Pub Date : 2026-01-23DOI: 10.1021/acsenergylett.5c03923
Hyeonseong Oh, Uigyeong Jeong, Junhyeok Choi, Jaejin Lim, Jun Tae Kim, Hyeon-Ji Shin, Jong-yeon Im, Hyun-Woo Gong, Jae-Pyoung Ahn, Yong Min Lee, Jongsoon Kim, Junyoung Mun, Kyung Yoon Chung, Si Hyoung Oh, Jong-Won Lee, Sang-Young Lee, Hun-Gi Jung
All-solid-state batteries employing sulfide solid electrolytes promise high energy density and safety but suffer from poor cycling stability and rate performance due to fundamental shortcomings in composite electrode architectures. To address challenges, this study introduces bimodal composite cathodes formed by blending large polycrystalline and small single-crystalline cathode active materials (CAMs). This bimodal configuration optimizes particle packing and porosity, thereby reducing ionic tortuosity and enhancing Li+ transport. At an extreme CAM loading of 90 wt%, a bimodal composition with a 7:3 mass ratio of polycrystalline to single-crystalline CAM exhibited enhanced rate performance and 87.8% capacity retention after 200 cycles, outperforming unimodal composite cathodes. Distribution-of-relaxation-times analysis, operando X-ray diffraction, operando electrochemical pressiometry, and three-dimensional simulations revealed that the enhanced mechanical performance of densely packed electrode structures originates not from stress relaxation but from uniform stress dispersion. These findings establish a comprehensive framework for advancing the design and optimization of complex composite cathodes.
{"title":"Bimodal Composite Cathodes Advancing the Chemo-Mechanical Integrity and Kinetics for All-Solid-State Batteries","authors":"Hyeonseong Oh, Uigyeong Jeong, Junhyeok Choi, Jaejin Lim, Jun Tae Kim, Hyeon-Ji Shin, Jong-yeon Im, Hyun-Woo Gong, Jae-Pyoung Ahn, Yong Min Lee, Jongsoon Kim, Junyoung Mun, Kyung Yoon Chung, Si Hyoung Oh, Jong-Won Lee, Sang-Young Lee, Hun-Gi Jung","doi":"10.1021/acsenergylett.5c03923","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03923","url":null,"abstract":"All-solid-state batteries employing sulfide solid electrolytes promise high energy density and safety but suffer from poor cycling stability and rate performance due to fundamental shortcomings in composite electrode architectures. To address challenges, this study introduces bimodal composite cathodes formed by blending large polycrystalline and small single-crystalline cathode active materials (CAMs). This bimodal configuration optimizes particle packing and porosity, thereby reducing ionic tortuosity and enhancing Li<sup>+</sup> transport. At an extreme CAM loading of 90 wt%, a bimodal composition with a 7:3 mass ratio of polycrystalline to single-crystalline CAM exhibited enhanced rate performance and 87.8% capacity retention after 200 cycles, outperforming unimodal composite cathodes. Distribution-of-relaxation-times analysis, operando X-ray diffraction, operando electrochemical pressiometry, and three-dimensional simulations revealed that the enhanced mechanical performance of densely packed electrode structures originates not from stress relaxation but from uniform stress dispersion. These findings establish a comprehensive framework for advancing the design and optimization of complex composite cathodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"25 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034215","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.5c04057
Pradeep R. Nair
Ultra-low-voltage operation of perovskite light emitting diodes (PeLEDs) was demonstrated in recent years. However, the light output at such conditions from PeLEDs is usually very low, and the maximum external quantum efficiency (EQE) and power conversion efficiency (PCE) are typically achieved at large biases with significant power consumption. Here, we explore the possibility of achieving maxima in EQE and PCE at sub-band-gap voltages for PeLEDs. Our analysis consistently interprets otherwise scattered experimental data from the literature, identifies the limits for low-voltage operation, and elucidates optimization routes for sub-band gap high-radiance operation of PeLEDs.
