remains a barrier to their commercialization. Film processing and device performance are highly sensitive to environmental factors during fabrication, yet these interactions are not well understood. Here, we present a systematic methodology to investigate the direct and coupled effects of environmental variables on the perovskite solar cell performance. To do this, we developed an integrated fabrication platform to independently control solvent partial pressure, absolute humidity, and temperature during spin-coating and thermal-annealing of perovskite films and combined it with a closed-loop Bayesian optimization framework to efficiently explore the multidimensional processing space. Efficiency maps reveal coupled nonlinear effects of these variables on device performance, validated by in situ structural characterization, which showed that humidity–solvent interactions affect film crystallization. To overcome the limitations of conventional SHapley Additive exPlanations in disentangling strongly coupled variables, we distilled the knowledge of a Gaussian teacher regressor into multiple student models within an interpretable machine learning framework that employs Shapley interaction analysis to decipher these coupled interactions. This study demonstrates active learning with interpretable machine learning as a powerful tool to explore complex processing landscapes and highlights the importance of environmental control for robust and generalizable processing protocols to accelerate scalable, high-performance, and reproducible perovskite solar cell manufacturing.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"117 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044953","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 : 2026-01-26DOI: 10.1021/acsenergylett.5c03653
Xinzhe Xue,Swetha Chandrasekaran,Cheng Zhu,Marcus A. Worsley,Yat Li
Three-dimensional (3D) architectural design has emerged as a powerful strategy to push electrochemical energy storage (EES) devices beyond the intrinsic limitations of conventional two-dimensional (2D) electrodes. While planar architectures enable high packing density and mature manufacturing, they suffer from limited ion transport and low active-material loading. In contrast, 3D architectures introduce low-tortuosity networks and high surface area that enhance charge and mass transport while supporting thick, high mass-loading electrodes. However, their practicality remains hindered by challenges in volumetric density, mechanical stability, and large-scale manufacturability. This Perspective examines the key evaluation and design principles that govern 3D device performance. We discuss the fundamental trade-offs between porosity, volumetric density, and mechanical stability that shape 3D design and highlight emerging strategies for integrating materials engineering, structural optimization, device integration, computational modeling, and scalable manufacturing. By aligning structural functionality with manufacturability, 3D architectures can evolve from laboratory prototypes to commercially viable energy storage systems.
{"title":"Architecting the Third Dimension of Electrochemical Energy Storage","authors":"Xinzhe Xue,Swetha Chandrasekaran,Cheng Zhu,Marcus A. Worsley,Yat Li","doi":"10.1021/acsenergylett.5c03653","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03653","url":null,"abstract":"Three-dimensional (3D) architectural design has emerged as a powerful strategy to push electrochemical energy storage (EES) devices beyond the intrinsic limitations of conventional two-dimensional (2D) electrodes. While planar architectures enable high packing density and mature manufacturing, they suffer from limited ion transport and low active-material loading. In contrast, 3D architectures introduce low-tortuosity networks and high surface area that enhance charge and mass transport while supporting thick, high mass-loading electrodes. However, their practicality remains hindered by challenges in volumetric density, mechanical stability, and large-scale manufacturability. This Perspective examines the key evaluation and design principles that govern 3D device performance. We discuss the fundamental trade-offs between porosity, volumetric density, and mechanical stability that shape 3D design and highlight emerging strategies for integrating materials engineering, structural optimization, device integration, computational modeling, and scalable manufacturing. By aligning structural functionality with manufacturability, 3D architectures can evolve from laboratory prototypes to commercially viable energy storage systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"288 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044956","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 : 2026-01-26DOI: 10.1021/acsenergylett.5c04112
Morgan P. Le Dû, Peter Müller-Buschbaum
Green hydrogen (H2) production from photocatalytic water splitting is not yet scalable, and most green H2 available today is still produced by water electrolysis. One of the main limitations arises from the reaction setup, where photocatalysts must be dispersed in liquid water. Hydrogels offer an alternative platform that acts simultaneously as a water reservoir and a host matrix for photocatalyst dispersion, supplying the water (H2O) required for water splitting while preventing catalyst aggregation. When designed appropriately, catalyst-loaded hydrogels can operate in a self-sustained manner. This Perspective discusses strategies to improve catalyst dispersion and to preserve the swelling behavior that maintains water availability. Polymer networks tailored for long-term water retention can prevent dehydration and sustain H2O feedstock during diurnal hygrometric cycles. Approaches for dark photocatalysis are also considered to enable H2 production during the night. Finally, advanced scattering techniques are highlighted as essential tools to probe the morphology and dynamics that govern the performance of these hydrogel systems.
