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":"32 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006308","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":"88 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006309","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.5c03404
Lixing Xue, Hongyan Pan, Yuejun Wang, Shu Hong, Qian Lin, Kuo Zhang, Xiangnan Bu, Maohui Bai, Kun Zhang, Bo Hong
Fluorinated solvents and gel electrolytes offer potential for safe sodium-ion batteries (SIBs); yet, conventional acrylate gels show polarity mismatch, poor compatibility, and sluggish Na+ transport. Here, we develop an all-fluorinated gel electrolyte by introducing a low-surface-energy perfluorinated acrylate monomer (PFHEA) into an FEMC/TFPC system. The −C8F17 chains enable polarity matching and uniform gelation, improving wettability, reducing interfacial resistance, and restructuring the Na+ solvation environment. Molecular dynamics and spectroscopic results indicate enhanced contact-ion pair formation and fluorine-rich SEI/CEI layers, boosting transport kinetics, interfacial stability, and thermal tolerance. Consequently, 2.6 Ah NCFM||HC pouch cells retain 88.1% capacity after 2600 cycles at 25 °C─representing 2–3-fold longer lifetimes than previously reported Ah-level Na pouch cells. A 115 Ah pouch cell further exhibits a negligible temperature rise during nail penetration, confirming intrinsic flame retardancy. This PFHEA-based gel provides a feasible route toward safe SIBs.
{"title":"Polarity-Matched Perfluorinated Gel Electrolytes toward Safe Sodium-Ion Batteries","authors":"Lixing Xue, Hongyan Pan, Yuejun Wang, Shu Hong, Qian Lin, Kuo Zhang, Xiangnan Bu, Maohui Bai, Kun Zhang, Bo Hong","doi":"10.1021/acsenergylett.5c03404","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03404","url":null,"abstract":"Fluorinated solvents and gel electrolytes offer potential for safe sodium-ion batteries (SIBs); yet, conventional acrylate gels show polarity mismatch, poor compatibility, and sluggish Na<sup>+</sup> transport. Here, we develop an all-fluorinated gel electrolyte by introducing a low-surface-energy perfluorinated acrylate monomer (PFHEA) into an FEMC/TFPC system. The −C<sub>8</sub>F<sub>17</sub> chains enable polarity matching and uniform gelation, improving wettability, reducing interfacial resistance, and restructuring the Na<sup>+</sup> solvation environment. Molecular dynamics and spectroscopic results indicate enhanced contact-ion pair formation and fluorine-rich SEI/CEI layers, boosting transport kinetics, interfacial stability, and thermal tolerance. Consequently, 2.6 Ah NCFM||HC pouch cells retain 88.1% capacity after 2600 cycles at 25 °C─representing 2–3-fold longer lifetimes than previously reported Ah-level Na pouch cells. A 115 Ah pouch cell further exhibits a negligible temperature rise during nail penetration, confirming intrinsic flame retardancy. This PFHEA-based gel provides a feasible route toward safe SIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"131 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146014740","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","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":"185 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006300","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,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,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":"56 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006304","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":"63 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006306","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":"6 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006310","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 : 2026-01-20DOI: 10.1021/acsenergylett.5c02838
Murillo Henrique de Matos Rodrigues,Josiane A. Sobrinho,Arthur Pignataro Machado,Zeno C. Brandao,Ingrid D. Barcelos,Cilene Labre,Rodrigo Szostak,Ana Flávia Nogueira
Bulky 2D alkylammonium cations in metal halide perovskites offer a route to improve both structural stability and optoelectronic performance. This study systematically explores the incorporation of alkylammonium iodides with different chain lengths─dodecylammonium (C12), hexadecylammonium (C16), and octadecylammonium (C18)─into perovskite films for solar cells. Using spectroscopic and nanoscale characterization techniques, we show that C12 provides the best results: enhanced [111] orientation, reduced nonradiative recombination, uniform cation distribution, and improved vertical conductivity. Nanoscale X-ray diffraction and AFM-based infrared spectroscopy revealed that intermediate chain lengths enable favorable lattice expansion and interfacial passivation without hindering crystal growth. Solar cells based on C12-modified films reached power conversion efficiencies over 20%, surpassing both pristine and longer-chain formulations. These findings demonstrate that tuning alkyl chain length is an effective molecular design strategy to guide perovskite crystallization and improve device performance and stability.
