Pub Date : 2025-12-12DOI: 10.1021/acsenergylett.5c02224
Moritz C. Schmidt, Agustin O. Alvarez, Riccardo Pallotta, Biruk A. Seid, Jeroen J. de Boer, Jarla Thiesbrummel, Felix Lang, Giulia Grancini, Bruno Ehrler
Mobile ions play a key role in the degradation of perovskite solar cells, making their quantification essential for enhancing device stability. Various electrical measurements have been applied to characterize mobile ions. However, discerning between different ionic migration processes can be difficult. Furthermore, multiple measurements at different temperatures are usually required to probe different ions and their activation energies. Here, we demonstrate a new characterization technique based on measuring the thermally activated ion current (TAIC) of perovskite solar cells. The method reveals density, diffusion coefficient, and activation energy of mobile ions within a single temperature sweep and offers an intuitive way to distinguish mobile ion species. We apply the TAIC technique to quantify mobile ions of MAPbI3 and triple-cation perovskite solar cells. We find a higher activation energy and a lower diffusion coefficient in the triple-cation devices. TAIC measurements are a simple yet powerful tool to better understand ion migration in perovskite solar cells.
{"title":"Quantification of Mobile Ions in Perovskite Solar Cells with Thermally Activated Ion Current Measurements","authors":"Moritz C. Schmidt, Agustin O. Alvarez, Riccardo Pallotta, Biruk A. Seid, Jeroen J. de Boer, Jarla Thiesbrummel, Felix Lang, Giulia Grancini, Bruno Ehrler","doi":"10.1021/acsenergylett.5c02224","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c02224","url":null,"abstract":"Mobile ions play a key role in the degradation of perovskite solar cells, making their quantification essential for enhancing device stability. Various electrical measurements have been applied to characterize mobile ions. However, discerning between different ionic migration processes can be difficult. Furthermore, multiple measurements at different temperatures are usually required to probe different ions and their activation energies. Here, we demonstrate a new characterization technique based on measuring the thermally activated ion current (TAIC) of perovskite solar cells. The method reveals density, diffusion coefficient, and activation energy of mobile ions within a single temperature sweep and offers an intuitive way to distinguish mobile ion species. We apply the TAIC technique to quantify mobile ions of MAPbI<sub>3</sub> and triple-cation perovskite solar cells. We find a higher activation energy and a lower diffusion coefficient in the triple-cation devices. TAIC measurements are a simple yet powerful tool to better understand ion migration in perovskite solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"29 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729193","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 : 2025-12-12DOI: 10.1021/acsenergylett.5c03199
Hao Zheng, Shaoke Chen, Jinlin Yin, Ping Lu, Yuqi Xi, Xinyan Jiang, Yujie Wu, Ning Zhang, Jin Wang, Zhengquan Li
Lead halide perovskites have demonstrated significant potential for CO2 photoreduction, yet achieving efficient conversion to value-added hydrocarbons (e.g., CH4) remains a challenge. This study proposes an iron-based halide photocatalyst, Cs3FeCl5 nanocrystals (NCs), which achieves a photocatalytic CO2-to-CH4 yield of 2.88 mmol g–1 h–1 with a selectivity nearing 100%. This performance surpasses that of most reported single-component photocatalysts for CO2 methanation. Experimental and theoretical studies reveal that Cs3FeCl5 NCs exhibit intrinsic spin polarization to enhance charge separation, and that their tetracoordinated Fe2+ centers strongly hybridize with CO2 via d–p orbital interaction, thus lowering the activation energy and stabilizing the *COOH intermediate for CH4 production. Under natural sunlight, Cs3FeCl5 NCs maintain an impressive photocatalytic performance, highlighting their significant potential for scalable CO2 conversion. This work underscores the critical role of strong CO2 activation in driving hydrocarbon conversion and provides new design principles for cost-effective solar-to-fuel photocatalysts.
