Pub Date : 2026-10-16DOI: 10.1021/acsenergylett.6c02792
Hossein Roshan,Guncem Ozgun Eren,Joost W. C. Reinders,Simon Letzer,Chiara Maria Solinas,Yurii P. Ivanov,Giorgio Divitini,Mirko Prato,Francesco De Boni,Caroline Murawski,Luca De Trizio,Henk J. Bolink,Kassio P. S. Zanoni,Liberato Manna,Francesco Di Stasio
Abstract Light-emitting diodes (LEDs) based on colloidal InAs quantum dots (QDs) have emerged as promising light sources for the short-wave infrared (SWIR) range. However, their development is limited by relatively low photoluminescence quantum yield as well as intrinsic device design challenges. Here, we report LEDs with electroluminescence (EL) in the SWIR based on InAs/ZnSe core/shell colloidal QDs, synthesized via a seedless one-pot approach that enables the rapid growth of relatively large InAs cores. Zirconium-doped indium oxide (InZrO) was used as the bottom transparent electrode owing to its significantly higher infrared transparency compared to the commonly employed tin-doped indium oxide (ITO). These two key innovations pushed the EL beyond 1500 nm, with external quantum efficiencies of 3.0, 1.2, and 0.6% at 1093, 1198, and 1547 nm, respectively.
{"title":"Overcoming Indium-Tin-Oxide Optical Losses in InAs Colloidal Quantum-Dot Light-Emitting Diodes at 1550 nm","authors":"Hossein Roshan,Guncem Ozgun Eren,Joost W. C. Reinders,Simon Letzer,Chiara Maria Solinas,Yurii P. Ivanov,Giorgio Divitini,Mirko Prato,Francesco De Boni,Caroline Murawski,Luca De Trizio,Henk J. Bolink,Kassio P. S. Zanoni,Liberato Manna,Francesco Di Stasio","doi":"10.1021/acsenergylett.6c02792","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02792","url":null,"abstract":"Abstract Light-emitting diodes (LEDs) based on colloidal InAs quantum dots (QDs) have emerged as promising light sources for the short-wave infrared (SWIR) range. However, their development is limited by relatively low photoluminescence quantum yield as well as intrinsic device design challenges. Here, we report LEDs with electroluminescence (EL) in the SWIR based on InAs/ZnSe core/shell colloidal QDs, synthesized via a seedless one-pot approach that enables the rapid growth of relatively large InAs cores. Zirconium-doped indium oxide (InZrO) was used as the bottom transparent electrode owing to its significantly higher infrared transparency compared to the commonly employed tin-doped indium oxide (ITO). These two key innovations pushed the EL beyond 1500 nm, with external quantum efficiencies of 3.0, 1.2, and 0.6% at 1093, 1198, and 1547 nm, respectively.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"52 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209880","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}
Abstract In anode-free Li metal batteries, a bare current collector must be converted into a reversible Li metal anode during the first charge, making Li nucleation decisive for reversibility. However, how current collector microstructure governs Li nucleation and growth remains poorly understood, since prior studies focused on single-crystal surfaces to identify favorable crystallographic orientations, leaving grain boundaries unexplored. Here, we identify grain boundary density and character in copper current collectors as key regulators of Li deposition uniformity. Systematic annealing decouples grain size from surface chemistry, revealing that deposition uniformity improves with copper grain coarsening but saturates as disordered boundaries are eliminated during grain growth, leaving predominantly low-energy configurations. Atomistic simulations show disordered boundaries impose high barriers to Li adatom migration, whereas ordered boundaries and adjacent low-index terraces provide low-barrier pathways for redistribution. Copper foils engineered beyond this threshold sustain uniform Li plating across diverse electrolytes and improve cyclability in anode-free cells.
