Pub Date : 2026-02-01DOI: 10.1021/acsenergylett.5c03844
Ping-Han Wu, T. Alan Hatton, Hyowon Seo
Pulsed chronopotentiometry lowers cell voltage and energy input in aqueous Neutral Red-mediated electrochemical CO2 capture. A pulse–reverse current (PRC) protocol provides a tunable operating mode that enables efficient control of polarization while preserving carbon capture performance. By adjustment of the pulse amplitude, duration, and duty cycle, PRC stabilizes the cell voltage and reduces energy consumption relative to direct-current (DC) operation at matched current density. Mechanistically, PRC regulates diffusion-layer dynamics by maintaining a thin, pulsation-controlled inner layer while periodically refreshing the outer layer, thereby suppressing concentration polarization and parasitic side reactions. Timing the on-period to Sand’s transition time preserves favorable near-surface Neutral Red/leuco-Neutral Red (NR/NRH2) concentrations without increasing solution flow. These results demonstrate that PRC can match or outperform DC operation through parameter optimization and offers a scalable, energy-efficient strategy compatible with diverse electrochemical reactor architectures.
{"title":"Pulsed Chronopotentiometry for Electrochemical CO2 Capture with Molecular Redox Mediators","authors":"Ping-Han Wu, T. Alan Hatton, Hyowon Seo","doi":"10.1021/acsenergylett.5c03844","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03844","url":null,"abstract":"Pulsed chronopotentiometry lowers cell voltage and energy input in aqueous Neutral Red-mediated electrochemical CO<sub>2</sub> capture. A pulse–reverse current (PRC) protocol provides a tunable operating mode that enables efficient control of polarization while preserving carbon capture performance. By adjustment of the pulse amplitude, duration, and duty cycle, PRC stabilizes the cell voltage and reduces energy consumption relative to direct-current (DC) operation at matched current density. Mechanistically, PRC regulates diffusion-layer dynamics by maintaining a thin, pulsation-controlled inner layer while periodically refreshing the outer layer, thereby suppressing concentration polarization and parasitic side reactions. Timing the on-period to Sand’s transition time preserves favorable near-surface Neutral Red/leuco-Neutral Red (NR/NRH<sub>2</sub>) concentrations without increasing solution flow. These results demonstrate that PRC can match or outperform DC operation through parameter optimization and offers a scalable, energy-efficient strategy compatible with diverse electrochemical reactor architectures.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"24 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097852","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-31DOI: 10.1021/acsenergylett.5c03875
Isabella Taupitz, Dorothee Menzel, Maxim Simmonds, Huagui Lai, Philippe Holzhey, Maximilian Hübner, Sebastian Berwig, Yeonghun Yun, Fan Fu, Eva Unger, Lars Korte, Philipp Tockhorn, Steve Albrecht
Self-assembling molecules (SAMs) are investigated as an alternative hole-transport layer to PEDOT:PSS for tin–lead (Sn–Pb) narrow-band gap (NBG) perovskite solar cells. Here we report on an unintended effect of the additive lead(II)-thiocyanate (Pb(SCN)2) in SAM-based NBG perovskite solar cells. Upon an increase in the amount of Pb(SCN)2, SAM-based layer stacks exhibit better film properties. Photoconversion efficiency reaches 18.5% for a concentration of 1% Pb(SCN)2 and declines drastically for higher concentrations. Time-resolved photoluminescence and surface photovoltage measurements show that carrier extraction is impeded in Pb(SCN)2-containing layer stacks with >1% Pb(SCN)2, and photoelectron spectroscopy reveals the unintended appearance of SAMs on the top surface of the perovskite layer. Relocated SAMs can be removed by solvent washing of the perovskite surface, recovering electron extraction but not the solar cell performance. This study highlights that commonly used additives must be adapted accordingly when introducing SAMs to NBG solar cells.
