Jacob Wall,Yizhao Wang,Lingyan Kong,Lin Li,Kai Zhu,Joseph J. Berry,Feng Yan
{"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}
{"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}
{"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}
Daeho Kim,Hyobin Nam,Sae Yane Paek,Soonsung So,Nayeon Kim,Heeseung Lee,Hyuk Jun Yoo,Sang Kyu Kwak,Jong Min Kim,Seung Yong Lee,Sang Soo Han
{"title":"Overcoming the Trade-off Between the Activity, Stability, and Cost of OER Catalysts for Proton Exchange Membrane Water Electrolysis in a Self-Driving Laboratory","authors":"Daeho Kim,Hyobin Nam,Sae Yane Paek,Soonsung So,Nayeon Kim,Heeseung Lee,Hyuk Jun Yoo,Sang Kyu Kwak,Jong Min Kim,Seung Yong Lee,Sang Soo Han","doi":"10.1021/acsenergylett.6c02486","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02486","url":null,"abstract":"Abstract Proton exchange membrane water electrolysis (PEMWE) offers a sustainable route to hydrogen production, yet its practical deployment is limited by trade-offs among activity, stability, and precursor cost of acidic oxygen evolution reaction (OER) catalysts. Here, we present a self-driving laboratory (SDL) integrating automated batch synthesis, electrochemical half-cell testing, and AI-guided decision-making to simultaneously optimize these properties. A composition-constrained design space, clustering-based batch selection, and relaxed-percentile Pareto filtering enable efficient exploration of ternary Ir–Ru–X (X = Ni, Co, Fe) systems. Using this framework, the platform conducted 24 experiments per ternary system and identified Ir10Ru65Ni25/C as a Pareto-balanced composition exhibiting an overpotential of 211.8 mV at 10 mA cm–2, limited degradation after accelerated durability testing, and reduced Ir content. In PEMWE, Ir10Ru65Ni25 delivered 3.90 A cm–2 at 1.8 V and stable operation for 1000 h at 1.0 A cm–2, demonstrating SDL-driven discovery of multimetallic OER catalysts.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"37 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209887","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}
John F. Koons,Jeremy H. Lawrence,Ashutosh Rana,James H. Nguyen,Md. Arif Faisal,Savannah M. Hatch,Taizhe Liu,Jeffrey E. Dick
{"title":"Addressing the Zinc Corrosion Conundrum: The Vital Role of Resting-State Kinetics","authors":"John F. Koons,Jeremy H. Lawrence,Ashutosh Rana,James H. Nguyen,Md. Arif Faisal,Savannah M. Hatch,Taizhe Liu,Jeffrey E. Dick","doi":"10.1021/acsenergylett.6c02361","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02361","url":null,"abstract":"Aqueous zinc metal batteries (AZMBs) have emerged as a highly desirable system for grid storage applications due to low-cost, high-energy density, and safe operating conditions. While AZMB studies often focus on functional mitigation of dendrite formation and the hydrogen evolution reaction (HER), corrosion remains a more ambiguous yet crucial limiting factor in anode performance. Specifically, recent work points to persistent chemical corrosion as a major source of resting capacity loss in AZMBs. In this work, we present a wide-ranging mechanism for galvanic corrosion based on fundamental electrochemical thermodynamics and kinetics, highlighting the key roles of battery components, electrolyte conditions, and other contributing factors. Importantly, this mechanistic framework also applies when plating and stripping Zn on the anode, offering additional insight into the ever-elusive mechanistic origins of HER during those operating regimes. We then propose several promising avenues of inquiry and methods for further predicting, understanding, and mitigating corrosion in AZMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"32 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152007","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}
Patrick Lechner,Jana Bischoff,Pavel Pokhilko,Fu-Li Sun,Adrian Ertl,Herwig Michor,Cornelia von Baeckmann,Johannes C. B. Dietschreit,Dominik Eder,Leticia González