{"title":"Grain Boundary Character Governs Lithium Deposition Uniformity on Polycrystalline Copper","authors":"Minhyung Kwon,Seungyun Jeon,Dong Yeon Kim,Uk Jung Kang,Gaeun Kim,Chang-Gon Jeong,Jihyun Hong,Minah Lee","doi":"10.1021/acsenergylett.6c02640","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02640","url":null,"abstract":"Abstract In anode-free Li metal batteries, a bare current collector must be converted into a reversible Li metal anode during the first charge, making Li nucleation decisive for reversibility. However, how current collector microstructure governs Li nucleation and growth remains poorly understood, since prior studies focused on single-crystal surfaces to identify favorable crystallographic orientations, leaving grain boundaries unexplored. Here, we identify grain boundary density and character in copper current collectors as key regulators of Li deposition uniformity. Systematic annealing decouples grain size from surface chemistry, revealing that deposition uniformity improves with copper grain coarsening but saturates as disordered boundaries are eliminated during grain growth, leaving predominantly low-energy configurations. Atomistic simulations show disordered boundaries impose high barriers to Li adatom migration, whereas ordered boundaries and adjacent low-index terraces provide low-barrier pathways for redistribution. Copper foils engineered beyond this threshold sustain uniform Li plating across diverse electrolytes and improve cyclability in anode-free cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"13 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209877","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}
Abstract Interfacial losses at the perovskite/C60 and C60/metal contacts limit inverted perovskite solar cell performance. Here, we introduce a vacuum-evaporated molecule with giant spontaneous orientation polarization, 6F-2PI, for simultaneously tailoring both interfaces. Incorporating 6F-2PI increases the work function of perovskite, reducing the conduction band offset at the perovskite/C60 interface, which facilitates electron extraction. Concurrently, its phthalimide moieties passivate defect states, suppressing nonradiative recombination, as evidenced by a 0.03 eV recovery in quasi-Fermi level splitting. At the C60/metal interface, 6F-2PI also delivers efficient charge extraction, improved interfacial contact, and thermal resilience. Moreover, its hydrophobic fluorinated units prevent moisture ingress. Consequently, this dual-interface modulation boosts PCE from 18.5% to 22.5% with exceptional device stability, retaining over 90% of its initial efficiency after 2000 h under ambient conditions. Furthermore, this framework exhibits universal compatibility across both vacuum-deposited and solution-processed devices and simplifies processing for mass production.
{"title":"Vacuum-Evaporated Molecules with Giant Spontaneous Orientation Polarization for Inverted Perovskite Solar Cells","authors":"Yun-Sheng Jheng,Hao-Cheng Lin,I-Ting Liu,Zong-Han Lee,Ping-Hsun Tsai,Hung-Ming Chen,Yu-Ting Chen,Tzung-Fang Guo,Masaki Tanaka,Hao-Wu Lin","doi":"10.1021/acsenergylett.6c02427","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02427","url":null,"abstract":"Abstract Interfacial losses at the perovskite/C60 and C60/metal contacts limit inverted perovskite solar cell performance. Here, we introduce a vacuum-evaporated molecule with giant spontaneous orientation polarization, 6F-2PI, for simultaneously tailoring both interfaces. Incorporating 6F-2PI increases the work function of perovskite, reducing the conduction band offset at the perovskite/C60 interface, which facilitates electron extraction. Concurrently, its phthalimide moieties passivate defect states, suppressing nonradiative recombination, as evidenced by a 0.03 eV recovery in quasi-Fermi level splitting. At the C60/metal interface, 6F-2PI also delivers efficient charge extraction, improved interfacial contact, and thermal resilience. Moreover, its hydrophobic fluorinated units prevent moisture ingress. Consequently, this dual-interface modulation boosts PCE from 18.5% to 22.5% with exceptional device stability, retaining over 90% of its initial efficiency after 2000 h under ambient conditions. Furthermore, this framework exhibits universal compatibility across both vacuum-deposited and solution-processed devices and simplifies processing for mass production.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209876","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 : 2026-10-15DOI: 10.1021/acsenergylett.6c01945
Milan Babu Poudel,Saleem Sidra,Dharma Raj Kandel,Ouattara Lelourou Abdoul Karim,Jaewoo Lee,Do Hwan Kim,Dong Jin Yoo
Abstract The performance of energy storage devices utilizing multilayered materials is governed by the complex interactions between electrolyte ions and the electrode. Consequently, inhibiting the irreversible oxidative failure of the electrodes is crucial. Herein, an in situ modification strategy that introduces NH4+ species in Nb2CTx MXene electrodes and integrates them with 1T phase VS2/WS2 heteronanosheets is evaluated. The resulting VS2/WS2–Nb2CTx–NH4+ electrodes demonstrate a specific capacity of up to 217.48 mA h g–1 at 1 A g–1 with excellent electrochemical stability at high current densities. Density functional theory simulations confirmed the strong electronic interaction between the NH4+-intercalated Nb2CTx and 1T-WS2/VS2 nanosheets, resulting in higher OH– adsorption energies. Operando Raman analysis revealed that the process involves cation dehydration and K+ rehydration. These results highlight the importance of NH4+ dynamics, thermodynamic stability, and interfacial interactions. A VS2/WS2–Nb2CTx–NH4+//N-doped nanocube-based asymmetric supercapacitor was fabricated, exhibiting a peak energy density of 54 Wh kg–1 and long-term cycling stability without significant performance degradation.
