Connor M. Davel,Nazanin Bassiri-Gharb,Juan-Pablo Correa-Baena
{"title":"Deliquescence Thresholds of Halide Perovskite Precursor Salts Govern Moisture Sensitivity","authors":"Connor M. Davel,Nazanin Bassiri-Gharb,Juan-Pablo Correa-Baena","doi":"10.1021/acsenergylett.6c02999","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02999","url":null,"abstract":"Lead halide perovskite precursor salts exhibit deliquescence, where water spontaneously condenses from the air above a discrete onset relative humidity to form a saturated aqueous salt solution. FABr salts exhibit the lowest deliquescence relative humidity (DRH), followed by MABr, MAI/FAI, and finally the inorganic PbBr2/PbI2 and perovskite MAPbBr3, identifying deliquescence as a threshold process that may accelerate moisture-induced degradation at organohalide-rich, lead-deficient perovskite surfaces.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149303293","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":"Vertically Graded Dual Salts to Suppress Interfacial Mobile-Ion Accumulation for Stable Perovskite Photovoltaics","authors":"Kaidi Liu,Zixiang Wang,Lu Bai,Lei Xu,Fanshuo Kong,Chengcheng Li,Jingya Lai,Jin Chang,Zhen Wang,Jianpu Wang","doi":"10.1021/acsenergylett.6c02002","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02002","url":null,"abstract":"Suppression of mobile-ion accumulation at the perovskite interface is critical for perovskite photovoltaic (PV) stability. Post-treatment with fluorinated aromatic ammonium salts can suppress ion migration at perovskite interfaces. However, these salts damage underlying three-dimensional (3D) perovskites during device operation, inducing interfacial mobile-ion accumulation. Although these cations form gradient low-dimensional perovskites for enhanced quality of bulk quasi-2D films, constructing an ultrathin gradient structure by post-treatment remains challenging. Here, we demonstrate a preferential spatial arrangement of dual fluorinated ammonium cations at the FA0.95Cs0.05PbI3 perovskite interface, which suppresses the interfacial mobile-ion accumulation. This arrangement includes both long-chain cations on the topmost surface and short-chain cations preferentially in the sub-surface region. This unique surface structure suppresses mobile-ion accumulation at the LD/3D heterostructure. Our n–i–p perovskite PV achieves an efficiency of 26.47% (certified 25.95%). Moreover, the resulting perovskite PVs exhibit an operational stability of 3600 h at 55 °C and a thermal stability of 3500 h at 85 °C.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"6 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149303296","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":"Constructing Hybrid Solid–Liquid Li+ Transport Networks for Fast-Charging Thick Electrodes","authors":"Jiacheng Zhu,Xuewei Gu,Hongmei Song,Defu Cao,Jiliang Qiu,Qi Yang,Huajun Li,Shuwei Li,Wenjun Li,Ziwei Wang,Qiu Fang,Cong Zhong,Zhaoxiang Wang,Byoungwoo Kang,Jizhou Li,Huigen Yu,Yejing Li,Hong Li,Tao Cheng,Xuefeng Wang","doi":"10.1021/acsenergylett.6c03027","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c03027","url":null,"abstract":"Fast-charging technology for high-energy-density lithium-ion batteries remains constrained by high interfacial impedance and sluggish Li+ transport within electrodes. Herein, hierarchical-sized Li1.5Al0.5Ti1.5(PO4)3 (LATP, particle ranging from 5 to 500 nm) is used to construct a hybrid solid–liquid Li+ transport network in high-mass-loading cathodes (27 mg cm–2). A combination of different characterization techniques is employed to understand the underlying working principle of LATP from the particle to the electrode scale. LATP nanograins (∼10 nm) adsorbed onto cathode particle surfaces reduce Li+ desolvation energy (43.30 vs 52.97 kJ mol–1) and stabilize a thin CEI after cycling. Submicron LATP particles (320–480 nm) infiltrate pores of thick electrodes, forming interconnected networks that increase the Li+ diffusion coefficient. Furthermore, LATP increases the Li+ transference number of the liquid electrolyte within LATP-permeated regions. Consequently, LiNi0.8Co0.1Mn0.1O2||Li cells with LATP-blended cathodes deliver dramatically enhanced rate performance (102 vs 36 mAh g–1 at 0.75C and –10 °C).","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"24 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149303305","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}
Min Gyu Choi,Seong Hyun Park,Young Je Park,Jin Huh,Soobin Yoon,Pilyoung Lee,Young-June Park,Chi-Young Jung,Kang Taek Lee