{"title":"Can Perovskite Light Emitting Diodes Achieve Maximum Efficiency at Sub-Band-Gap Voltages?","authors":"Pradeep R. Nair","doi":"10.1021/acsenergylett.5c04057","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04057","url":null,"abstract":"Ultra-low-voltage operation of perovskite light emitting diodes (PeLEDs) was demonstrated in recent years. However, the light output at such conditions from PeLEDs is usually very low, and the maximum external quantum efficiency (EQE) and power conversion efficiency (PCE) are typically achieved at large biases with significant power consumption. Here, we explore the possibility of achieving maxima in EQE and PCE at sub-band-gap voltages for PeLEDs. Our analysis consistently interprets otherwise scattered experimental data from the literature, identifies the limits for low-voltage operation, and elucidates optimization routes for sub-band gap high-radiance operation of PeLEDs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034155","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 stability of Sn–Pb perovskite semiconductors thin films remains a major challenge for their integration into efficient and durable photovoltaic devices. In this work, we demonstrate that the incorporation of methylammonium chloride (MACl) in DMSO-free Sn–Pb precursor solutions significantly enhances both the structural and operational stability of Sn–Pb perovskite films and solar cells. MACl-processed films exhibit enhanced crystallinity, environmental stability and photostability, thus tackling the most critical instabilities related to the defect chemistry of tin in tin-based perovskites and halides in lead-based perovskites. We show that Cl– preferentially resides at the Pb0.5Sn0.5I-terminated surface, reducing the formation probability of halide interstitials, preventing I2 loss under illumination and reducing O2 uptake under ambient air exposition. As a result, solar cells incorporating MACl-treated films maintain stable performance under maximum power point tracking for over 900 h. This work highlights the crucial role of interfaces and paves the way for more durable perovskite solar cells.
{"title":"DMSO-Free Processing of Tin–Lead Perovskite Thin Films for Solar Cells with Enhanced Stability","authors":"Isabella Poli, Mirko Prato, Hui Li, Cecilia D. Costa, Luca Gregori, Daniele Meggiolaro, Tristan Quinson, Angelica Chiodoni, Filippo De Angelis, Annamaria Petrozza","doi":"10.1021/acsenergylett.5c03416","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03416","url":null,"abstract":"The stability of Sn–Pb perovskite semiconductors thin films remains a major challenge for their integration into efficient and durable photovoltaic devices. In this work, we demonstrate that the incorporation of methylammonium chloride (MACl) in DMSO-free Sn–Pb precursor solutions significantly enhances both the structural and operational stability of Sn–Pb perovskite films and solar cells. MACl-processed films exhibit enhanced crystallinity, environmental stability and photostability, thus tackling the most critical instabilities related to the defect chemistry of tin in tin-based perovskites and halides in lead-based perovskites. We show that Cl<sup>–</sup> preferentially resides at the Pb<sub>0.5</sub>Sn<sub>0.5</sub>I-terminated surface, reducing the formation probability of halide interstitials, preventing I<sub>2</sub> loss under illumination and reducing O<sub>2</sub> uptake under ambient air exposition. As a result, solar cells incorporating MACl-treated films maintain stable performance under maximum power point tracking for over 900 h. This work highlights the crucial role of interfaces and paves the way for more durable perovskite solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"50 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034214","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-rich oxides (LROs) offer theoretical energy densities exceeding 1000 Wh kg–1. Nonetheless, their poor electron/ion conduction properties, as well as severe structural instability during high-voltage cycling, result in limited capacity and rapid performance degradation. Herein, coherent spinel structure bands are in situ constructed in the LRO matrix by lattice distortion relaxation after initial activation. These bands significantly enhance Li+ and electron transport while mitigating cyclic stress through coherent effects. As a result, the modified LRO delivers a specific capacity of 294 mAh g–1 at 0.1C, with an initial energy density reaching 1049.6 Wh kg–1. Furthermore, it shows a capacity retention of 90.5% after 500 cycles at 1 C. This study demonstrates lattice coherent engineering driven by distortion relaxation as an effective strategy for developing lithium-ion battery cathodes.