摘要多层材料储能装置的性能受电解质离子与电极之间复杂相互作用的支配。因此，抑制电极的不可逆氧化失效是至关重要的。本研究评估了在Nb2CTx MXene电极中引入NH4+物种并将其与1T相VS2/WS2杂烷片整合的原位修饰策略。所得的VS2/ WS2-Nb2CTx-NH4 +电极在1 a g-1时的比容量高达217.48 mA h g-1，在高电流密度下具有优异的电化学稳定性。密度泛函理论模拟证实了NH4+插层Nb2CTx与1T-WS2/VS2纳米片之间的强电子相互作用，从而导致更高的OH -吸附能。Operando拉曼分析表明，该过程涉及阳离子脱水和K+再水化。这些结果强调了NH4+动力学、热力学稳定性和界面相互作用的重要性。制备了VS2/ WS2-Nb2CTx-NH4 +// n掺杂的纳米立方基非对称超级电容器，峰值能量密度为54 Wh kg-1，长期循环稳定，性能没有明显下降。
{"title":"Ammonium Ion Intercalation Enabled Stable 1T-VS2/WS2-Nb2CTx Heterostructures during Electrochemical Charge Storage","authors":"Milan Babu Poudel,Saleem Sidra,Dharma Raj Kandel,Ouattara Lelourou Abdoul Karim,Jaewoo Lee,Do Hwan Kim,Dong Jin Yoo","doi":"10.1021/acsenergylett.6c01945","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01945","url":null,"abstract":"Abstract The performance of energy storage devices utilizing multilayered materials is governed by the complex interactions between electrolyte ions and the electrode. Consequently, inhibiting the irreversible oxidative failure of the electrodes is crucial. Herein, an in situ modification strategy that introduces NH4+ species in Nb2CTx MXene electrodes and integrates them with 1T phase VS2/WS2 heteronanosheets is evaluated. The resulting VS2/WS2–Nb2CTx–NH4+ electrodes demonstrate a specific capacity of up to 217.48 mA h g–1 at 1 A g–1 with excellent electrochemical stability at high current densities. Density functional theory simulations confirmed the strong electronic interaction between the NH4+-intercalated Nb2CTx and 1T-WS2/VS2 nanosheets, resulting in higher OH– adsorption energies. Operando Raman analysis revealed that the process involves cation dehydration and K+ rehydration. These results highlight the importance of NH4+ dynamics, thermodynamic stability, and interfacial interactions. A VS2/WS2–Nb2CTx–NH4+//N-doped nanocube-based asymmetric supercapacitor was fabricated, exhibiting a peak energy density of 54 Wh kg–1 and long-term cycling stability without significant performance degradation.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209879","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 : 2026-10-15DOI: 10.1021/acsenergylett.6c02336
Lennart van den Hengel,Nathan Rodkey,Vladimir Held,Ana Puchades Ortiz,Cristina Roldán-Carmona,Tom Baines,Henk J. Bolink
Abstract A large number of publications, using diverse production techniques, are demonstrating the potential of metal halide perovskite thin-film devices. Promising records in power conversion efficiencies, device lifetimes and photo-electrical applications have been reported worldwide. A simple and rapid deposition method, however, is still missing. This work introduces a possible answer: Gas Flow Assisted Flash Evaporation (Gas-FE). Gas-FE is a solvent-free deposition method operating under modest vacuum conditions that enables the deposition of complex perovskites with components having varying vapor pressures. We demonstrate its capabilities by subliming complex powder compositions relevant for perovskite photovoltaics and show a proof-of-concept methylammonium lead iodide-based (MAPbI3) solar cell containing methylammonium chloride and lithium TFSI as dopants. Growth rates exceeding 1 µm/min are obtained for crystalline, highly oriented perovskite films with good optical and electronic properties. The perovskite film is integrated into a fully vacuum-deposited p-i-n photovoltaic device, yielding a promising power conversion efficiency of 9.6%.