{"title":"Gradient Engineered Microporous Layers for Enhanced Oxygen Transport in PEM Water Electrolysis","authors":"Min Gyu Choi,Seong Hyun Park,Young Je Park,Jin Huh,Soobin Yoon,Pilyoung Lee,Young-June Park,Chi-Young Jung,Kang Taek Lee","doi":"10.1021/acsenergylett.6c02173","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02173","url":null,"abstract":"Microporous layers (MPLs) improve catalyst utilization in proton exchange membrane water electrolysis (PEMWE), but must accommodate rapid oxygen removal at high current densities. Dense or poorly oriented MPLs can convert an interfacial benefit into a gas-transport penalty. Here, we introduce a gradient engineered MPL (G-MPL) where porosity and pore size increase from the catalyst side toward the porous transport layer (PTL). This architecture reduces voltage to 2.161 V at 5 A cm–2, outperforming uniform and reverse-gradient MPLs. Electrochemical analysis indicates the gain arises from reduced ohmic and transport-related losses, rather than from interfacial contact alone. Digital twin analyses show the pore gradient promotes oxygen evacuation and limits gas-filled regions restricting water access. Under limited water supply, the G-MPL retains stable operation at high current density. These results establish directional pore grading as an MPL design strategy for maintaining catalyst layer/PTL contact while managing oxygen-water transport in high current density PEMWE.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"4 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149303295","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}
Varanasi Sai Subhankar,Michael Baldea,Graeme Henkelman,C. Buddie Mullins,Thomas C. Underwood
{"title":"Predictive Design Principles for Plasma-Catalysis","authors":"Varanasi Sai Subhankar,Michael Baldea,Graeme Henkelman,C. Buddie Mullins,Thomas C. Underwood","doi":"10.1021/acsenergylett.6c02711","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02711","url":null,"abstract":"Centralized production of fuels and commodity chemicals emits 1.4–2 Gt CO2 yr–1 and depends on fossil-fuel supply chains that prevent distributed deployment. Nonthermal plasmas offer a path to decentralized, electrified production by generating vibrationally excited molecules, radicals, and ions without bulk heating of gas. Despite this potential, plasma-catalysis remains difficult to design because plasma excitation, surface reaction energetics, and intermediate removal are treated separately, and activity trends do not transfer across chemistries. This perspective develops a quantitative framework connecting nonequilibrium excitation, surface binding energetics, coreactant chemistry, and surface temperature to reaction rates, selectivity, and catalyst stability. Reactions are classified into three kinetic regimes by the balance between intermediate supply and removal rates, each with distinct rate-controlling steps and deactivation modes. Design tools and principles derived from this classification are applied to four example case studies that transfer across chemistries without reparameterization and provide a basis for reactor design at scale.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"16 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149281780","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}
Haoyu Kong,Byron Ross,Amandine Bruyndonckx,Bin Wang,David G. Kwabi
{"title":"A 2.2 V Aqueous Redox Flow Battery Enabled by Passive pH Decoupling","authors":"Haoyu Kong,Byron Ross,Amandine Bruyndonckx,Bin Wang,David G. Kwabi","doi":"10.1021/acsenergylett.6c02731","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02731","url":null,"abstract":"Aqueous redox flow batteries (ARFBs) comprising earth-abundant charge carriers could cheaply store grid-scale renewable electricity, but most lab-scale systems have a low open-circuit potential (OCP) that inflates system cost. We report a non-hybrid aqueous flow cell with an OCP of 2.2 V, among the highest reported for this class, pairing an alkaline chromium-1,3-propylenediaminetetraacetate negolyte with an acidic bromide posolyte. The two electrolytes maintain an approximately seven-unit pH gradient across a single cation-exchange membrane, without external oxygen or a bipolar-membrane recovery sub-cell: operando pH measurements and a zero-dimensional model show that the difference is sustained passively by balancing slow proton crossover against hydrogen evolution and positive-side acid generation. The cell cycles for 240 h with a Coulombic efficiency of up to 99.5%; tuning the posolyte additive, electrode, and membrane raises the peak power density to 534 mW cm–2 at 43 °C.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"16 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149269153","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":"Operando Raman Spectroscopy-Guided 24-Hour Aging Assessment of Activated Carbon Positive Electrodes for Lithium-Ion Capacitors","authors":"Yu-Chun Chen,Liang-Chieh Tseng,Hsiang-Sheng Wei,Hao-Hsuan Hsia,Yun Lin,Chen-Wei Tai,Yi-Cheng Liao,Jing-Cheng Liang,Chung-Yu Hsu,Pei-Lin Yang,Jie-Yu Liao,Fu-Ming Wang,Tsu-Chin Chou,Chi-Chang Hu","doi":"10.1021/acsenergylett.6c02322","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02322","url":null,"abstract":"While high-power lithium-ion capacitors (LICs) with high energy density emerge as promising pulse-/peak-power solutions for AI data centers, their long-term viability remains severely hindered by the degradation of the activated carbon (AC) positive electrode. To evaluate this aging behavior, we propose a 24-h high-voltage cycling (HVC) protocol integrated with operando Raman spectroscopy, demonstrating that the turning point in the D1 band can serve as a sensitive indicator of corrosion severity. During the early-stage HVC aging, cathode–electrolyte interphase (CEI) formation and gas evolution passivate defect-related Raman signals, narrowing the D1 band. As aging proceeds, carbon corrosion becomes dominant and broadens the D1 band. By validating this approach across various ACs, we establish a direct correlation between an earlier structural turning point and accelerated capacity decay, thereby uncovering carbon aging mechanisms and offering an unprecedented, rapid diagnostic technique for capacitor-type materials.