富锂氧化物（LROs）的理论能量密度超过1000 Wh kg-1。然而，它们的电子/离子传导性能差，以及在高压循环过程中严重的结构不稳定性，导致容量有限，性能迅速下降。在初始激活后，通过晶格畸变弛豫在LRO基体中原位构建了相干尖晶石结构带。这些条带显著增强了Li+和电子输运，同时通过相干效应减轻了循环应力。因此，改进后的LRO在0.1C时的比容量为294 mAh g-1，初始能量密度达到1049.6 Wh kg-1。此外，在1℃下循环500次后，其容量保持率为90.5%。该研究表明，由畸变松弛驱动的晶格相干工程是开发锂离子电池阴极的有效策略。
{"title":"Lattice-Distortion-Driven In Situ Formation of Coherent Structural Bands Lithium-Rich Oxides as Lithium-Ion Battery Cathodes","authors":"Shengnan He, Rui Zhang, Yufa Zhou, Chenchen Li, Xu Xue, Chao Zheng, Zhijun Wu, Jiantuo Gan, Liaona She, Fulai Qi, Yanxia Liu, Yaxiong Yang, Wubin Du, Yinzhu Jiang, Mingxia Gao, Hongge Pan","doi":"10.1021/acsenergylett.5c03989","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03989","url":null,"abstract":"Lithium-rich oxides (LROs) offer theoretical energy densities exceeding 1000 Wh kg<sup>–1</sup>. Nonetheless, their poor electron/ion conduction properties, as well as severe structural instability during high-voltage cycling, result in limited capacity and rapid performance degradation. Herein, coherent spinel structure bands are <i>in situ</i> constructed in the LRO matrix by lattice distortion relaxation after initial activation. These bands significantly enhance Li<sup>+</sup> and electron transport while mitigating cyclic stress through coherent effects. As a result, the modified LRO delivers a specific capacity of 294 mAh g<sup>–1</sup> at 0.1C, with an initial energy density reaching 1049.6 Wh kg<sup>–1</sup>. Furthermore, it shows a capacity retention of 90.5% after 500 cycles at 1 C. This study demonstrates lattice coherent engineering driven by distortion relaxation as an effective strategy for developing lithium-ion battery cathodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"31 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034216","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 : 2026-01-21DOI: 10.1021/acsenergylett.5c04062
Sarah J. Ghazi,Alexis J. Vincent,Adam J. Abbott,Jeffrey J. Warren
Electrochemical valorization of waste molecules such as carbon dioxide (CO2) is an ongoing challenge. Molecular electrocatalysts, and materials derived from molecular precursors, offer promising strategies for using CO2 as a feedstock. However, consistent methods for benchmarking and comparing catalyst performance are still needed. In particular, frameworks that extract kinetic parameters from cyclic voltammetry data are important. One factor that is unevenly reported in such analyses is internal, or uncompensated, resistance compensation (iR compensation). While recent studies emphasize the importance of iR compensation for solid-state electrocatalysts, its impact on voltammetry-based kinetic analysis of molecular catalysts is less well understood. Here, iron tetraphenylporphyrin-mediated CO2 reduction is used as a model system to examine how iR compensation affects extracted rate constants. We find that rate constants derived from uncompensated voltammetry data can be up to 2-fold smaller than those obtained from compensated data. General recommendations for analyzing voltammetry-derived kinetic data are also discussed.
{"title":"Resistance Is Not Futile: The Role of Internal Resistance in Homogeneous Carbon Dioxide Reduction Mediated by Iron(0) Tetraphenylporphyrin","authors":"Sarah J. Ghazi,Alexis J. Vincent,Adam J. Abbott,Jeffrey J. Warren","doi":"10.1021/acsenergylett.5c04062","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04062","url":null,"abstract":"Electrochemical valorization of waste molecules such as carbon dioxide (CO2) is an ongoing challenge. Molecular electrocatalysts, and materials derived from molecular precursors, offer promising strategies for using CO2 as a feedstock. However, consistent methods for benchmarking and comparing catalyst performance are still needed. In particular, frameworks that extract kinetic parameters from cyclic voltammetry data are important. One factor that is unevenly reported in such analyses is internal, or uncompensated, resistance compensation (iR compensation). While recent studies emphasize the importance of iR compensation for solid-state electrocatalysts, its impact on voltammetry-based kinetic analysis of molecular catalysts is less well understood. Here, iron tetraphenylporphyrin-mediated CO2 reduction is used as a model system to examine how iR compensation affects extracted rate constants. We find that rate constants derived from uncompensated voltammetry data can be up to 2-fold smaller than those obtained from compensated data. General recommendations for analyzing voltammetry-derived kinetic data are also discussed.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"64 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006305","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 : 2026-01-21DOI: 10.1021/acsenergylett.5c04296
Lulu Lyu,Wenqi Fan,Jiadong Shen,Dongjun Lee,Qichen Wang,Jong-woan Chung,Yong-Mook Kang
Aqueous metal–air batteries (AMBs) represent next-generation energy storage technologies due to the intrinsic safety of aqueous electrolytes and environmental benignity. Yet, their practical deployment remains impeded by persistent interfacial instabilities at both electrodes. However, a comprehensive discussion on interface engineering strategies for AMBs is lacking. This review provides a holistic overview of recent progress in interface engineering strategies for both anodes and cathodes in AMBs. We first dissect the interfacial chemistry of metal anodes (Zn, Al, Fe, Mg, and Sn), highlighting degradation pathways in aqueous electrolytes and corresponding mitigation approaches. Next, we examine the mechanistic origins of kinetic bottlenecks at cathodes, analyzing oxygen reduction/evolution reaction pathways and the structure–activity correlations of catalysts. Methods for simultaneously optimizing the anode and cathode interfaces are presented. Finally, a critical outlook on the remaining challenges and future opportunities is given, underscoring the significance of the rational interfacial design for AMBs.