{"title":"Unintended Additive-Mediated Relocation of Self-Assembling Molecules Limits Charge Extraction in Sn–Pb-Based Perovskite Solar Cells","authors":"Isabella Taupitz, Dorothee Menzel, Maxim Simmonds, Huagui Lai, Philippe Holzhey, Maximilian Hübner, Sebastian Berwig, Yeonghun Yun, Fan Fu, Eva Unger, Lars Korte, Philipp Tockhorn, Steve Albrecht","doi":"10.1021/acsenergylett.5c03875","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03875","url":null,"abstract":"Self-assembling molecules (SAMs) are investigated as an alternative hole-transport layer to PEDOT:PSS for tin–lead (Sn–Pb) narrow-band gap (NBG) perovskite solar cells. Here we report on an unintended effect of the additive lead(II)-thiocyanate (Pb(SCN)<sub>2</sub>) in SAM-based NBG perovskite solar cells. Upon an increase in the amount of Pb(SCN)<sub>2</sub>, SAM-based layer stacks exhibit better film properties. Photoconversion efficiency reaches 18.5% for a concentration of 1% Pb(SCN)<sub>2</sub> and declines drastically for higher concentrations. Time-resolved photoluminescence and surface photovoltage measurements show that carrier extraction is impeded in Pb(SCN)<sub>2</sub>-containing layer stacks with >1% Pb(SCN)<sub>2</sub>, and photoelectron spectroscopy reveals the unintended appearance of SAMs on the top surface of the perovskite layer. Relocated SAMs can be removed by solvent washing of the perovskite surface, recovering electron extraction but not the solar cell performance. This study highlights that commonly used additives must be adapted accordingly when introducing SAMs to NBG solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"82 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097853","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-31DOI: 10.1021/acsenergylett.5c03511
Grace Wei, Luca Binci, Gerbrand Ceder
Sodium-ion solid electrolytes offer a sustainable route toward next-generation batteries, but few match the performance of their lithium counterparts. Halide-based NaMOCl4 (M = Nb, Ta) has recently emerged as a promising analogue to LiMOCl4, yet its structure–transport relationships remain unclear due to poor crystallinity in experiments. Here, we combine density functional theory and machine-learned molecular dynamics to reveal that crystalline NaMOCl4 exhibits negligible room-temperature conductivity with high activation barriers arising from vacancy-mediated diffusion below an order–disorder transition. Above this transition, rotational and translational motion of the [MO2/2Cl4–]∞ chains create new Na sites and enhances transport. In contrast, the amorphous phase inherently supports facile, three-dimensional Na diffusion through dynamic framework flexibility. These results show that ordered crystalline phases hinder ionic transport, while disorder – either thermally induced or structural – facilitates it, revising prior assumptions from the Li system and providing design principles for high-conductivity Na halide electrolytes.
{"title":"Microscopic Mechanisms of Superionic Na-ion Conductivity in Crystalline and Amorphous NaMOCl4 (M = Nb, Ta) Solid Electrolytes","authors":"Grace Wei, Luca Binci, Gerbrand Ceder","doi":"10.1021/acsenergylett.5c03511","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03511","url":null,"abstract":"Sodium-ion solid electrolytes offer a sustainable route toward next-generation batteries, but few match the performance of their lithium counterparts. Halide-based NaMOCl<sub>4</sub> (M = Nb, Ta) has recently emerged as a promising analogue to LiMOCl<sub>4</sub>, yet its structure–transport relationships remain unclear due to poor crystallinity in experiments. Here, we combine density functional theory and machine-learned molecular dynamics to reveal that crystalline NaMOCl<sub>4</sub> exhibits negligible room-temperature conductivity with high activation barriers arising from vacancy-mediated diffusion below an order–disorder transition. Above this transition, rotational and translational motion of the [MO<sub>2/2</sub>Cl<sub>4</sub><sup>–</sup>]<sub>∞</sub> chains create new Na sites and enhances transport. In contrast, the amorphous phase inherently supports facile, three-dimensional Na diffusion through dynamic framework flexibility. These results show that ordered crystalline phases hinder ionic transport, while disorder – either thermally induced or structural – facilitates it, revising prior assumptions from the Li system and providing design principles for high-conductivity Na halide electrolytes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"8 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097829","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-30DOI: 10.1021/acsenergylett.5c02607
Longlong Wang, Bingkun Hu, Christopher Doerrer, Shengming Zhang, Lechen Yang, Liquan Pi, Max Jenkins, Boyang Liu, Shengda D. Pu, Yi Yuan, Hui Gao, Alex W. Robertson, Patrick S. Grant, Xiangwen Gao, Peter G. Bruce
Sulfide solid electrolytes have high ionic conductivities necessary to achieve high-rate solid-state cathodes at room temperature and low pressure. Cathode active materials generally require coatings to avoid deleterious oxidative decomposition reactions with the electrolyte. Coatings add cost and complexity to the manufacture. Here we decouple the effect of double and triple phase boundaries on the decomposition in the thick (i.e., ∼110 μm) uncoated solid state cathode. We show that more severe oxidative decomposition of solid electrolytes occurs when the cathode active materials, carbon, and the solid electrolyte coexist, highlighting the importance of the triple phase boundary concerning the decomposition. By regulating the electronic pathways at the triple phase boundary, a thick uncoated electrode at 1 mA cm–2 and 2 MPa stack pressure, delivers an initial areal capacity of ∼4.6 mAh cm–2 at 30 °C and ∼85% capacity retention after 500 cycles.