{"title":"Fast, Hybrid Perovskite Deposition via Gas Flow Assisted Single Source Flash Evaporation","authors":"Lennart van den Hengel,Nathan Rodkey,Vladimir Held,Ana Puchades Ortiz,Cristina Roldán-Carmona,Tom Baines,Henk J. Bolink","doi":"10.1021/acsenergylett.6c02336","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02336","url":null,"abstract":"Abstract A large number of publications, using diverse production techniques, are demonstrating the potential of metal halide perovskite thin-film devices. Promising records in power conversion efficiencies, device lifetimes and photo-electrical applications have been reported worldwide. A simple and rapid deposition method, however, is still missing. This work introduces a possible answer: Gas Flow Assisted Flash Evaporation (Gas-FE). Gas-FE is a solvent-free deposition method operating under modest vacuum conditions that enables the deposition of complex perovskites with components having varying vapor pressures. We demonstrate its capabilities by subliming complex powder compositions relevant for perovskite photovoltaics and show a proof-of-concept methylammonium lead iodide-based (MAPbI3) solar cell containing methylammonium chloride and lithium TFSI as dopants. Growth rates exceeding 1 µm/min are obtained for crystalline, highly oriented perovskite films with good optical and electronic properties. The perovskite film is integrated into a fully vacuum-deposited p-i-n photovoltaic device, yielding a promising power conversion efficiency of 9.6%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"77 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209881","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}
Abstract Two-dimensional/three-dimensional (2D/3D) mixed tin halide perovskites are promising lead-free photovoltaic absorbers, but uncontrolled crystallization produces excessive low-n phases that impede charge extraction due to a quantum confinement effect. Here, we employ 1,4-benzenediammonium iodide (1,4-BDI2) as a multifunctional additive to regulate crystallization, phase distribution, and defects. The additive modulates precursor colloid assembly and retards low-dimensional crystal growth, yielding dense films dominated by highly oriented three-dimensional perovskites with suppressed n = 1 and reduced n = 2 phases. Meanwhile, 1,4-BD2+ cations and unincorporated organic ligands accumulate at grain boundaries to form a passivating complex that passivates deep-trap states and forms favorable interfacial energy-level alignment to promote charge transfer. Consequently, inverted tin perovskite solar cells achieve a power conversion efficiency of 15.94% and an open-circuit voltage of 0.91 V, together with improved operational and storage stability. This work establishes an integrated molecular strategy for phase regulation and defect passivation in efficient lead-free photovoltaics.
