Catalyst lifetime is a primary technical bottleneck obstructing Cu-based CO2 reduction (CO2R), with restructuring via dissolution-redeposition being a commonly reported reason for selectivity loss. Here we examine how atomistic restructuring manifests at the microlevel of gas diffusion electrode (GDE)-based systems, ultimately compromising long-term CO2R performance. Using a flow-cell CO2R electrolyzer configuration and a copper-coated PTFE GDE, we first show how voltage gradients result in directional in-plane copper migration and porosity changes, causing a decrease in CO and ethylene production due to blocked catalyst pores. By the incorporation of different ionomer and inert carbon overlayers onto copper, we then demonstrate how in-plane degradation is mitigated by modulating the local pH and voltage homogeneity of the electrode, extending ethylene lifetimes by 10-fold. Ultimately, through-plane compaction of copper then becomes the limiting degradation pathway. Combined, these results provide rationale for the paradox of why copper degradation in membrane-electrode assemblies illustrates 100-fold greater stabilities than H-cell and flow-cell architecture.
{"title":"Role of the Copper Microstructure on Ethylene Stability during CO2 Electrolysis","authors":"Jesse Kok,Nikita Kolobov,Mohammed Sharah,Amirhossein Foroozan,Shayan Angizi,Konstantinos Dimitriou,Drew Higgins,Thomas Burdyny","doi":"10.1021/acsenergylett.6c00513","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00513","url":null,"abstract":"Catalyst lifetime is a primary technical bottleneck obstructing Cu-based CO2 reduction (CO2R), with restructuring via dissolution-redeposition being a commonly reported reason for selectivity loss. Here we examine how atomistic restructuring manifests at the microlevel of gas diffusion electrode (GDE)-based systems, ultimately compromising long-term CO2R performance. Using a flow-cell CO2R electrolyzer configuration and a copper-coated PTFE GDE, we first show how voltage gradients result in directional in-plane copper migration and porosity changes, causing a decrease in CO and ethylene production due to blocked catalyst pores. By the incorporation of different ionomer and inert carbon overlayers onto copper, we then demonstrate how in-plane degradation is mitigated by modulating the local pH and voltage homogeneity of the electrode, extending ethylene lifetimes by 10-fold. Ultimately, through-plane compaction of copper then becomes the limiting degradation pathway. Combined, these results provide rationale for the paradox of why copper degradation in membrane-electrode assemblies illustrates 100-fold greater stabilities than H-cell and flow-cell architecture.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"7 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147383839","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}
Solid polymer electrolytes are pivotal to safe, high-energy sodium–metal batteries but suffer from low ionic conductivity and poor interfacial stability. Here we pioneer a single-salt quasi-solid polymer electrolyte (PSDF) using NaDFOB, where dissolution is driven by interaction with C–O–C bonds rather than C═O groups. Together with succinonitrile-optimized solvation, PSDF achieves an ionic conductivity of 0.89 mS cm–1, a Na+ transference number of 0.58, and an oxidation potential of 5.1 V (vs Na+/Na). DFOB– preferentially forms B/F-rich interphases on both anode and cathode, enabling good interfacial stability. This allows the Na||PSDF||Na3V2(PO4)3 cell to retain 98.2% capacity after 3500 cycles, while operating effectively across a wide temperature range (−10 to 90 °C). Impressively, the cell respectively maintains 98 and 81.2% of its room-temperature capacity at 0 and −10 °C, and retains capacity retention >85% after 500 cycles at 80 and 90 °C. Besides, the Na||PSDF||Na3V2(PO4)3 pouch cells also show decent electrochemical performance and safety.