{"title":"Bridging Anode and Cathode Interfaces: Integrated Interfacial Strategies for Aqueous Metal–Air Batteries","authors":"Lulu Lyu,Wenqi Fan,Jiadong Shen,Dongjun Lee,Qichen Wang,Jong-woan Chung,Yong-Mook Kang","doi":"10.1021/acsenergylett.5c04296","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04296","url":null,"abstract":"Aqueous metal–air batteries (AMBs) represent next-generation energy storage technologies due to the intrinsic safety of aqueous electrolytes and environmental benignity. Yet, their practical deployment remains impeded by persistent interfacial instabilities at both electrodes. However, a comprehensive discussion on interface engineering strategies for AMBs is lacking. This review provides a holistic overview of recent progress in interface engineering strategies for both anodes and cathodes in AMBs. We first dissect the interfacial chemistry of metal anodes (Zn, Al, Fe, Mg, and Sn), highlighting degradation pathways in aqueous electrolytes and corresponding mitigation approaches. Next, we examine the mechanistic origins of kinetic bottlenecks at cathodes, analyzing oxygen reduction/evolution reaction pathways and the structure–activity correlations of catalysts. Methods for simultaneously optimizing the anode and cathode interfaces are presented. Finally, a critical outlook on the remaining challenges and future opportunities is given, underscoring the significance of the rational interfacial design for AMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"64 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006307","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 : 2026-01-21DOI: 10.1021/acsenergylett.5c03933
Namji Lee,Derrick Allan Taylor,Donghyun Choi,Dohyun Kwak,Jong-Soo Lee
The precise patterning of quantum dots (QDs) is crucial for integrating advanced optoelectronic devices, including quantum dot light-emitting diodes (QLEDs) and photodetectors. However, conventional patterning techniques often suffer from poor film uniformity and degradation of the optical and electronic properties of QDs. Recently, direct optical lithography has emerged as a powerful alternative, enabling high-resolution patterning while better preserving QD integrity. In this review, we summarize the representative photopatterning mechanisms, including ligand exchange, ligand cross-linking, ligand decomposition, and ligand desorption and discuss the associated material considerations, including QDs, surface ligands, and charge-transport layers. We further highlight recent breakthroughs in applying these strategies to QLEDs and photodetectors. Finally, we outline the remaining challenges – including solubility control, industrial scalability, photodamage mitigation, and the optimization of processing conditions – and propose potential strategies for enhancing patterning quality, device performance, and manufacturability.