硫化物固体电解质具有高离子电导率，是在室温和低压下实现高速率固态阴极所必需的。阴极活性材料通常要求涂层避免与电解质发生有害的氧化分解反应。涂料增加了制造成本和复杂性。在这里，我们解耦了双相和三相边界对厚（即~ 110 μm）无涂层固态阴极分解的影响。我们发现，当阴极活性材料、碳和固体电解质共存时，固体电解质发生更严重的氧化分解，突出了三相边界对分解的重要性。通过调节三相边界的电子路径，在1 mA cm-2和2 MPa堆叠压力下，厚的无涂层电极在30°C下提供约4.6 mAh cm-2的初始面积容量，500次循环后容量保持约85%。
{"title":"Understanding the Role of Triple Phase Boundaries on Coating-Free Solid-State Cathodes","authors":"Longlong Wang, Bingkun Hu, Christopher Doerrer, Shengming Zhang, Lechen Yang, Liquan Pi, Max Jenkins, Boyang Liu, Shengda D. Pu, Yi Yuan, Hui Gao, Alex W. Robertson, Patrick S. Grant, Xiangwen Gao, Peter G. Bruce","doi":"10.1021/acsenergylett.5c02607","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c02607","url":null,"abstract":"Sulfide solid electrolytes have high ionic conductivities necessary to achieve high-rate solid-state cathodes at room temperature and low pressure. Cathode active materials generally require coatings to avoid deleterious oxidative decomposition reactions with the electrolyte. Coatings add cost and complexity to the manufacture. Here we decouple the effect of double and triple phase boundaries on the decomposition in the thick (i.e., ∼110 μm) uncoated solid state cathode. We show that more severe oxidative decomposition of solid electrolytes occurs when the cathode active materials, carbon, and the solid electrolyte coexist, highlighting the importance of the triple phase boundary concerning the decomposition. By regulating the electronic pathways at the triple phase boundary, a thick uncoated electrode at 1 mA cm<sup>–2</sup> and 2 MPa stack pressure, delivers an initial areal capacity of ∼4.6 mAh cm<sup>–2</sup> at 30 °C and ∼85% capacity retention after 500 cycles.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"93 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-30DOI: 10.1021/acsenergylett.5c04035
Miguel Torre Cachafeiro, Carys A. Worsley, Fuxiang Ji, Trystan M. Watson, Wolfgang Tress
The most typical hysteresis in the current density–voltage (J–V) curve of perovskite solar cells (PSCs) shows better performance in the backward (BW) than in the forward (FW) voltage scan (normal hysteresis). The opposite, where the FW scan yields higher photocurrent, is known as inverted hysteresis and is also frequently observed. Here, we examine PSCs exhibiting both normal and inverted hysteresis, depending on scan rate and preconditioning. Spectral changes in the external quantum efficiency (EQE) linked to ionic redistribution reveal that inverted hysteresis arises from blue-range photocurrent losses caused by enhanced recombination at the interfaces due to ionic accumulation. This trend is consistent across PSC architectures, as demonstrated for triple mesoscopic carbon-based (C-PSCs) and planar p-i-n devices. Combined with drift-diffusion simulations, the results show that ionic losses can be bidirectional, and the hysteresis direction depends on how the ionic distribution impacts charge collection efficiency.