固体聚合物电解质是安全、高能钠金属电池的关键，但其离子电导率低，界面稳定性差。在这里，我们使用NaDFOB开拓了一种单盐准固体聚合物电解质（PSDF），其中溶解是由与C - O - C键而不是C = O基团的相互作用驱动的。通过丁二腈优化溶剂化，PSDF的离子电导率为0.89 mS cm-1， Na+转移数为0.58，氧化电位为5.1 V （vs Na+/Na）。DFOB -在阳极和阴极均优先形成富B/ f界面相，具有良好的界面稳定性。这使得Na||PSDF||Na3V2(PO4)3电池在3500次循环后保持98.2%的容量，同时在宽温度范围（- 10至90°C）内有效工作。令人印象深刻的是，电池在0°C和- 10°C下分别保持其室温容量的98%和81.2%，在80°C和90°C下循环500次后容量保持>85%。此外，Na||PSDF||Na3V2(PO4)3袋状电池也表现出良好的电化学性能和安全性。
{"title":"NaDFOB-Based Single-Salt Polymer Electrolyte for Long-Lifespan and Wide-Temperature Sodium–Metal Batteries","authors":"Jiaxuan Wang,Chunye Yang,Jing Wang,Xinping Ai,Yuliang Cao,Yongjin Fang","doi":"10.1021/acsenergylett.6c00051","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00051","url":null,"abstract":"Solid polymer electrolytes are pivotal to safe, high-energy sodium–metal batteries but suffer from low ionic conductivity and poor interfacial stability. Here we pioneer a single-salt quasi-solid polymer electrolyte (PSDF) using NaDFOB, where dissolution is driven by interaction with C–O–C bonds rather than C═O groups. Together with succinonitrile-optimized solvation, PSDF achieves an ionic conductivity of 0.89 mS cm–1, a Na+ transference number of 0.58, and an oxidation potential of 5.1 V (vs Na+/Na). DFOB– preferentially forms B/F-rich interphases on both anode and cathode, enabling good interfacial stability. This allows the Na||PSDF||Na3V2(PO4)3 cell to retain 98.2% capacity after 3500 cycles, while operating effectively across a wide temperature range (−10 to 90 °C). Impressively, the cell respectively maintains 98 and 81.2% of its room-temperature capacity at 0 and −10 °C, and retains capacity retention >85% after 500 cycles at 80 and 90 °C. Besides, the Na||PSDF||Na3V2(PO4)3 pouch cells also show decent electrochemical performance and safety.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"74 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147383840","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 : 2026-03-11DOI: 10.1021/acsenergylett.5c04139
Jason Pfeilsticker,Ethan Coleman,Theodore Krueger,Ankur Gupta,Wilson A. Smith
When designing a chemical process, the local balance of transport and kinetics, collectively referred to as the diffuse microenvironment, plays a critical role in performance but is difficult to directly observe. This work demonstrates a method of two-dimensional spatial chemical mapping of the diffuse microenvironment in the context of alkali metal hydroxide direct air capture of carbon dioxide using a custom operando gas-absorption flow cell along with confocal Raman spectroscopy. Notably, we observe the concentration boundary layer near the gas–liquid interface and elucidate the interplay of carbonate and bicarbonate ions within it while inferring local hydroxide depletion through continuum modeling. These first of their kind observations provide a technique to compare the performance of direct air capture solvents based on diffuse microenvironment dynamics while also providing metrics important for air contactor design such as boundary layer thickness. Overall, this work showcases a new experimental platform to study interfacial diffuse microenvironments in and outside of the field of direct air capture of carbon dioxide.
{"title":"Spatially Mapping the CO2 Alkaline Sorbent Diffuse Microenvironment Using Operando Raman Spectroscopy","authors":"Jason Pfeilsticker,Ethan Coleman,Theodore Krueger,Ankur Gupta,Wilson A. Smith","doi":"10.1021/acsenergylett.5c04139","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04139","url":null,"abstract":"When designing a chemical process, the local balance of transport and kinetics, collectively referred to as the diffuse microenvironment, plays a critical role in performance but is difficult to directly observe. This work demonstrates a method of two-dimensional spatial chemical mapping of the diffuse microenvironment in the context of alkali metal hydroxide direct air capture of carbon dioxide using a custom operando gas-absorption flow cell along with confocal Raman spectroscopy. Notably, we observe the concentration boundary layer near the gas–liquid interface and elucidate the interplay of carbonate and bicarbonate ions within it while inferring local hydroxide depletion through continuum modeling. These first of their kind observations provide a technique to compare the performance of direct air capture solvents based on diffuse microenvironment dynamics while also providing metrics important for air contactor design such as boundary layer thickness. Overall, this work showcases a new experimental platform to study interfacial diffuse microenvironments in and outside of the field of direct air capture of carbon dioxide.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"47 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147383842","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}
During the development of perovskite–silicon tandem solar cells, the impact of transport layers of perovskite top cells on the short-circuit current density (JSC) has rarely been considered. Here, we report ultrathin electron-selective contacts as new architectures of electron transport layers (ETLs) by decreasing the C60 thickness to 1 nm, where the carrier collection efficiency is proven to be independent of C60 thickness with tin oxide as a buffer layer. Benefiting from the lowest C60 parasitic absorption, the JSC in the tandem device with ultrathin C60 is enhanced by 0.24 mA/cm2. Moreover, to recover the damage from atomic layer deposition on uncovered perovskite surface, we use poly(methyl methacrylate) (PMMA) as a protective layer. Combining ultrathin C60 and PMMA protective layer, an efficiency of 31.70% is finally achieved in tandem solar cells. These findings demonstrate the feasibility of ultrathin ETLs or ETL-free designs for perovskite–silicon tandem solar cells.