{"title":"Tuning Structure and Performance of 2D/3D Perovskites by Alkyl Chain Length Engineering","authors":"Murillo Henrique de Matos Rodrigues,Josiane A. Sobrinho,Arthur Pignataro Machado,Zeno C. Brandao,Ingrid D. Barcelos,Cilene Labre,Rodrigo Szostak,Ana Flávia Nogueira","doi":"10.1021/acsenergylett.5c02838","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c02838","url":null,"abstract":"Bulky 2D alkylammonium cations in metal halide perovskites offer a route to improve both structural stability and optoelectronic performance. This study systematically explores the incorporation of alkylammonium iodides with different chain lengths─dodecylammonium (C12), hexadecylammonium (C16), and octadecylammonium (C18)─into perovskite films for solar cells. Using spectroscopic and nanoscale characterization techniques, we show that C12 provides the best results: enhanced [111] orientation, reduced nonradiative recombination, uniform cation distribution, and improved vertical conductivity. Nanoscale X-ray diffraction and AFM-based infrared spectroscopy revealed that intermediate chain lengths enable favorable lattice expansion and interfacial passivation without hindering crystal growth. Solar cells based on C12-modified films reached power conversion efficiencies over 20%, surpassing both pristine and longer-chain formulations. These findings demonstrate that tuning alkyl chain length is an effective molecular design strategy to guide perovskite crystallization and improve device performance and stability.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"276 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006311","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 : 2026-01-20DOI: 10.1021/acsenergylett.5c02838
Murillo Henrique de Matos Rodrigues,Josiane A. Sobrinho,Arthur Pignataro Machado,Zeno C. Brandao,Ingrid D. Barcelos,Cilene Labre,Rodrigo Szostak,Ana Flávia Nogueira
Bulky 2D alkylammonium cations in metal halide perovskites offer a route to improve both structural stability and optoelectronic performance. This study systematically explores the incorporation of alkylammonium iodides with different chain lengths─dodecylammonium (C12), hexadecylammonium (C16), and octadecylammonium (C18)─into perovskite films for solar cells. Using spectroscopic and nanoscale characterization techniques, we show that C12 provides the best results: enhanced [111] orientation, reduced nonradiative recombination, uniform cation distribution, and improved vertical conductivity. Nanoscale X-ray diffraction and AFM-based infrared spectroscopy revealed that intermediate chain lengths enable favorable lattice expansion and interfacial passivation without hindering crystal growth. Solar cells based on C12-modified films reached power conversion efficiencies over 20%, surpassing both pristine and longer-chain formulations. These findings demonstrate that tuning alkyl chain length is an effective molecular design strategy to guide perovskite crystallization and improve device performance and stability.