{"title":"Inverted J–V Hysteresis in Perovskite Solar Cells: Insights from Photovoltaic Quantum Efficiency","authors":"Miguel Torre Cachafeiro, Carys A. Worsley, Fuxiang Ji, Trystan M. Watson, Wolfgang Tress","doi":"10.1021/acsenergylett.5c04035","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04035","url":null,"abstract":"The most typical hysteresis in the current density–voltage (<i>J</i>–<i>V</i>) curve of perovskite solar cells (PSCs) shows better performance in the backward (BW) than in the forward (FW) voltage scan (normal hysteresis). The opposite, where the FW scan yields higher photocurrent, is known as inverted hysteresis and is also frequently observed. Here, we examine PSCs exhibiting both normal and inverted hysteresis, depending on scan rate and preconditioning. Spectral changes in the external quantum efficiency (EQE) linked to ionic redistribution reveal that inverted hysteresis arises from blue-range photocurrent losses caused by enhanced recombination at the interfaces due to ionic accumulation. This trend is consistent across PSC architectures, as demonstrated for triple mesoscopic carbon-based (C-PSCs) and planar p-i-n devices. Combined with drift-diffusion simulations, the results show that ionic losses can be bidirectional, and the hysteresis direction depends on how the ionic distribution impacts charge collection efficiency.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"8 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-30DOI: 10.1021/acsenergylett.5c04221
Erwin Hüger, Jochen Stahn, Harald Schmidt
The reversible incorporation of lithium into electrodes is a key process in energy storage in Li-ion batteries. A detailed understanding of lithiation and delithiation mechanisms acting in electrodes is therefore essential for both fundamental and application-oriented research. We introduce an approach that combines isotope multilayer electrodes with neutron reflectometry to directly probe the lithiation mechanism in operando during electrochemical cycling. The core idea is that the isotope multilayer transforms complex reflectivity patterns into simpler patterns characterized by a single, well-defined Bragg peak. The evolution of the peak (scattering vector position and intensity) as a function of state-of-charge provides a signature of the underlying mechanism. This drastically simplifies data analysis and, in some cases, makes it possible at all. Proof-of-concept experiments on 73Ge/Ge multilayer electrodes demonstrate the effectiveness of the method. A direct and easy comparison between experimental results and simulations indicates a homogeneous lithiation and delithiation mechanism, independent of cycle number and cycling rate.
{"title":"Identification of Lithiation Mechanisms in Li-Ion Batteries: Multilayer Electrodes and Neutron Reflectometry","authors":"Erwin Hüger, Jochen Stahn, Harald Schmidt","doi":"10.1021/acsenergylett.5c04221","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04221","url":null,"abstract":"The reversible incorporation of lithium into electrodes is a key process in energy storage in Li-ion batteries. A detailed understanding of lithiation and delithiation mechanisms acting in electrodes is therefore essential for both fundamental and application-oriented research. We introduce an approach that combines isotope multilayer electrodes with neutron reflectometry to directly probe the lithiation mechanism <i>in operando</i> during electrochemical cycling. The core idea is that the isotope multilayer transforms complex reflectivity patterns into simpler patterns characterized by a single, well-defined Bragg peak. The evolution of the peak (scattering vector position and intensity) as a function of state-of-charge provides a signature of the underlying mechanism. This drastically simplifies data analysis and, in some cases, makes it possible at all. Proof-of-concept experiments on <sup>73</sup>Ge/Ge multilayer electrodes demonstrate the effectiveness of the method. A direct and easy comparison between experimental results and simulations indicates a homogeneous lithiation and delithiation mechanism, independent of cycle number and cycling rate.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"91 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097854","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-30DOI: 10.1021/acsenergylett.5c03829
Piyush Kumar Verma, Charles C. L. McCrory
The electrochemical reactive capture of CO2 (e-RCC) process, in which the capture of CO2 from industrial point sources is integrated with electrochemical conversion into valuable fuels and chemical feedstocks, is an ambitious technological frontier in energy science and industrial waste upcycling. We present an e-RCC system to capture and convert CO2 to CO using amines as sorbents and molecular cobalt electrocatalysts with pyridyldiimine-based ligands. Sparging dilute CO2 through water/acetonitrile electrolyte solutions containing n-butylamine and the cobalt catalyst enables the electroreduction of CO2 with enhanced activity and selectivity. Even at flue-gas concentrations of CO2 (5% v/v CO2, balance N2), the presence of n-butylamine in the electrolyte enables the reduction of CO2 to CO with 3-fold higher activity (TOFcat ∼3.3 × 104 s–1) compared to the catalyst system without amine. This study serves as a proof of concept for direct electrochemical reduction of CO2 from dilute streams using an amine-based e-RCC process.