{"title":"Unlocking Quantum Confinement in Two-/Three-Dimensional Tin-Based Perovskites for High-Efficiency Photovoltaics","authors":"Tianyue Wang,Wenqiu Deng,Jianjun Mei,Xiao Wu,Zhiqiang Guan,Miaomiao Xue,Haotian Guo,Qi Wei,Laigang Hu,Mingjie Li,Xiaomin Xu,Xinhui Lu,Feng Yan","doi":"10.1021/acsenergylett.6c02557","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02557","url":null,"abstract":"Abstract Two-dimensional/three-dimensional (2D/3D) mixed tin halide perovskites are promising lead-free photovoltaic absorbers, but uncontrolled crystallization produces excessive low-n phases that impede charge extraction due to a quantum confinement effect. Here, we employ 1,4-benzenediammonium iodide (1,4-BDI2) as a multifunctional additive to regulate crystallization, phase distribution, and defects. The additive modulates precursor colloid assembly and retards low-dimensional crystal growth, yielding dense films dominated by highly oriented three-dimensional perovskites with suppressed n = 1 and reduced n = 2 phases. Meanwhile, 1,4-BD2+ cations and unincorporated organic ligands accumulate at grain boundaries to form a passivating complex that passivates deep-trap states and forms favorable interfacial energy-level alignment to promote charge transfer. Consequently, inverted tin perovskite solar cells achieve a power conversion efficiency of 15.94% and an open-circuit voltage of 0.91 V, together with improved operational and storage stability. This work establishes an integrated molecular strategy for phase regulation and defect passivation in efficient lead-free photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"13 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209884","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}
Abstract The electrochemical carbon monoxide oxidation reaction (COOR) is an attractive anodic alternative to the oxygen evolution reaction, offering a route to lower the energy demand of electrosynthesis while utilizing abundant industrial waste gas. However, COOR has rarely been implemented in practical paired electrolysis systems because of modest device-level performance, reliance on purified CO feedstocks, and operational instability. Here, we establish a COOR∥two-electron oxygen reduction reaction paired electrolysis platform for H2O2 and CO32– coproduction using simulated CO-rich steelmaking flue gas. The system sustains bias-free operation for >140 h. Under high-current-density operation, in situ surface analysis revealed that interfacial carbonate accumulation causes anodic passivation and current decay. Pulsed electrolysis was introduced to alleviate such carbonate buildup and stabilized operation at 100 mA cm–2. Techno-economic analysis estimated an H2O2 minimum selling price of $0.71 kg–1. Together, these results establish COOR as a practical strategy for energy-efficient electrosynthesis using industrial waste gas.
{"title":"Carbon Monoxide Oxidation Enables Energy-Efficient Hydrogen Peroxide and Carbonate Coproduction from CO-Rich Flue Gas and Air","authors":"Eunseul Kong,Ye Chan Lee,Hyeongoo Kim,Junghye Lee,Tae Hoon Oh,Jungki Ryu","doi":"10.1021/acsenergylett.6c02386","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02386","url":null,"abstract":"Abstract The electrochemical carbon monoxide oxidation reaction (COOR) is an attractive anodic alternative to the oxygen evolution reaction, offering a route to lower the energy demand of electrosynthesis while utilizing abundant industrial waste gas. However, COOR has rarely been implemented in practical paired electrolysis systems because of modest device-level performance, reliance on purified CO feedstocks, and operational instability. Here, we establish a COOR∥two-electron oxygen reduction reaction paired electrolysis platform for H2O2 and CO32– coproduction using simulated CO-rich steelmaking flue gas. The system sustains bias-free operation for >140 h. Under high-current-density operation, in situ surface analysis revealed that interfacial carbonate accumulation causes anodic passivation and current decay. Pulsed electrolysis was introduced to alleviate such carbonate buildup and stabilized operation at 100 mA cm–2. Techno-economic analysis estimated an H2O2 minimum selling price of $0.71 kg–1. Together, these results establish COOR as a practical strategy for energy-efficient electrosynthesis using industrial waste gas.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"89 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209885","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 : 2026-10-14DOI: 10.1021/acsenergylett.6c01850
Jacob Wall,Yizhao Wang,Lingyan Kong,Lin Li,Kai Zhu,Joseph J. Berry,Feng Yan
Abstract Integrating dry carbon electrodes (CEs) into inverted perovskite solar cells (PSCs) offers a solvent-free, scalable route to low-cost photovoltaics. However, mechanical stress during lamination and the large work-function mismatch between the CE and the electron transport layer (ETL) can compromise performance. Here, we report an interface engineering strategy utilizing a silver-2-mercaptobenzothiazole (Ag-MBT) metal-polymer buffer layer to enable high-efficiency inverted CE-based PSCs (C-PSCs). XPS reveals Ag-induced changes in the sulfur and nitrogen chemical environments of MBT, consistent with the formation of an Ag-MBT interfacial coordination layer involving Ag–S coordination. This coordination-derived interlayer serves a dual function: it acts as a structural buffer, enabling damage-free dry CE lamination, and it establishes an energetic band alignment that bridges the ETL/CE work-function gap. Consequently, our devices achieve a champion power conversion efficiency (PCE) of 20.12% and maintain their initial efficiency after 1000 h of dark N2 storage, establishing metal-polymer interfacial coordination as a viable pathway for robust inverted C-PSCs.