{"title":"Advances in Photopatterning of Quantum Dots: Mechanisms, Materials, and Device Applications","authors":"Namji Lee,Derrick Allan Taylor,Donghyun Choi,Dohyun Kwak,Jong-Soo Lee","doi":"10.1021/acsenergylett.5c03933","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03933","url":null,"abstract":"The precise patterning of quantum dots (QDs) is crucial for integrating advanced optoelectronic devices, including quantum dot light-emitting diodes (QLEDs) and photodetectors. However, conventional patterning techniques often suffer from poor film uniformity and degradation of the optical and electronic properties of QDs. Recently, direct optical lithography has emerged as a powerful alternative, enabling high-resolution patterning while better preserving QD integrity. In this review, we summarize the representative photopatterning mechanisms, including ligand exchange, ligand cross-linking, ligand decomposition, and ligand desorption and discuss the associated material considerations, including QDs, surface ligands, and charge-transport layers. We further highlight recent breakthroughs in applying these strategies to QLEDs and photodetectors. Finally, we outline the remaining challenges – including solubility control, industrial scalability, photodamage mitigation, and the optimization of processing conditions – and propose potential strategies for enhancing patterning quality, device performance, and manufacturability.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"50 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006302","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 : 2026-01-21DOI: 10.1021/acsenergylett.5c04062
Sarah J. Ghazi,Alexis J. Vincent,Adam J. Abbott,Jeffrey J. Warren
Electrochemical valorization of waste molecules such as carbon dioxide (CO2) is an ongoing challenge. Molecular electrocatalysts, and materials derived from molecular precursors, offer promising strategies for using CO2 as a feedstock. However, consistent methods for benchmarking and comparing catalyst performance are still needed. In particular, frameworks that extract kinetic parameters from cyclic voltammetry data are important. One factor that is unevenly reported in such analyses is internal, or uncompensated, resistance compensation (iR compensation). While recent studies emphasize the importance of iR compensation for solid-state electrocatalysts, its impact on voltammetry-based kinetic analysis of molecular catalysts is less well understood. Here, iron tetraphenylporphyrin-mediated CO2 reduction is used as a model system to examine how iR compensation affects extracted rate constants. We find that rate constants derived from uncompensated voltammetry data can be up to 2-fold smaller than those obtained from compensated data. General recommendations for analyzing voltammetry-derived kinetic data are also discussed.
{"title":"Resistance Is Not Futile: The Role of Internal Resistance in Homogeneous Carbon Dioxide Reduction Mediated by Iron(0) Tetraphenylporphyrin","authors":"Sarah J. Ghazi,Alexis J. Vincent,Adam J. Abbott,Jeffrey J. Warren","doi":"10.1021/acsenergylett.5c04062","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04062","url":null,"abstract":"Electrochemical valorization of waste molecules such as carbon dioxide (CO2) is an ongoing challenge. Molecular electrocatalysts, and materials derived from molecular precursors, offer promising strategies for using CO2 as a feedstock. However, consistent methods for benchmarking and comparing catalyst performance are still needed. In particular, frameworks that extract kinetic parameters from cyclic voltammetry data are important. One factor that is unevenly reported in such analyses is internal, or uncompensated, resistance compensation (iR compensation). While recent studies emphasize the importance of iR compensation for solid-state electrocatalysts, its impact on voltammetry-based kinetic analysis of molecular catalysts is less well understood. Here, iron tetraphenylporphyrin-mediated CO2 reduction is used as a model system to examine how iR compensation affects extracted rate constants. We find that rate constants derived from uncompensated voltammetry data can be up to 2-fold smaller than those obtained from compensated data. General recommendations for analyzing voltammetry-derived kinetic data are also discussed.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006303","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}
Integrated capture and conversion of low-concentration CO2 is a critical step toward carbon neutrality. Here, we demonstrate a gas diffusion electrode (GDE) modified with oxygen- and nitrogen-functionalized porous graphitic carbon (ONC) that enables efficient electroreduction of dilute CO2. Under 15% CO2 gas (without O2), the ONC-modified GDE achieved a CO2-to-formic acid conversion rate of 250 μmol/h·cm2, 2.5 times higher than that of the bare GDE, with a Faradaic efficiency (FE) of 98%. Even in flue gas containing 8% O2, the modified GDE achieved 22 μmol/h·cm2 formic acid production (8% FE) at −1.4 VRHE. Mechanistic and simulation studies revealed that the oxygen functional groups in ONC enhance CO2 adsorption while suppressing O2 permeation, imparting strong oxygen tolerance. In particular, the ONC-modified GDE remains active at a CO2 concentration as low as 1% and 400 ppm, suggesting potential applicability in integrated capture–conversion systems that utilize dilute CO2 streams from flue gas and ambient air.