{"title":"Impact of Ultrathin Electron-Selective Contacts on Perovskite–Silicon Tandem Solar Cells","authors":"Gaosheng Huang,Nan Sun,Niklas Scheer,Samah Akel,Qing Yang,Benjamin Klingebiel,Karsten Bittkau,Andreas Lambertz,Rüdiger-A. Eichel,Florian Hausen,Thomas Kirchartz,Uwe Rau,Kaining Ding","doi":"10.1021/acsenergylett.5c04082","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04082","url":null,"abstract":"During the development of perovskite–silicon tandem solar cells, the impact of transport layers of perovskite top cells on the short-circuit current density (JSC) has rarely been considered. Here, we report ultrathin electron-selective contacts as new architectures of electron transport layers (ETLs) by decreasing the C60 thickness to 1 nm, where the carrier collection efficiency is proven to be independent of C60 thickness with tin oxide as a buffer layer. Benefiting from the lowest C60 parasitic absorption, the JSC in the tandem device with ultrathin C60 is enhanced by 0.24 mA/cm2. Moreover, to recover the damage from atomic layer deposition on uncovered perovskite surface, we use poly(methyl methacrylate) (PMMA) as a protective layer. Combining ultrathin C60 and PMMA protective layer, an efficiency of 31.70% is finally achieved in tandem solar cells. These findings demonstrate the feasibility of ultrathin ETLs or ETL-free designs for perovskite–silicon tandem solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"6 10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147383844","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 : 2026-03-10DOI: 10.1021/acsenergylett.6c00321
Animesh Dutta,Kan Homlamai,Jeffin James Abraham,Thitiphum Sangsanit,Andrew O’Brien,Yixiang Zhang,Michel Johnson,Eytan Mendel-Elias,Montree Sawangphruk,J. R. Dahn
To achieve high energy density in medium-nickel-layered oxide (NMC) cathodes, the most straightforward approach is to increase the upper cutoff voltage. However, this reduces the cycle life due to enhanced electrolyte oxidation. Many coating elements have been introduced to improve the lifetime, and tungsten (W) is a common vendor choice. We find that surface tungsten compounds dissolve during electrochemical cycling, with the rate increasing at higher cutoff voltages. X-ray photoelectron spectroscopy (XPS) confirms W deposition in the form of metallic W and tungsten oxides on the graphite negative electrode, and X-ray fluorescence (XRF) quantified W content. Surprisingly, a significant amount of W dissolves under high-voltage operation, a problem that becomes more severe because vendors generally employ only trace amounts of coating, which leaves the surface increasingly exposed as the coatings dissolve. This work also investigates the impact of deposited W on the lithiated graphite negative electrode through simulated storage experiments.