{"title":"Solar-Driven CO2-to-CH4 Conversion Enabled by Fe Tetrahedra in Cs3FeCl5","authors":"Hao Zheng, Shaoke Chen, Jinlin Yin, Ping Lu, Yuqi Xi, Xinyan Jiang, Yujie Wu, Ning Zhang, Jin Wang, Zhengquan Li","doi":"10.1021/acsenergylett.5c03199","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03199","url":null,"abstract":"Lead halide perovskites have demonstrated significant potential for CO<sub>2</sub> photoreduction, yet achieving efficient conversion to value-added hydrocarbons (e.g., CH<sub>4</sub>) remains a challenge. This study proposes an iron-based halide photocatalyst, Cs<sub>3</sub>FeCl<sub>5</sub> nanocrystals (NCs), which achieves a photocatalytic CO<sub>2</sub>-to-CH<sub>4</sub> yield of 2.88 mmol g<sup>–1</sup> h<sup>–1</sup> with a selectivity nearing 100%. This performance surpasses that of most reported single-component photocatalysts for CO<sub>2</sub> methanation. Experimental and theoretical studies reveal that Cs<sub>3</sub>FeCl<sub>5</sub> NCs exhibit intrinsic spin polarization to enhance charge separation, and that their tetracoordinated Fe<sup>2+</sup> centers strongly hybridize with CO<sub>2</sub> via d–p orbital interaction, thus lowering the activation energy and stabilizing the *COOH intermediate for CH<sub>4</sub> production. Under natural sunlight, Cs<sub>3</sub>FeCl<sub>5</sub> NCs maintain an impressive photocatalytic performance, highlighting their significant potential for scalable CO<sub>2</sub> conversion. This work underscores the critical role of strong CO<sub>2</sub> activation in driving hydrocarbon conversion and provides new design principles for cost-effective solar-to-fuel photocatalysts.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729044","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}
MXenes, a family of two-dimensional transition metal carbides, nitrides, and carbonitrides, have emerged as promising materials for energy storage and conversion. Their hydrophilicity, metallic conductivity, and solution processability make them suitable for catalytic applications. However, challenges such as structural instability, limited active sites, and complex surface chemistry hinder their practical use. Recent efforts have focused on enhancing MXene-based catalysts for the oxygen evolution reaction (OER) through structural engineering and hybridization with layered double hydroxides (LDHs) and transition metal oxides (TMOs). This Perspective summarizes key developments in understanding the intrinsic properties of MXenes and their impact on catalytic performance. Moreover, mechanistic insights, ongoing challenges, and opportunities for the rational design of multifunctional MXene hybrids are highlighted. Addressing these fundamental issues will be essential for unlocking the full potential of MXenes in sustainable energy conversion technologies.
{"title":"Insights into MXene-Based Electrocatalysts for the Oxygen Evolution Reaction","authors":"Jizhen Zhang, Zihan Zhang, Renzhi Ma, Takayoshi Sasaki","doi":"10.1021/acsenergylett.5c03334","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03334","url":null,"abstract":"MXenes, a family of two-dimensional transition metal carbides, nitrides, and carbonitrides, have emerged as promising materials for energy storage and conversion. Their hydrophilicity, metallic conductivity, and solution processability make them suitable for catalytic applications. However, challenges such as structural instability, limited active sites, and complex surface chemistry hinder their practical use. Recent efforts have focused on enhancing MXene-based catalysts for the oxygen evolution reaction (OER) through structural engineering and hybridization with layered double hydroxides (LDHs) and transition metal oxides (TMOs). This Perspective summarizes key developments in understanding the intrinsic properties of MXenes and their impact on catalytic performance. Moreover, mechanistic insights, ongoing challenges, and opportunities for the rational design of multifunctional MXene hybrids are highlighted. Addressing these fundamental issues will be essential for unlocking the full potential of MXenes in sustainable energy conversion technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"143 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729046","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 practical application of sodium-ion batteries is hindered by slow ion transport and structural degradation of anodes during cycling. To address this, we report an iodine-doped MoS2 heterostructure with carbon intercalation (I-MoS2@C), constructed via an in situ hydrothermal strategy that integrates phase engineering with interfacial modulation. Glucose-derived carbon layers confine reversible 2H-1T phase transformations, enhancing structural adaptability and ion transport. Concurrently, electron transfer from iodine stabilizes the 1T phase, improving Na+ adsorption and electronic conductivity. At the interface, I–C catalytic sites promote fluorine release and the formation of a NaF-rich SEI, strengthening interfacial ion kinetics and stability. As a result of these synergistic effects, the I-MoS2@C anode exhibits high-rate capability (220 mAh g–1 at 20 A g–1) and exceptional cycling durability. This work demonstrates a strategy for designing dynamically reconstructable, interface-optimized heterostructures for high-performance sodium-ion storage.