{"title":"Integrated Capture and Conversion of Dilute CO2 Using an Oxygen Tolerant Porous Carbon Modified Gas Diffusion Electrode","authors":"Donglai Pan,Jaeyeon Yang,Devthade Vidyasagar,Dayoung Kwon,Ulfi Muliane,Geun Ho Gu,Wooyul Kim,Jeongmin Kim,Myoung Hwan Oh,Wonyong Choi,Donglai Pan,Jaeyeon Yang,Devthade Vidyasagar,Dayoung Kwon,Ulfi Muliane,Geun Ho Gu,Wooyul Kim,Jeongmin Kim,Myoung Hwan Oh,Wonyong Choi","doi":"10.1021/acsenergylett.5c03504","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03504","url":null,"abstract":"Integrated capture and conversion of low-concentration CO2 is a critical step toward carbon neutrality. Here, we demonstrate a gas diffusion electrode (GDE) modified with oxygen- and nitrogen-functionalized porous graphitic carbon (ONC) that enables efficient electroreduction of dilute CO2. Under 15% CO2 gas (without O2), the ONC-modified GDE achieved a CO2-to-formic acid conversion rate of 250 μmol/h·cm2, 2.5 times higher than that of the bare GDE, with a Faradaic efficiency (FE) of 98%. Even in flue gas containing 8% O2, the modified GDE achieved 22 μmol/h·cm2 formic acid production (8% FE) at −1.4 VRHE. Mechanistic and simulation studies revealed that the oxygen functional groups in ONC enhance CO2 adsorption while suppressing O2 permeation, imparting strong oxygen tolerance. In particular, the ONC-modified GDE remains active at a CO2 concentration as low as 1% and 400 ppm, suggesting potential applicability in integrated capture–conversion systems that utilize dilute CO2 streams from flue gas and ambient air.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"64 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006298","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 : 2026-01-21DOI: 10.1021/acsenergylett.5c03933
Namji Lee,Derrick Allan Taylor,Donghyun Choi,Dohyun Kwak,Jong-Soo Lee,Namji Lee,Derrick Allan Taylor,Donghyun Choi,Dohyun Kwak,Jong-Soo Lee
The precise patterning of quantum dots (QDs) is crucial for integrating advanced optoelectronic devices, including quantum dot light-emitting diodes (QLEDs) and photodetectors. However, conventional patterning techniques often suffer from poor film uniformity and degradation of the optical and electronic properties of QDs. Recently, direct optical lithography has emerged as a powerful alternative, enabling high-resolution patterning while better preserving QD integrity. In this review, we summarize the representative photopatterning mechanisms, including ligand exchange, ligand cross-linking, ligand decomposition, and ligand desorption and discuss the associated material considerations, including QDs, surface ligands, and charge-transport layers. We further highlight recent breakthroughs in applying these strategies to QLEDs and photodetectors. Finally, we outline the remaining challenges – including solubility control, industrial scalability, photodamage mitigation, and the optimization of processing conditions – and propose potential strategies for enhancing patterning quality, device performance, and manufacturability.
{"title":"Advances in Photopatterning of Quantum Dots: Mechanisms, Materials, and Device Applications","authors":"Namji Lee,Derrick Allan Taylor,Donghyun Choi,Dohyun Kwak,Jong-Soo Lee,Namji Lee,Derrick Allan Taylor,Donghyun Choi,Dohyun Kwak,Jong-Soo Lee","doi":"10.1021/acsenergylett.5c03933","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03933","url":null,"abstract":"The precise patterning of quantum dots (QDs) is crucial for integrating advanced optoelectronic devices, including quantum dot light-emitting diodes (QLEDs) and photodetectors. However, conventional patterning techniques often suffer from poor film uniformity and degradation of the optical and electronic properties of QDs. Recently, direct optical lithography has emerged as a powerful alternative, enabling high-resolution patterning while better preserving QD integrity. In this review, we summarize the representative photopatterning mechanisms, including ligand exchange, ligand cross-linking, ligand decomposition, and ligand desorption and discuss the associated material considerations, including QDs, surface ligands, and charge-transport layers. We further highlight recent breakthroughs in applying these strategies to QLEDs and photodetectors. Finally, we outline the remaining challenges – including solubility control, industrial scalability, photodamage mitigation, and the optimization of processing conditions – and propose potential strategies for enhancing patterning quality, device performance, and manufacturability.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"276 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006301","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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