{"title":"Metal-Dependent Magnetic Exchange Topology as a Fingerprint of N2 Binding in Isostructural MOF Nodes","authors":"Patrick Lechner,Jana Bischoff,Pavel Pokhilko,Fu-Li Sun,Adrian Ertl,Herwig Michor,Cornelia von Baeckmann,Johannes C. B. Dietschreit,Dominik Eder,Leticia González","doi":"10.1021/acsenergylett.6c02509","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02509","url":null,"abstract":"Triangular metal-oxo nodes are widely employed as catalytic motifs in metal–organic frameworks. Photocatalytic N2 fixation using the all-iron nodes can be switched off by replacing them with all-chromium nodes. However, the two nodes bind N2 in the opposite order to their activity. The present contribution shows that the electronic structure of the metal, which governs the small-molecule binding to the framework, determines the magnetic exchange topology of the [MIII3(μ3-O)] node. Combining broken-symmetry and non-collinear DFT, Hamiltonian-based reconstruction of Mössbauer spectra, and quantitative modeling of temperature-dependent magnetic susceptibility, one finds that FeIII exhibits a genuinely frustrated triangle of comparable antiferromagnetic interactions, whereas CrIII features an asymmetric dimer-plus-monomer governed by unusually strong biquadratic interaction, placing it outside the conventional Heisenberg regime. The distinct electronic structure is reflected in markedly different magnetic topologies and N2 binding strengths, rationalizing the contrasting photocatalytic activities of the two frameworks. These results establish magnetic exchange topology as an experimentally accessible descriptor of chemical function in trinuclear MOF nodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"167 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152008","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}
Youngmin Ko,Dong-Min Kim,Andrew Dopilka,Marco-Tulio Fonseca Rodrigues,Gabriel D. Parker,Steven Lam,Xiao-Ying Yu,Amanda L. Musgrove,Robert Kostecki,Brett A. Helms
{"title":"Improving the Calendar Life of Silicon Anodes with Inorganic Solid–Electrolyte Interphases","authors":"Youngmin Ko,Dong-Min Kim,Andrew Dopilka,Marco-Tulio Fonseca Rodrigues,Gabriel D. Parker,Steven Lam,Xiao-Ying Yu,Amanda L. Musgrove,Robert Kostecki,Brett A. Helms","doi":"10.1021/acsenergylett.6c02871","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02871","url":null,"abstract":"Abstract Silicon anodes unlock higher energy density in Li-ion batteries but suffer from poor calendar life due to inadequately passivating solid–electrolyte interphases (SEIs). Here, we contrast the calendar aging behaviors of single- and mixed-salt locally superconcentrated electrolytes (LSCEs) against carbonate electrolytes. Mixed-salt LSCE cells retained 96% and 44% of precalendar capacity after one month and then after five months, while carbonate electrolyte cells retained 77% and 1%, respectively. The mixed-salt LSCE advantage is tied to the formation of a predominantly inorganic SEI, evidenced by nanoscale Fourier transform infrared spectromicroscopy, X-ray photoelectron spectroscopy, and 3D time-of-flight secondary ion mass spectrometry. After 5 months, however, perturbations to SEIs were evident in all cells, accelerating voltage decay and capacity loss by lithium inventory loss associated with SEI growth. These findings suggest that future electrolytes may benefit from strategies that continuously reinforce the SEI through controlled anion and solvent redox in LSCEs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"88 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151303","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}
{"title":"Formamidinium-Solvent Intermediates Mediate Self-Seeding Crystallization for Efficient Inverted α-FAPbI3 Perovskite Solar Cells","authors":"Yezhi Li,Shuyuan Wan,Yang Yang,Fengyuan Li,Xu Xiao,Haoze Lu,Zihao Fan,Zhiyuan Dai,Yaqian Zhou,Yerzhan Mukhametkarimov,Ruihao Chen,Hongqiang Wang","doi":"10.1021/acsenergylett.6c01690","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01690","url":null,"abstract":"Abstract Formamidinium lead iodide (FAPbI3) perovskites are promising for high-performance solar cells; however, the low surface energy of self-assembled monolayers (SAMs) impedes α-phase nucleation in inverted devices. Here, we report a formamidinium (FA)-solvent intermediate-mediated self-seeding crystallization strategy to enable quality α-phase FAPbI3. By employing N-formylmorpholine (NFM) as a non-toxic solvent, (FA···NFM)PbI3 intermediates are formed, thereby lowering the phase-transition barrier and promoting the spontaneous formation of α-phase nuclei at the early stage of crystallization. These preformed nuclei serve as intrinsic seeds, facilitating rapid nucleation and orientated crystal growth. Consequently, NFM-based devices achieve efficiencies of 26.41% and 26.56% using 2-methoxyethanol (2-Me) and N,N-dimethylformamide (DMF) as primary solvents, respectively, with a 1 cm2 device reaching 25.47%. The unencapsulated devices retain 85% and 90% of their initial efficiencies after 1200 h illumination and 1400 h thermal aging at 85 °C, respectively.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"12 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151302","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}