钠离子电池的实际应用受到循环过程中离子传输缓慢和阳极结构退化的阻碍。为了解决这个问题，我们报道了一个碘掺杂的MoS2异质结构与碳嵌入（I-MoS2@C），通过原位水热策略，相工程与界面调制相结合构建。葡萄糖衍生的碳层限制了可逆的2H-1T相变，增强了结构适应性和离子传输。同时，来自碘的电子转移稳定了1T相，提高了Na+的吸附和电子导电性。在界面处，I-C催化位点促进氟的释放和富naf SEI的形成，增强了界面离子动力学和稳定性。由于这些协同效应，I-MoS2@C阳极表现出高倍率能力（20 a g-1时220 mAh g-1）和卓越的循环耐久性。这项工作展示了一种设计用于高性能钠离子存储的动态可重构、界面优化异质结构的策略。
{"title":"Phase-Reconstructable MoS2 Heterostructures for High-Performance Sodium-Ion Batteries","authors":"Xin Zhang, Yanchen Fan, Hui Li, Guanyi Wang, Zhaoying Li, Jiantao Li, Chunrong Ma","doi":"10.1021/acsenergylett.5c03845","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03845","url":null,"abstract":"The practical application of sodium-ion batteries is hindered by slow ion transport and structural degradation of anodes during cycling. To address this, we report an iodine-doped MoS<sub>2</sub> heterostructure with carbon intercalation (I-MoS<sub>2</sub>@C), constructed via an in situ hydrothermal strategy that integrates phase engineering with interfacial modulation. Glucose-derived carbon layers confine reversible 2H-1T phase transformations, enhancing structural adaptability and ion transport. Concurrently, electron transfer from iodine stabilizes the 1T phase, improving Na<sup>+</sup> adsorption and electronic conductivity. At the interface, I–C catalytic sites promote fluorine release and the formation of a NaF-rich SEI, strengthening interfacial ion kinetics and stability. As a result of these synergistic effects, the I-MoS<sub>2</sub>@C anode exhibits high-rate capability (220 mAh g<sup>–1</sup> at 20 A g<sup>–1</sup>) and exceptional cycling durability. This work demonstrates a strategy for designing dynamically reconstructable, interface-optimized heterostructures for high-performance sodium-ion storage.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"111 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729088","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 : 2025-12-12DOI: 10.1021/acsenergylett.5c03275
Yameen Ahmed, Xingnan Qi, Parinaz Moazzezi, Makhsud I. Saidaminov
The choice of the perovskite composition is pivotal for solar cells. In this Perspective, we argue that, among known perovskite compositions, formamidinium lead iodide (FAPbI3) stands out due to its optimal bandgap, absence of halide segregation observed in mixed-halide alloys, and immunity against oxidation unlike in tin-based perovskites. However, stabilizing the photoactive α-FAPbI3 remains a major challenge, as it readily transforms into the thermodynamically stable δ-FAPbI3 at room temperature. In this Perspective, we briefly review the challenges in stabilizing α-FAPbI3, summarize strategies to address this instability with minimal and no bandgap penalty, and offer our outlook on future directions: (i) stabilization of α-FAPbI3 without bandgap compromise; (ii) understanding the mechanisms of additive-less stabilized α-FAPbI3 single-crystal perovskite solar cells (PSCs); (iii) development of all-ambient air fabricated tandem solar cells using α-FAPbI3 as a narrow-bandgap subcell; and (iv) adoption of only green solvents to enable scalable, sustainable, and widespread manufacturing of perovskite solar modules.