{"title":"Electrochemical Reactive Capture of Carbon Dioxide Using an Amine Sorbent and a Homogeneous Cobalt Electrocatalyst","authors":"Piyush Kumar Verma, Charles C. L. McCrory","doi":"10.1021/acsenergylett.5c03829","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03829","url":null,"abstract":"The electrochemical reactive capture of CO<sub>2</sub> (<i>e</i>-RCC) process, in which the capture of CO<sub>2</sub> from industrial point sources is integrated with electrochemical conversion into valuable fuels and chemical feedstocks, is an ambitious technological frontier in energy science and industrial waste upcycling. We present an <i>e</i>-RCC system to capture and convert CO<sub>2</sub> to CO using amines as sorbents and molecular cobalt electrocatalysts with pyridyldiimine-based ligands. Sparging dilute CO<sub>2</sub> through water/acetonitrile electrolyte solutions containing <i>n</i>-butylamine and the cobalt catalyst enables the electroreduction of CO<sub>2</sub> with enhanced activity and selectivity. Even at flue-gas concentrations of CO<sub>2</sub> (5% v/v CO<sub>2</sub>, balance N<sub>2</sub>), the presence of <i>n</i>-butylamine in the electrolyte enables the reduction of CO<sub>2</sub> to CO with 3-fold higher activity (TOF<sub>cat</sub> ∼3.3 × 10<sup>4</sup> s<sup>–1</sup>) compared to the catalyst system without amine. This study serves as a proof of concept for direct electrochemical reduction of CO<sub>2</sub> from dilute streams using an amine-based <i>e</i>-RCC process.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"75 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072431","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-29DOI: 10.1021/acsenergylett.5c03205
Zhuo Li, Daren Wu, Simon Si Ming Ji, Ana G. Claus, Hui Zhong, Sanjit K. Ghose, Kelsey B. Hatzell
This study investigates lithium plating texture in anode-free solid-state batteries using synchrotron-based X-ray diffraction. Conventional methods are limited by lithium’s low electron density and softness, which hinders direct interrogation in anode-free solid-state batteries. Results reveal that lithium plating texture is influenced by temperature and current density. Under mild conditions, lithium exhibited a ⟨110⟩ fiber texture. However, higher current densities and elevated temperatures led to a more randomized orientation, suggesting a dependence on plating conditions. The results highlight how the operating and processing conditions for lithium metal can influence the texture of lithium metal and reversible operation.
{"title":"Texture Evolution of Plated Lithium in Anode-Free Solid-State Batteries","authors":"Zhuo Li, Daren Wu, Simon Si Ming Ji, Ana G. Claus, Hui Zhong, Sanjit K. Ghose, Kelsey B. Hatzell","doi":"10.1021/acsenergylett.5c03205","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03205","url":null,"abstract":"This study investigates lithium plating texture in anode-free solid-state batteries using synchrotron-based X-ray diffraction. Conventional methods are limited by lithium’s low electron density and softness, which hinders direct interrogation in anode-free solid-state batteries. Results reveal that lithium plating texture is influenced by temperature and current density. Under mild conditions, lithium exhibited a ⟨110⟩ fiber texture. However, higher current densities and elevated temperatures led to a more randomized orientation, suggesting a dependence on plating conditions. The results highlight how the operating and processing conditions for lithium metal can influence the texture of lithium metal and reversible operation.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"392 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-29DOI: 10.1021/acsenergylett.5c03748
Seryeong Lee, Dawson A. Grimes, Milad Ahmadi Khoshooei, Haomiao Xie, Justin Notestein, Massimiliano Delferro, Omar K. Farha
The selective conversion of hydrocarbons into higher-value fuels and feedstocks is essential to the global energy and chemistry landscape. While porous inorganic materials have enabled significant progress in these transformations, achieving high activity, selectivity, and stability under industrially relevant conditions remains challenging. Metal–organic frameworks (MOFs) are a promising platform to precisely control active-site environments and interrogate structure–function relationships due to their crystallinity, tunability, and porosity. This review highlights relevant hydrocarbon transformations and outlines the general mechanisms for oxidation, oligomerization, and isomerization. Metal node acidity, confinement effects, and active site dispersion are analyzed for their impact on reactivity and selectivity across the three reactions. Finally, we discuss current limitations in catalyst stability and offer a perspective on integrating reticular chemistry with high-throughput experimentation and machine learning to accelerate the discovery and design of robust, next-generation MOF catalysts.