ACS Energy Letters Pub Date : 2026-10-09Epub Date: 2026-07-25DOI: 10.1021/acsenergylett.6c01307
Jose J. Jeronimo-Rendon, Mahdi Malekshahi Byranvand, Sofya Svetlosanova, Rajarshi Roy, Seyma Topcu, Asfaw Negash, Mayank Kedia, Somayeh Gholipour, Anna Zhuravlova, Paolo Samorì, Antonio Gaetano Ricciardulli, Michael Saliba
{"title":"Sulfolane-Based Solvent Polishing of Perovskite Films for Optimized Solar Cells","authors":"Jose J. Jeronimo-Rendon, Mahdi Malekshahi Byranvand, Sofya Svetlosanova, Rajarshi Roy, Seyma Topcu, Asfaw Negash, Mayank Kedia, Somayeh Gholipour, Anna Zhuravlova, Paolo Samorì, Antonio Gaetano Ricciardulli, Michael Saliba","doi":"10.1021/acsenergylett.6c01307","DOIUrl":"10.1021/acsenergylett.6c01307","url":null,"abstract":"<p>The complex crystallization of solution-processed polycrystalline perovskite films leads to the formation of deep-trap states, ultimately hindering the performance of perovskite solar cells (PSCs). Here, we have devised a facile and practical solvent polishing (SP) approach utilizing a sulfolane and chlorobenzene mixture to reconstruct the surface of triple-cation perovskite films. This strategy enables the removal of the surface-oriented phases containing trap sites, exposing compact vertically aligned crystalline domains with lower defectiveness and lower surface roughness, ultimately leading to enhanced carrier transport, facilitating interfacial charge extraction, and suppressing nonradiative recombination losses. Consequently, the PSCs fabricated with SP exhibit a higher power conversion efficiency (PCE) of 22.0% with a remarkable fill factor (FF) of 82%, surpassing the control device (20.5% PCE and 79% FF). Additionally, the SP-treated devices retain 94% of their initial efficiency after 40 days at 40% relative humidity, indicating improved shelf stability under moderately humid conditions.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6487–6496"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148595867","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}
ACS Energy Letters Pub Date : 2026-10-09Epub Date: 2026-07-28DOI: 10.1021/acsenergylett.6c01697
Yanlin Huang, Mingyang Wang, Youjin Reo, Xiaomin Yang, Sai Bai, Zhikai Le, Ao Liu, Yong-Young Noh, Huihui Zhu
{"title":"Antisolvent-Free Crystallization-Directed Two-Dimensional/Three-Dimensional Tin Perovskites for Ambient-Tolerant Electronics","authors":"Yanlin Huang, Mingyang Wang, Youjin Reo, Xiaomin Yang, Sai Bai, Zhikai Le, Ao Liu, Yong-Young Noh, Huihui Zhu","doi":"10.1021/acsenergylett.6c01697","DOIUrl":"10.1021/acsenergylett.6c01697","url":null,"abstract":"<p>Tin (Sn<sup>2+</sup>) halide perovskites offer a promising lead-free semiconductor platform, yet their practical application is hindered by severe ambient instability. Here, we regulate the early-stage oxygen response of mixed-dimensional Sn<sup>2+</sup> perovskites through crystallization pathway engineering without introducing additional stabilizing molecules. Removing antisolvent quenching enables gradual solvent evaporation and cation redistribution, leading to a vertically organized structure with a two-dimensional (2D)-rich surface region and a three-dimensional (3D) FASnI<sub>3</sub> transport framework. This architecture balances environmental tolerance and charge transport, where low-dimensional regions contribute to oxygen regulation while the 3D framework maintains efficient hole conduction. Field-effect measurements reveal reversible oxygen-induced conductivity enhancement, suggesting weak oxygen adsorption dominates the initial response. Polymer/oxide encapsulation further improves air stability, and integration with oxide n-channel transistors demonstrates the potential of this approach for complementary thin-film electronics.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6548–6555"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148595812","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}