{"title":"Fate of Tungsten-Coated NMC Cathodes in Li-Ion Cells","authors":"Animesh Dutta,Kan Homlamai,Jeffin James Abraham,Thitiphum Sangsanit,Andrew O’Brien,Yixiang Zhang,Michel Johnson,Eytan Mendel-Elias,Montree Sawangphruk,J. R. Dahn","doi":"10.1021/acsenergylett.6c00321","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00321","url":null,"abstract":"To achieve high energy density in medium-nickel-layered oxide (NMC) cathodes, the most straightforward approach is to increase the upper cutoff voltage. However, this reduces the cycle life due to enhanced electrolyte oxidation. Many coating elements have been introduced to improve the lifetime, and tungsten (W) is a common vendor choice. We find that surface tungsten compounds dissolve during electrochemical cycling, with the rate increasing at higher cutoff voltages. X-ray photoelectron spectroscopy (XPS) confirms W deposition in the form of metallic W and tungsten oxides on the graphite negative electrode, and X-ray fluorescence (XRF) quantified W content. Surprisingly, a significant amount of W dissolves under high-voltage operation, a problem that becomes more severe because vendors generally employ only trace amounts of coating, which leaves the surface increasingly exposed as the coatings dissolve. This work also investigates the impact of deposited W on the lithiated graphite negative electrode through simulated storage experiments.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"45 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147383843","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}
Chromogenic materials that can reversibly change their body color in response to external stimuli are attracting intense interest for advanced sensing, smart buildings, and optical information storage. Photochromic materials are one of the most important chromogenic materials, but their application is greatly limited by an insufficient color-changing rate and unclear mechanism. Herein, we report an electrophotochromic effect in NaNbO3:Pr3+ ceramics, which can synergize the electric-field-driven and light-induced structural changes in the same material to yield more stable color changes. This synergistic mechanism resulted in an ∼87% enhancement in the maximum reflectance difference (ΔR) at 542 nm, compared with photochromism alone. Systematic studies indicate that the electrophotochromism arises from polarization-driven migration and surface accumulation of charge carriers, along with the resulting built-in electric field. Due to the excellent chromogenic responsiveness to light, electricity, and heat, we demonstrate applications of the NaNbO3:Pr3+ ceramics in temperature–time indicators, showing the advantages of integration between real-time visual and delayed quantitative sensing. This work not only reveals the physical mechanism underlying color-changing behavior but also provides a new approach for designing stimulus-responsive materials.
{"title":"Built-in Electric-Field-Induced Electrophotochromism in NaNbO3:Pr3+ Ceramics toward Dual-Mode Time–Temperature Sensing","authors":"Yu-Chen Ao,Rujun Yang,Shu-Juan Zhao,Yuantian Zheng,Ge-Mei Cai,Yixi Zhuang,Rong-Jun Xie","doi":"10.1021/acsenergylett.5c04242","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04242","url":null,"abstract":"Chromogenic materials that can reversibly change their body color in response to external stimuli are attracting intense interest for advanced sensing, smart buildings, and optical information storage. Photochromic materials are one of the most important chromogenic materials, but their application is greatly limited by an insufficient color-changing rate and unclear mechanism. Herein, we report an electrophotochromic effect in NaNbO3:Pr3+ ceramics, which can synergize the electric-field-driven and light-induced structural changes in the same material to yield more stable color changes. This synergistic mechanism resulted in an ∼87% enhancement in the maximum reflectance difference (ΔR) at 542 nm, compared with photochromism alone. Systematic studies indicate that the electrophotochromism arises from polarization-driven migration and surface accumulation of charge carriers, along with the resulting built-in electric field. Due to the excellent chromogenic responsiveness to light, electricity, and heat, we demonstrate applications of the NaNbO3:Pr3+ ceramics in temperature–time indicators, showing the advantages of integration between real-time visual and delayed quantitative sensing. This work not only reveals the physical mechanism underlying color-changing behavior but also provides a new approach for designing stimulus-responsive materials.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"54 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147383845","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 : 2026-03-09DOI: 10.1021/acsenergylett.5c03584
Si Zhao, Yuhang Li, Kaiyue Feng, Bingyan Wang, Mingjie Wang, Hong Li, Lituo Zheng, Mingdeng Wei, Zhensheng Hong
Hard carbon (HC) anode based solid-state sodium-ion batteries (SSIBs) possess highly intrinsic safety and cost effectiveness in the application of large-scale energy storage. However, it is hindered by large interfacial impedance and sluggish Na+ transport kinetics from the solid–solid electrode contact. Here, we propose an electrochemical presodiation strategy to in situ form a thin, uniform, and inorganic-rich (NaF/Na2O) solid-electrolyte interphase (SEI) on the HC anode. Such an SEI layer provides stable and good contact, leading to markedly reduced charge-transfer resistance and robust Na+ transport in a polymer-based solid electrolyte. The evidence for reversible Na+ insertion/extraction in the HC anode for SSIBs was first revealed by in situ X-ray diffraction. Consequently, the presodiated HC-based half-cell exhibits a reversible capacity of 275.2 mAh·g–1 and good cycling stability with 90.9% retention after 100 cycles at 0.1 C. Finally, the presodiated HC-based SSIBs were constructed with the Na3V2(PO4)3 cathode, delivering a high capacity of 106.9 mAh·g–1 at 0.1 C and good cycling stability without external pressure. These findings highlight inorganic engineering of the SEI as a powerful strategy for boosting interfacial kinetics toward regular pressure HC anode-based SSIBs.