{"title":"Tautomeric Metal-Polymer Coordination Enables Damage-Free Laminated Carbon Electrodes in Inverted Perovskite Solar Cells","authors":"Jacob Wall,Yizhao Wang,Lingyan Kong,Lin Li,Kai Zhu,Joseph J. Berry,Feng Yan","doi":"10.1021/acsenergylett.6c01850","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01850","url":null,"abstract":"Abstract Integrating dry carbon electrodes (CEs) into inverted perovskite solar cells (PSCs) offers a solvent-free, scalable route to low-cost photovoltaics. However, mechanical stress during lamination and the large work-function mismatch between the CE and the electron transport layer (ETL) can compromise performance. Here, we report an interface engineering strategy utilizing a silver-2-mercaptobenzothiazole (Ag-MBT) metal-polymer buffer layer to enable high-efficiency inverted CE-based PSCs (C-PSCs). XPS reveals Ag-induced changes in the sulfur and nitrogen chemical environments of MBT, consistent with the formation of an Ag-MBT interfacial coordination layer involving Ag–S coordination. This coordination-derived interlayer serves a dual function: it acts as a structural buffer, enabling damage-free dry CE lamination, and it establishes an energetic band alignment that bridges the ETL/CE work-function gap. Consequently, our devices achieve a champion power conversion efficiency (PCE) of 20.12% and maintain their initial efficiency after 1000 h of dark N2 storage, establishing metal-polymer interfacial coordination as a viable pathway for robust inverted C-PSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"87 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209883","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 : 2026-10-13DOI: 10.1021/acsenergylett.6c01934
Ziqing Wang,C. Buddie Mullins,Kent J. X. Zheng
Aqueous zinc metal batteries offer a safe and low-cost option for scalable energy storage; however, their practical reversibility is limited by nonuniform Zn plating/stripping and dendritic growth. Here, Zn single-crystal electrodes exposing well-defined (002), (100), and (101) crystalline facets were used to isolate the role of crystallography in Zn metal cycling. Zn deposition is strongly facet-dependent, forming hexagonal, rectangular/prismatic, and corner-defined morphologies on (002), (100), and (101) facets, respectively. Time-dependent SEM further reveals that Zn growth proceeds via discrete edge- or corner-initiated crystallographic units rather than uniform terrace coverage. During stripping, Zn metal is removed via facet-preserved mesoscopic dissolution domains, leaving geometry-defined pits rather than random corrosion-like features. However, these pits are not preferentially refilled during subsequent plating. Repeated cycling redirects Zn growth to protrusions and roughened regions, causing mossy/dendritic accumulation, mixed-texture evolution, and loss of epitaxial reversibility. These findings highlight the need to control both oriented deposition and poststripping surface reconstruction.