{"title":"Perovskite Photovoltaics: Pick FAPbI3 and Stick to It","authors":"Yameen Ahmed, Xingnan Qi, Parinaz Moazzezi, Makhsud I. Saidaminov","doi":"10.1021/acsenergylett.5c03275","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03275","url":null,"abstract":"The choice of the perovskite composition is pivotal for solar cells. In this Perspective, we argue that, among known perovskite compositions, formamidinium lead iodide (FAPbI<sub>3</sub>) stands out due to its optimal bandgap, absence of halide segregation observed in mixed-halide alloys, and immunity against oxidation unlike in tin-based perovskites. However, stabilizing the photoactive α-FAPbI<sub>3</sub> remains a major challenge, as it readily transforms into the thermodynamically stable δ-FAPbI<sub>3</sub> at room temperature. In this Perspective, we briefly review the challenges in stabilizing α-FAPbI<sub>3</sub>, summarize strategies to address this instability with minimal and no bandgap penalty, and offer our outlook on future directions: (i) stabilization of α-FAPbI<sub>3</sub> without bandgap compromise; (ii) understanding the mechanisms of additive-less stabilized α-FAPbI<sub>3</sub> single-crystal perovskite solar cells (PSCs); (iii) development of all-ambient air fabricated tandem solar cells using α-FAPbI<sub>3</sub> as a narrow-bandgap subcell; and (iv) adoption of only green solvents to enable scalable, sustainable, and widespread manufacturing of perovskite solar modules.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"74 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729045","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 : 2025-12-12DOI: 10.1021/acsenergylett.5c03378
Wei Li, Qingyang Yin, Zheng Chen
Direct recycling offers a more sustainable and energy-efficient alternative to conventional metallurgical methods for treating end-of-life lithium-ion batteries (LIBs). However, the large-scale deployment of direct regeneration is limited by its low tolerance to impurities, making the production of high-purity feedstocks and impurity management essential for viability. Drawing on insights into how impurities affect cathode regeneration, this Perspective discusses current and emerging separation and purification technologies and delineates the remaining gap to the mass production of high-quality feedstocks. We propose integrated, high-efficiency approaches that elevate feedstock quality and broaden impurity control across the entire workflow, positioning impurity management in both preprocessing and regeneration as being essential to the economic and environmental performance of direct recycling. The result is a research roadmap to enable scalable, sustainable, and cost-effective battery recycling practices.
{"title":"Managing Impurities in Direct Battery Recycling: Advancing Separation and Purification for High-Quality Feedstocks","authors":"Wei Li, Qingyang Yin, Zheng Chen","doi":"10.1021/acsenergylett.5c03378","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03378","url":null,"abstract":"Direct recycling offers a more sustainable and energy-efficient alternative to conventional metallurgical methods for treating end-of-life lithium-ion batteries (LIBs). However, the large-scale deployment of direct regeneration is limited by its low tolerance to impurities, making the production of high-purity feedstocks and impurity management essential for viability. Drawing on insights into how impurities affect cathode regeneration, this Perspective discusses current and emerging separation and purification technologies and delineates the remaining gap to the mass production of high-quality feedstocks. We propose integrated, high-efficiency approaches that elevate feedstock quality and broaden impurity control across the entire workflow, positioning impurity management in both preprocessing and regeneration as being essential to the economic and environmental performance of direct recycling. The result is a research roadmap to enable scalable, sustainable, and cost-effective battery recycling practices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"36 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729050","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 : 2025-12-12DOI: 10.1021/acsenergylett.5c03201
Zuhong Zhang, Kexin Zhao, Bingchen He, Zhenhuang Su, Weiwei Zuo, Bekele Hailegnaw, Yanru Xue, Ying Tang, Xingyu Gao, Michael Saliba, Antonio Abate, Meng Li, Jinsheng Song
Achieving high-efficiency, stable perovskite solar cells (PSCs) requires simultaneous control of film defects and buried interfaces. Here, we report a codeposition strategy using rationally designed 4PACz oligomers. Featuring multidirectional phosphate groups, these oligomers self-assemble to tune the substrate work function, facilitate charge transport, and guide crystallization while passivating defects. Specifically, tri-4PACz achieves an optimal balance between solubility and defect suppression. Consequently, tri-4PACz-based PSCs deliver efficiencies of 26.2% (0.098 cm2) and 22.2% (69.5 cm2 modules). Unencapsulated devices retain 98.7% of initial efficiency after 1000 h of illumination and 96.6% after 500 h at 85 °C. This strategy effectively resolves the trade-off between structural control and defect passivation, paving the way for high-performance, stable PSCs.