{"title":"Presodiated Hard Carbon Anode with an Inorganic-Rich Interphase for Solid-State Sodium Batteries","authors":"Si Zhao, Yuhang Li, Kaiyue Feng, Bingyan Wang, Mingjie Wang, Hong Li, Lituo Zheng, Mingdeng Wei, Zhensheng Hong","doi":"10.1021/acsenergylett.5c03584","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03584","url":null,"abstract":"Hard carbon (HC) anode based solid-state sodium-ion batteries (SSIBs) possess highly intrinsic safety and cost effectiveness in the application of large-scale energy storage. However, it is hindered by large interfacial impedance and sluggish Na<sup>+</sup> transport kinetics from the solid–solid electrode contact. Here, we propose an electrochemical presodiation strategy to in situ form a thin, uniform, and inorganic-rich (NaF/Na<sub>2</sub>O) solid-electrolyte interphase (SEI) on the HC anode. Such an SEI layer provides stable and good contact, leading to markedly reduced charge-transfer resistance and robust Na<sup>+</sup> transport in a polymer-based solid electrolyte. The evidence for reversible Na<sup>+</sup> insertion/extraction in the HC anode for SSIBs was first revealed by in situ X-ray diffraction. Consequently, the presodiated HC-based half-cell exhibits a reversible capacity of 275.2 mAh·g<sup>–1</sup> and good cycling stability with 90.9% retention after 100 cycles at 0.1 C. Finally, the presodiated HC-based SSIBs were constructed with the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode, delivering a high capacity of 106.9 mAh·g<sup>–1</sup> at 0.1 C and good cycling stability without external pressure. These findings highlight inorganic engineering of the SEI as a powerful strategy for boosting interfacial kinetics toward regular pressure HC anode-based SSIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"44 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147381092","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The deployment of aqueous zinc batteries in next-generation energy storage is hindered by interfacial instability of the zinc anode, closely linked to the spatiotemporal evolution of interfacial chemical fields. Herein, an in-situ 3D pH visualization platform directly reveals a spontaneous and persistent gravity-aligned pH gradient at the zinc-electrolyte interface, reaching ∼0.6 between the upper and lower regions. Coupled multiphysics simulations show that electrochemically induced electrolyte density stratification drives natural convection, dominating ion and proton transport and sustaining pH and Zn2+ gradients. The resulting vertical chemical stratification spatially decouples interfacial reactions, leading to directional zinc redistribution. As a proof of concept, suppressing convection using a mixed-salt electrolyte homogenizes the interfacial pH (ΔpH < 0.1) and extends the cycling lifetime of symmetric zinc batteries by over 75%. This work reveals a gravity-coupled mechanism governing interfacial chemical field evolution, providing general physical principles for stabilizing aqueous metal anodes.