{"title":"Hydrogels as Functional Media in Photocatalytic Energy Systems: Toward Self-Sustained Green H2 Generation","authors":"Morgan P. Le Dû, Peter Müller-Buschbaum","doi":"10.1021/acsenergylett.5c04112","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04112","url":null,"abstract":"Green hydrogen (H<sub>2</sub>) production from photocatalytic water splitting is not yet scalable, and most green H<sub>2</sub> available today is still produced by water electrolysis. One of the main limitations arises from the reaction setup, where photocatalysts must be dispersed in liquid water. Hydrogels offer an alternative platform that acts simultaneously as a water reservoir and a host matrix for photocatalyst dispersion, supplying the water (H<sub>2</sub>O) required for water splitting while preventing catalyst aggregation. When designed appropriately, catalyst-loaded hydrogels can operate in a self-sustained manner. This Perspective discusses strategies to improve catalyst dispersion and to preserve the swelling behavior that maintains water availability. Polymer networks tailored for long-term water retention can prevent dehydration and sustain H<sub>2</sub>O feedstock during diurnal hygrometric cycles. Approaches for dark photocatalysis are also considered to enable H<sub>2</sub> production during the night. Finally, advanced scattering techniques are highlighted as essential tools to probe the morphology and dynamics that govern the performance of these hydrogel systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146044827","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 : 2026-01-24DOI: 10.1021/acsenergylett.5c03711
Haobin Song, Yang-Feng Cui, Yue Wang, Nan Zhao, Wenjing Li, Cong Huang, Hui Ying Yang
Aqueous zinc-ion batteries (AZIBs) have gained increasing attention as next-generation energy storage systems owing to their intrinsic safety, environmental benignity, and low cost. Nevertheless, zinc dendrite growth and surface corrosion at the anode, together with sluggish ion transport and structural degradation at the cathode, hinder practical deployment. Crystalline materials have been extensively employed as anode coatings to suppress dendrite formation or as cathode materials to achieve high capacity, yet their inherent rigidity often causes cracking and delamination under interfacial stress, while narrow diffusion channels constrain Zn2+ transport. In contrast, amorphous materials, characterized by short-range order and mechanical flexibility, provide isotropic ion pathways that enable uniform Zn2+ flux and inhibit dendrite nucleation. Their compliant bonding networks accommodate volume variation and promote stable interphase formation. Despite their promise, a comprehensive assessment of amorphous materials for AZIBs remains lacking. This review summarizes recent progress and emerging opportunities in amorphous design strategies for AZIBs.
{"title":"Recent Advances in Amorphous Electrode Materials for Aqueous Zinc-Ion Batteries","authors":"Haobin Song, Yang-Feng Cui, Yue Wang, Nan Zhao, Wenjing Li, Cong Huang, Hui Ying Yang","doi":"10.1021/acsenergylett.5c03711","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03711","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) have gained increasing attention as next-generation energy storage systems owing to their intrinsic safety, environmental benignity, and low cost. Nevertheless, zinc dendrite growth and surface corrosion at the anode, together with sluggish ion transport and structural degradation at the cathode, hinder practical deployment. Crystalline materials have been extensively employed as anode coatings to suppress dendrite formation or as cathode materials to achieve high capacity, yet their inherent rigidity often causes cracking and delamination under interfacial stress, while narrow diffusion channels constrain Zn<sup>2+</sup> transport. In contrast, amorphous materials, characterized by short-range order and mechanical flexibility, provide isotropic ion pathways that enable uniform Zn<sup>2+</sup> flux and inhibit dendrite nucleation. Their compliant bonding networks accommodate volume variation and promote stable interphase formation. Despite their promise, a comprehensive assessment of amorphous materials for AZIBs remains lacking. This review summarizes recent progress and emerging opportunities in amorphous design strategies for AZIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"31 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034213","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 : 2026-01-23DOI: 10.1021/acsenergylett.5c03494
Qiu He, Jiangyuan Xing, Xingyu Chen, Fei Wang, Yan Zhao
The increasing global demand for renewable, high-energy-density energy storage systems has revitalized interest in lithium–metal-based batteries (LMBs) as a viable alternative to conventional graphite-based Li-ion batteries. Electrolyte engineering has emerged as a promising approach to mitigate the persistent issue of Li dendrite formation, which is a critical barrier to the practical implementation of LMBs. This strategy aims to optimize the dynamic solvation structure and regulate ion transport via orchestrating the composition of the electrolyte and the distribution of constituents within the electrode–electrolyte interphase layer. This review focuses on the achievements of aprotic liquid electrolytes over the past five years, particularly in the context of LMBs with high-nickel layered oxide-based and sulfur-based cathodes, emphasizing high-concentration electrolytes and their localized variants, electrolyte additives, and novel electrolyte systems. The design principles, operating mechanisms, and performance trade-offs of leading electrolyte strategies are presented, culminating in insights and future prospects for practical LMBs.
{"title":"Electrolyte-Induced Interphase Programming for Aprotic High-Energy Lithium Metal Batteries","authors":"Qiu He, Jiangyuan Xing, Xingyu Chen, Fei Wang, Yan Zhao","doi":"10.1021/acsenergylett.5c03494","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03494","url":null,"abstract":"The increasing global demand for renewable, high-energy-density energy storage systems has revitalized interest in lithium–metal-based batteries (LMBs) as a viable alternative to conventional graphite-based Li-ion batteries. Electrolyte engineering has emerged as a promising approach to mitigate the persistent issue of Li dendrite formation, which is a critical barrier to the practical implementation of LMBs. This strategy aims to optimize the dynamic solvation structure and regulate ion transport via orchestrating the composition of the electrolyte and the distribution of constituents within the electrode–electrolyte interphase layer. This review focuses on the achievements of aprotic liquid electrolytes over the past five years, particularly in the context of LMBs with high-nickel layered oxide-based and sulfur-based cathodes, emphasizing high-concentration electrolytes and their localized variants, electrolyte additives, and novel electrolyte systems. The design principles, operating mechanisms, and performance trade-offs of leading electrolyte strategies are presented, culminating in insights and future prospects for practical LMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"142 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034188","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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