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"4 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149269155","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":"Current Density as a Critical Factor Governing the Cycle Life of Polysulfide-Based Redox Flow Batteries","authors":"Cheuk Yin Lee,Jiafeng Lei,Yi-Chun Lu","doi":"10.1021/acsenergylett.6c02652","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02652","url":null,"abstract":"Aqueous polysulfide redox flow batteries (RFBs) are promising for large-scale energy storage owing to their low cost and high safety. However, stable operation at high current density remains challenging for polysulfide RFBs (typically cycling below 40 mA cm–2), with the degradation mechanisms remaining poorly understood. Here, we identify current density as a critical factor governing the cycle life and elucidate sulfur deposition-induced degradation. Increasing current density simultaneously accelerates polysulfide crossover and promotes the formation of compact sulfur deposits, which block ion-transport pathways and lead to rapid cell failure. Based on this mechanistic understanding, a surfactant additive was employed to regulate sulfur nucleation and growth, extending the cycle life of polysulfide/ferrocyanide RFBs from 30 cycles to over 500 cycles at 60 mA cm–2. This work elucidates current density and sulfur morphology as critical factors governing polysulfide RFB degradation and provides design principles for durable, high-rate polysulfide-based RFBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"84 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149269115","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}
Zhiyu Wang,Yunzhou Lu,Mengxiao Li,Zhi Wei Javier Ang,Pengbo Zhang,Dao Gen Lek,Zhong Jin,Qing Wang
{"title":"Decoupled Water Electrolysis with an Air-Stable Zwitterionic Azo Mediator","authors":"Zhiyu Wang,Yunzhou Lu,Mengxiao Li,Zhi Wei Javier Ang,Pengbo Zhang,Dao Gen Lek,Zhong Jin,Qing Wang","doi":"10.1021/acsenergylett.6c02938","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02938","url":null,"abstract":"Decoupled water electrolysis (DWE) separates H2 and O2 evolution, improving safety and flexibility under intermittent renewable electricity, but requires durable, oxygen-tolerant redox mediators. Here we evaluate 4,4′-azo-bis(1-pyridinium-3-propane-sulfonate) (ABPS), a zwitterionic azo molecule, as an electron-coupled proton buffer for acidic DWE. Its azo/hydrazo core supports reversible two-electron/two-proton chemistry at 0.81 V vs RHE, while zwitterionic substituents provide high aqueous solubility and suppress crossover through low-cost sulfonated poly(ether ether ketone) membranes. Reduced H2ABPS shows no detectable oxidation after 90 days in air or during >5 h of continuous pure-O2 bubbling. Symmetric flow-cell cycling over 1000 h yields a capacity-fade rate below 1% year–1. With commercial catalysts at room temperature, decoupled flow cells reach 1.2 A cm–2 and operate for >200 h at 500 mA cm–2 with near-quantitative Faradaic efficiencies while producing high-purity H2 and O2. These results establish zwitterionic azo chemistry as an oxygen-tolerant, durable platform for high-rate decoupled hydrogen production.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"34 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149250874","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":"Microphase-Engineered Homologous Ion-Exchange Layers for High-Current-Density Bipolar Membrane Electrolysis","authors":"Jingjing Tu,Zongliang Wan,Xiaojiang Li,Fen Luo,Yiming Liang,Xian Liang,Cenfeng Fu,Jin Ran,Weisheng Yu,Liang Wu,Tongwen Xu","doi":"10.1021/acsenergylett.6c02765","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02765","url":null,"abstract":"Bipolar membranes (BPMs) maintain separated acidic and alkaline environments via water dissociation at the junction, but high-current-density operation remains challenging because rapid hydrated H+/OH– migration away from the junction must be coupled with sufficient water replenishment toward it. A transport imbalance between these opposing processes causes interfacial dehydration and limits long-term operation. Here, we develop microphase-engineered homologous ion-exchange layers to balance this coupled transport. These layers are fabricated from homologous multiblock poly(biphenyl alkylene) ionomers sharing a common backbone and block architecture, promoting interlayer compatibility and interconnected ionic domains. The hydrated pathways accelerate water replenishment and ion transport, thereby maintaining a stably hydrated junction. The resulting BPM enables pure-water electrolysis at 2.11 V at 1000 mA cm–2 and sustains high-purity hydrogen production for over 1100 h at 500 mA cm–2. This work establishes molecularly engineered ion-exchange layers as an effective approach for improving mass transport in high-current-density BPM systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"21 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149250875","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}