{"title":"Three-Dimensional Visualization of Chemical Stratification and Pathological Redistribution in Aqueous Zinc Batteries","authors":"Zhongxi Zhao, Yongtang Chen, Yongfu Liu, Jiangfeng Huang, Junshuo Lian, Yaoming Leng, Peng Tan","doi":"10.1021/acsenergylett.6c00171","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00171","url":null,"abstract":"The deployment of aqueous zinc batteries in next-generation energy storage is hindered by interfacial instability of the zinc anode, closely linked to the spatiotemporal evolution of interfacial chemical fields. Herein, an in-situ 3D pH visualization platform directly reveals a spontaneous and persistent gravity-aligned pH gradient at the zinc-electrolyte interface, reaching ∼0.6 between the upper and lower regions. Coupled multiphysics simulations show that electrochemically induced electrolyte density stratification drives natural convection, dominating ion and proton transport and sustaining pH and Zn<sup>2+</sup> gradients. The resulting vertical chemical stratification spatially decouples interfacial reactions, leading to directional zinc redistribution. As a proof of concept, suppressing convection using a mixed-salt electrolyte homogenizes the interfacial pH (ΔpH < 0.1) and extends the cycling lifetime of symmetric zinc batteries by over 75%. This work reveals a gravity-coupled mechanism governing interfacial chemical field evolution, providing general physical principles for stabilizing aqueous metal anodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"137 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147380779","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 : 2026-03-06DOI: 10.1021/acsenergylett.5c04161
Robin Schot, Imme Schuringa, Álvaro Rodríguez Echarri, Lars Sonneveld, Tom Veeken, Yang Lu, Samuel D. Stranks, Albert Polman, Bruno Ehrler, Saskia Fiedler
Halide perovskite semiconductors are promising materials for high-efficiency solar cells. Their optical properties can vary within and between crystallographic grains. We present spatially resolved cathodoluminescence (CL) spectroscopy at 2 and 5 keV on polycrystalline CsPbBr3 perovskite films to study these variations at the nanoscale. The CL maps show a strongly reduced intensity near the polycrystalline grain boundaries. We perform numerical simulations of the far-field emission of the electron beam-generated optical near fields by using the surface profiles from AFM as input. We find that near grain boundaries the light outcoupling is strongly reduced due to enhanced internal reflection and light trapping at the curved surfaces. Lateral variations in CL intensity inside grains are due to Fabry–Pérot-like resonances in the film, with the substrate acting as a back reflector. Our results show that near-field coupling and interference effects can dominate nanoscale luminescence maps of halide perovskite films. The results are broadly relevant for the analysis of CL and the photoluminescence of corrugated thin films.
{"title":"Near-Field Effects on Cathodoluminescence Outcoupling in Perovskite Thin Films","authors":"Robin Schot, Imme Schuringa, Álvaro Rodríguez Echarri, Lars Sonneveld, Tom Veeken, Yang Lu, Samuel D. Stranks, Albert Polman, Bruno Ehrler, Saskia Fiedler","doi":"10.1021/acsenergylett.5c04161","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04161","url":null,"abstract":"Halide perovskite semiconductors are promising materials for high-efficiency solar cells. Their optical properties can vary within and between crystallographic grains. We present spatially resolved cathodoluminescence (CL) spectroscopy at 2 and 5 keV on polycrystalline CsPbBr<sub>3</sub> perovskite films to study these variations at the nanoscale. The CL maps show a strongly reduced intensity near the polycrystalline grain boundaries. We perform numerical simulations of the far-field emission of the electron beam-generated optical near fields by using the surface profiles from AFM as input. We find that near grain boundaries the light outcoupling is strongly reduced due to enhanced internal reflection and light trapping at the curved surfaces. Lateral variations in CL intensity inside grains are due to Fabry–Pérot-like resonances in the film, with the substrate acting as a back reflector. Our results show that near-field coupling and interference effects can dominate nanoscale luminescence maps of halide perovskite films. The results are broadly relevant for the analysis of CL and the photoluminescence of corrugated thin films.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147359733","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 : 2026-03-06DOI: 10.1021/acsenergylett.6c00423
Marieke S. van Leeuwen, Philippe M. Vereecken
The integration of CO2 sorbents into electrochemical CO2 reduction (CO2RR) systems is often proposed as a strategy to enhance the local CO2 availability and improve the process efficiency. However, a critical analysis of recent literature reveals that many implementations fall short of their theoretical potential. This Perspective highlights the conceptual and experimental pitfalls in current sorbent-augmented CO2RR research, showing that performance gains are frequently limited by system-level constraints rather than sorbent properties. By benchmarking reported partial current densities against diffusion-limited theoretical maxima, we demonstrate that sorbent integration is rarely the true performance-limiting factor. We argue that future work must prioritize rigorous benchmarking, clearer mechanistic hypotheses, and system-aware design to unlock the full potential of integrated CO2 capture and conversion.
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