{"title":"Oxidation, Oligomerization, Isomerization of Hydrocarbons Using Metal–Organic Frameworks","authors":"Seryeong Lee, Dawson A. Grimes, Milad Ahmadi Khoshooei, Haomiao Xie, Justin Notestein, Massimiliano Delferro, Omar K. Farha","doi":"10.1021/acsenergylett.5c03748","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03748","url":null,"abstract":"The selective conversion of hydrocarbons into higher-value fuels and feedstocks is essential to the global energy and chemistry landscape. While porous inorganic materials have enabled significant progress in these transformations, achieving high activity, selectivity, and stability under industrially relevant conditions remains challenging. Metal–organic frameworks (MOFs) are a promising platform to precisely control active-site environments and interrogate structure–function relationships due to their crystallinity, tunability, and porosity. This review highlights relevant hydrocarbon transformations and outlines the general mechanisms for oxidation, oligomerization, and isomerization. Metal node acidity, confinement effects, and active site dispersion are analyzed for their impact on reactivity and selectivity across the three reactions. Finally, we discuss current limitations in catalyst stability and offer a perspective on integrating reticular chemistry with high-throughput experimentation and machine learning to accelerate the discovery and design of robust, next-generation MOF catalysts.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"281 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072433","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-29DOI: 10.1021/acsenergylett.5c04249
Raul A. Marquez, Adam C. Nielander, Joaquin Resasco, Thomas F. Jaramillo, C. Buddie Mullins
Electrochemical ocean-based negative emission technologies (EC-ONETs) are emerging strategies that harness the ocean’s capacity for carbon dioxide removal. These systems can couple carbon capture with renewable electricity and water treatment infrastructure and, in the long term, support more ambitious industrial and environmental remediation projects. However, progress─from early demonstrations to deployment at scale─hinges on a more nuanced understanding of electrochemical and transport phenomena in seawater, rigorous field validation, and identification of ecological risks. In this Perspective, we map the current portfolio of EC-ONETs, synthesize reported performance metrics, and outline their limitations and future opportunities. We emphasize the need for a better understanding of pH swing mechanisms and failure modes in seawater, benchmarking standards, biogeochemical impact assessment, coordination with marine sciences, and enhanced public trust through transparent risk assessment and regulatory alignment. We aim to clarify the steps the community can take to advance the practical application of EC-ONETs.
{"title":"Electrochemical Ocean-Based Carbon Capture: Roadblocks to Scale-Up","authors":"Raul A. Marquez, Adam C. Nielander, Joaquin Resasco, Thomas F. Jaramillo, C. Buddie Mullins","doi":"10.1021/acsenergylett.5c04249","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04249","url":null,"abstract":"Electrochemical ocean-based negative emission technologies (EC-ONETs) are emerging strategies that harness the ocean’s capacity for carbon dioxide removal. These systems can couple carbon capture with renewable electricity and water treatment infrastructure and, in the long term, support more ambitious industrial and environmental remediation projects. However, progress─from early demonstrations to deployment at scale─hinges on a more nuanced understanding of electrochemical and transport phenomena in seawater, rigorous field validation, and identification of ecological risks. In this Perspective, we map the current portfolio of EC-ONETs, synthesize reported performance metrics, and outline their limitations and future opportunities. We emphasize the need for a better understanding of pH swing mechanisms and failure modes in seawater, benchmarking standards, biogeochemical impact assessment, coordination with marine sciences, and enhanced public trust through transparent risk assessment and regulatory alignment. We aim to clarify the steps the community can take to advance the practical application of EC-ONETs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"41 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072520","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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