{"title":"Molecular Design of Oligomers for Codeposited Perovskite Solar Cells: Enabling Synergistic Control of Crystallization and Carrier Dynamics","authors":"Zuhong Zhang, Kexin Zhao, Bingchen He, Zhenhuang Su, Weiwei Zuo, Bekele Hailegnaw, Yanru Xue, Ying Tang, Xingyu Gao, Michael Saliba, Antonio Abate, Meng Li, Jinsheng Song","doi":"10.1021/acsenergylett.5c03201","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03201","url":null,"abstract":"Achieving high-efficiency, stable perovskite solar cells (PSCs) requires simultaneous control of film defects and buried interfaces. Here, we report a codeposition strategy using rationally designed 4PACz oligomers. Featuring multidirectional phosphate groups, these oligomers self-assemble to tune the substrate work function, facilitate charge transport, and guide crystallization while passivating defects. Specifically, tri-4PACz achieves an optimal balance between solubility and defect suppression. Consequently, tri-4PACz-based PSCs deliver efficiencies of 26.2% (0.098 cm<sup>2</sup>) and 22.2% (69.5 cm<sup>2</sup> modules). Unencapsulated devices retain 98.7% of initial efficiency after 1000 h of illumination and 96.6% after 500 h at 85 °C. This strategy effectively resolves the trade-off between structural control and defect passivation, paving the way for high-performance, stable PSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"226 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729051","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 : 2025-12-12DOI: 10.1021/acsenergylett.5c03644
Tuo Wang, Feifei Li, Liwei Xue, Yang Hu, Guangzhe Wang, Li Xiao, Gongwei Wang, Lin Zhuang
Water management is crucial in low-temperature electrochemical technologies (e.g., fuel cells, water electrolysis, and CO2 electrolysis). Herein, we introduce a real-time adjustable water management strategy for CO2 membrane electrode assembly (MEA) electrolyzers. It exploits the semipermeable nature of alkaline polyelectrolyte (APE) membranes, which selectively allow the passage of OH– and water. By adding a controlled amount of 6-azoniaspiro[5.5]undecane cation ([ASU]+) to the anolyte, we can modulate the osmotic pressure across the APE membrane and create a hydrophobic barrier layer via electric field-driven self-assembly. This allows precise gating control of the transmembrane water transport flux from the anode to the cathode, thereby significantly impacting the cathode CO2 reduction performance. A continuous CO2 electrolysis test further shows that simply switching the anolyte between pure water and [ASU]OH solution enables real-time modulation of the cathode water content and, consequently, the CO2 reduction selectivity, underscoring the simplicity and effectiveness of this approach.