{"title":"Tuning Structure and Performance of 2D/3D Perovskites by Alkyl Chain Length Engineering","authors":"Murillo Henrique de Matos Rodrigues,Josiane A. Sobrinho,Arthur Pignataro Machado,Zeno C. Brandao,Ingrid D. Barcelos,Cilene Labre,Rodrigo Szostak,Ana Flávia Nogueira","doi":"10.1021/acsenergylett.5c02838","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c02838","url":null,"abstract":"Bulky 2D alkylammonium cations in metal halide perovskites offer a route to improve both structural stability and optoelectronic performance. This study systematically explores the incorporation of alkylammonium iodides with different chain lengths─dodecylammonium (C12), hexadecylammonium (C16), and octadecylammonium (C18)─into perovskite films for solar cells. Using spectroscopic and nanoscale characterization techniques, we show that C12 provides the best results: enhanced [111] orientation, reduced nonradiative recombination, uniform cation distribution, and improved vertical conductivity. Nanoscale X-ray diffraction and AFM-based infrared spectroscopy revealed that intermediate chain lengths enable favorable lattice expansion and interfacial passivation without hindering crystal growth. Solar cells based on C12-modified films reached power conversion efficiencies over 20%, surpassing both pristine and longer-chain formulations. These findings demonstrate that tuning alkyl chain length is an effective molecular design strategy to guide perovskite crystallization and improve device performance and stability.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"50 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006312","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 : 2026-01-20DOI: 10.1021/acsenergylett.5c03891
Zhentao Yang, Jiande Wang, Julius J. Oppenheim, Mircea Dincă
Rapid and selective ion transport defines the effectiveness of quasi-solid-state electrolytes (QSSEs) in next-generation solid-state batteries. Although metal–organic frameworks (MOFs) hold promise in this sense due to their compositional variety, tunable porosity, and ability to host electrolytes in the pores while maintaining solid-state processability, MOF-based QSSEs exhibit lower ionic conductivity, transference numbers, and electrochemical stability than often expected. We envision enhancing these parameters by using anionic MOFs with mobile pore cations and diffuse anionic charges. In this study, we present a postsynthetic modification approach for the anionic MOF SU-102 ([(CH3)2NH2]2[Zr(HL)2]; H4L = ellagic acid), involving substitution of charge-balancing dimethylammonium with various single metal cations (SU-102-M; M = Li+, Na+, K+, Mg2+, Al3+). This modification yields solid electrolytes with Li+, Na+, and Al3+ conductivities that rival current top-performing materials (5.16 × 10–4, 1.49 × 10–3, and 7.14 × 10–5 S/cm, respectively). These MOFs demonstrate high cation transference numbers for Li+ (0.899), Na+ (0.833), and Al3+ (0.706) as well as broad and stable operational potential windows spanning up to 4 V.
{"title":"SU-102 Is a Versatile Anionic Quasi-Solid Electrolyte for Fast Li+, Na+, and Al3+ Transport","authors":"Zhentao Yang, Jiande Wang, Julius J. Oppenheim, Mircea Dincă","doi":"10.1021/acsenergylett.5c03891","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03891","url":null,"abstract":"Rapid and selective ion transport defines the effectiveness of quasi-solid-state electrolytes (QSSEs) in next-generation solid-state batteries. Although metal–organic frameworks (MOFs) hold promise in this sense due to their compositional variety, tunable porosity, and ability to host electrolytes in the pores while maintaining solid-state processability, MOF-based QSSEs exhibit lower ionic conductivity, transference numbers, and electrochemical stability than often expected. We envision enhancing these parameters by using anionic MOFs with mobile pore cations and diffuse anionic charges. In this study, we present a postsynthetic modification approach for the anionic MOF SU-102 ([(CH<sub>3</sub>)<sub>2</sub>NH<sub>2</sub>]<sub>2</sub>[Zr(HL)<sub>2</sub>]; H<sub>4</sub>L = ellagic acid), involving substitution of charge-balancing dimethylammonium with various single metal cations (SU-102-M; M = Li<sup>+</sup>, Na<sup>+</sup>, K<sup>+</sup>, Mg<sup>2+</sup>, Al<sup>3+</sup>). This modification yields solid electrolytes with Li<sup>+</sup>, Na<sup>+</sup>, and Al<sup>3+</sup> conductivities that rival current top-performing materials (5.16 × 10<sup>–4</sup>, 1.49 × 10<sup>–3</sup>, and 7.14 × 10<sup>–5</sup> S/cm, respectively). These MOFs demonstrate high cation transference numbers for Li<sup>+</sup> (0.899), Na<sup>+</sup> (0.833), and Al<sup>3+</sup> (0.706) as well as broad and stable operational potential windows spanning up to 4 V.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"17 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001566","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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