{"title":"Facet-Dependent Plating/Stripping Behavior and Crystallographic Evolution during Cycling on Zn Metal Anodes","authors":"Ziqing Wang,C. Buddie Mullins,Kent J. X. Zheng","doi":"10.1021/acsenergylett.6c01934","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01934","url":null,"abstract":"Aqueous zinc metal batteries offer a safe and low-cost option for scalable energy storage; however, their practical reversibility is limited by nonuniform Zn plating/stripping and dendritic growth. Here, Zn single-crystal electrodes exposing well-defined (002), (100), and (101) crystalline facets were used to isolate the role of crystallography in Zn metal cycling. Zn deposition is strongly facet-dependent, forming hexagonal, rectangular/prismatic, and corner-defined morphologies on (002), (100), and (101) facets, respectively. Time-dependent SEM further reveals that Zn growth proceeds via discrete edge- or corner-initiated crystallographic units rather than uniform terrace coverage. During stripping, Zn metal is removed via facet-preserved mesoscopic dissolution domains, leaving geometry-defined pits rather than random corrosion-like features. However, these pits are not preferentially refilled during subsequent plating. Repeated cycling redirects Zn growth to protrusions and roughened regions, causing mossy/dendritic accumulation, mixed-texture evolution, and loss of epitaxial reversibility. These findings highlight the need to control both oriented deposition and poststripping surface reconstruction.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"31 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152701","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}
Polymer coatings are widely used to stabilize silicon anodes, yet repeated volume changes can fracture the coating and accelerate continuous SEI reconstruction. Here, we construct a self-healing fluorinated acrylate/methacrylate copolymer coating in situ on silicon-based anodes through the UV-induced copolymerization of HFBA and MPS. The resulting copolymer combines strong adhesion with dynamic self-recovery through reversible dipole-dipole interactions, enabling microcrack repair within 1 min. Meanwhile, the HFBA-derived segments act as a fluorine reservoir, promoting the formation of a thin SEI with a polymer-rich outer layer and a LiF-rich inner layer. Consequently, SiOx-P(HFBA+MPS)||Li cells deliver 73.5% capacity retention after 500 cycles at 800 mA g–1. A practical 1.5 Ah NCM811||Si/C/Gr-P(HFBA+MPS) pouch cell achieves 71.9% capacity retention after 300 cycles and shows improved thermal safety. This work provides a scalable strategy for durable and safe silicon-based batteries by integrating autonomous self-healing of the polymer coating with sustained fluorine-assisted interphase stabilization.
聚合物涂层广泛用于稳定硅阳极，但反复的体积变化会破坏涂层并加速持续的SEI重建。在这里，我们通过紫外诱导的HFBA和MPS的共聚，在硅基阳极上原位构建了一种自修复的氟化丙烯酸酯/甲基丙烯酸酯共聚物涂层。通过可逆的偶极子-偶极子相互作用，这种共聚物结合了强附着力和动态自恢复能力，可以在1分钟内修复微裂纹。同时，hfba衍生的片段充当氟储层，促进形成具有富聚合物外层和富liff内层的薄SEI。因此，SiOx-P(HFBA+MPS)||锂电池在800 mA g-1下循环500次后，容量保持率为73.5%。实用的1.5 Ah NCM811||Si/C/Gr-P（HFBA+MPS）袋状电池在300次循环后容量保持率达到71.9%，并显示出更好的热安全性。这项工作通过将聚合物涂层的自主自愈与持续的氟辅助相间稳定相结合，为耐用和安全的硅基电池提供了一种可扩展的策略。
{"title":"Self-Healing Armor Enables Electrode Integrity and Interfacial Stability for Durable Silicon Anodes","authors":"Mengnan Shen,Yi Zhang,Ruifeng Song,Haolin Wang,Kai Huang,Zhuo Li,Yunhui Huang,Henghui Xu","doi":"10.1021/acsenergylett.6c02225","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02225","url":null,"abstract":"Polymer coatings are widely used to stabilize silicon anodes, yet repeated volume changes can fracture the coating and accelerate continuous SEI reconstruction. Here, we construct a self-healing fluorinated acrylate/methacrylate copolymer coating in situ on silicon-based anodes through the UV-induced copolymerization of HFBA and MPS. The resulting copolymer combines strong adhesion with dynamic self-recovery through reversible dipole-dipole interactions, enabling microcrack repair within 1 min. Meanwhile, the HFBA-derived segments act as a fluorine reservoir, promoting the formation of a thin SEI with a polymer-rich outer layer and a LiF-rich inner layer. Consequently, SiOx-P(HFBA+MPS)||Li cells deliver 73.5% capacity retention after 500 cycles at 800 mA g–1. A practical 1.5 Ah NCM811||Si/C/Gr-P(HFBA+MPS) pouch cell achieves 71.9% capacity retention after 300 cycles and shows improved thermal safety. This work provides a scalable strategy for durable and safe silicon-based batteries by integrating autonomous self-healing of the polymer coating with sustained fluorine-assisted interphase stabilization.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"18 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152702","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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