{"title":"Organic Cation Gating Control for Water Management in CO2 Membrane Electrode Assembly Electrolyzers","authors":"Tuo Wang, Feifei Li, Liwei Xue, Yang Hu, Guangzhe Wang, Li Xiao, Gongwei Wang, Lin Zhuang","doi":"10.1021/acsenergylett.5c03644","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03644","url":null,"abstract":"Water management is crucial in low-temperature electrochemical technologies (e.g., fuel cells, water electrolysis, and CO<sub>2</sub> electrolysis). Herein, we introduce a real-time adjustable water management strategy for CO<sub>2</sub> membrane electrode assembly (MEA) electrolyzers. It exploits the semipermeable nature of alkaline polyelectrolyte (APE) membranes, which selectively allow the passage of OH<sup>–</sup> and water. By adding a controlled amount of 6-azoniaspiro[5.5]undecane cation ([ASU]<sup>+</sup>) to the anolyte, we can modulate the osmotic pressure across the APE membrane and create a hydrophobic barrier layer via electric field-driven self-assembly. This allows precise gating control of the transmembrane water transport flux from the anode to the cathode, thereby significantly impacting the cathode CO<sub>2</sub> reduction performance. A continuous CO<sub>2</sub> electrolysis test further shows that simply switching the anolyte between pure water and [ASU]OH solution enables real-time modulation of the cathode water content and, consequently, the CO<sub>2</sub> reduction selectivity, underscoring the simplicity and effectiveness of this approach.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"147 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729052","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 : 2025-12-12DOI: 10.1021/acsenergylett.5c03842
Prashant V. Kamat*, and , Greco González Miera*,
{"title":"Abstract vs Conclusion: Articulating Purpose, Structure, and Impact","authors":"Prashant V. Kamat*, and , Greco González Miera*, ","doi":"10.1021/acsenergylett.5c03842","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03842","url":null,"abstract":"","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 12","pages":"6576–6577"},"PeriodicalIF":18.2,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718600","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 : 2025-12-12DOI: 10.1021/acsenergylett.5c03204
Mengmeng Li, Yajing Liu, Xiufu Hua, Dazhuan Wu, Li Yao, Zhengdong Cheng, Xiuyu Wang
The sluggish kinetics of the oxygen reduction reaction (ORR)─a critical bottleneck in fuel cells and metal–air batteries─originate from intertwined charge, spin, and coordination constraints, compounded by the high dissociation barrier of the O═O bond. To address these limitations, we engineer a two-sequential-kinetics control strategy, demonstrated by L10-FePt/Fe core–shell nanocatalysts featuring a chemically ordered ferromagnetic L10-FePt core and an epitaxial Fe monolayer shell. The single-atom-like Fe shell reconfigures O2 adsorption from Pauling-type vertical top-site (Fe–O═O) to Yeager-type parallel bridge-site (Fe–O–O–Fe) coordination, optimizing O2 adsorption kinetics. Sequentially, the ferromagnetic exchange-coupled interface induces a spin pinning effect (pinning ratio of 70%) under magnetic fields, which facilitates the spin-selective flip of added electrons, thereby eliminating spin-forbidden kinetic barriers in the spin transition process between the Yeager-type adsorbed triplet O2 (S = 1) and singlet H2O (S = 0) during the ORR. This strategy delivers a 10.9-fold enhancement in specific activity versus that of commercial Pt/C, with transformative implications for spin-constrained electrocatalysis.
氧还原反应（ORR）的缓慢动力学──燃料电池和金属-空气电池中的一个关键瓶颈──源于纠缠在一起的电荷、自旋和配位限制，以及O = O键的高解离势垒。为了解决这些限制，我们设计了一种双顺序动力学控制策略，通过L10-FePt/Fe核壳纳米催化剂来证明，该催化剂具有化学有序的铁磁性L10-FePt核和外延铁单层壳。单原子状铁壳层将O2吸附从鲍林型垂直顶位（Fe - O = O）重新配置为耶格尔型平行桥位（Fe - O - O - Fe）配位，优化了O2吸附动力学。随后，铁磁交换耦合界面在磁场作用下产生自旋钉住效应（钉住率为70%），有利于添加电子的自旋选择性翻转，从而消除了在ORR过程中yeager型吸附三重态O2 （S = 1）和单重态H2O （S = 0）之间自旋跃迁过程中的自旋禁止动力学障碍。与商用Pt/C相比，该策略的比活性提高了10.9倍，对自旋约束电催化具有变革性意义。
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