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Electric Double Layer Charging, a New Framework for Optimizing Electrocatalyst Design and Performance 电双层充电:优化电催化剂设计和性能的新框架
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-09 DOI: 10.1021/acsenergylett.5c04144
Minho M. Kim,Chang Hyuck Choi,Hyungjun Kim
Electrochemical reactions occur at charged interfaces where the accumulation and redistribution of charge within the electric double layer (EDL) fundamentally govern the reaction kinetics. Despite its ubiquity, the mechanistic connection between EDL charging and electrocatalytic activity remains underexplored. This Perspective highlights recent theoretical and experimental advances─focusing on studies from our group and others─that link the degree of EDL charging, characterized by the surface charge density (σ), to catalytic activity. We categorized the types of charge accumulated in the EDL as space charge, ionic charge, and pseudocapacitive charge and discussed how these components mechanistically influence electrocatalytic activity. Together, these insights suggest σ as a key descriptor that representatively captures the microenvironment effect of the EDL, bridging interfacial charge dynamics and catalytic performance and thereby suggesting new opportunities for the rational design of high-performance electrochemical interfaces.
{"title":"Electric Double Layer Charging, a New Framework for Optimizing Electrocatalyst Design and Performance","authors":"Minho M. Kim,Chang Hyuck Choi,Hyungjun Kim","doi":"10.1021/acsenergylett.5c04144","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04144","url":null,"abstract":"Electrochemical reactions occur at charged interfaces where the accumulation and redistribution of charge within the electric double layer (EDL) fundamentally govern the reaction kinetics. Despite its ubiquity, the mechanistic connection between EDL charging and electrocatalytic activity remains underexplored. This Perspective highlights recent theoretical and experimental advances─focusing on studies from our group and others─that link the degree of EDL charging, characterized by the surface charge density (σ), to catalytic activity. We categorized the types of charge accumulated in the EDL as space charge, ionic charge, and pseudocapacitive charge and discussed how these components mechanistically influence electrocatalytic activity. Together, these insights suggest σ as a key descriptor that representatively captures the microenvironment effect of the EDL, bridging interfacial charge dynamics and catalytic performance and thereby suggesting new opportunities for the rational design of high-performance electrochemical interfaces.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138862","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}
引用次数: 0
Measuring pH Changes Inside a Bipolar Membrane Junction 测量双极膜结内的pH值变化
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-09 DOI: 10.1021/acsenergylett.5c03710
Shujin Hou,T. Nathan Stovall,Adam Z. Weber,Shannon W. Boettcher
The local pH environment within bipolar membrane (BPM) junctions is complex and not well understood, yet it is important to control for advancing the performance of BPM-based electrochemical systems. We report a voltammetric strategy using an ultrathin Ni mesh pH probe to spatially resolve pH changes in the BPM junction during model BPM electrolyzer operation. Under reverse bias, we observe depletion of OH– at the anion-exchange layer (AEL) interface, with a degree diminishing with increasing distance from the AEL. These gradients correlate with current-dependent water dissociation (WD) and are modulated by the electric field and the surface charge state of the catalyst. By correlating spatial pH profiles with the surface-charging behavior of WD catalysts, we explore a mechanism of catalyst-mediated H+ and OH– transfer facilitated by hydrogen-bonding networks. These findings highlight the role of local chemistry and electrostatics in BPM performance and offer new methods to probe and engineer catalytic junctions in electrochemical energy devices.
{"title":"Measuring pH Changes Inside a Bipolar Membrane Junction","authors":"Shujin Hou,T. Nathan Stovall,Adam Z. Weber,Shannon W. Boettcher","doi":"10.1021/acsenergylett.5c03710","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03710","url":null,"abstract":"The local pH environment within bipolar membrane (BPM) junctions is complex and not well understood, yet it is important to control for advancing the performance of BPM-based electrochemical systems. We report a voltammetric strategy using an ultrathin Ni mesh pH probe to spatially resolve pH changes in the BPM junction during model BPM electrolyzer operation. Under reverse bias, we observe depletion of OH– at the anion-exchange layer (AEL) interface, with a degree diminishing with increasing distance from the AEL. These gradients correlate with current-dependent water dissociation (WD) and are modulated by the electric field and the surface charge state of the catalyst. By correlating spatial pH profiles with the surface-charging behavior of WD catalysts, we explore a mechanism of catalyst-mediated H+ and OH– transfer facilitated by hydrogen-bonding networks. These findings highlight the role of local chemistry and electrostatics in BPM performance and offer new methods to probe and engineer catalytic junctions in electrochemical energy devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"5 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138978","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}
引用次数: 0
Protective Solid Interphase via Composite Additives for Long-Life Aqueous Zinc Batteries 复合添加剂用于长寿命锌水电池的固相保护
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-09 DOI: 10.1021/acsenergylett.5c03837
Xianting Zhao,Di Liu,Kuang-Yen Chiu,Xinya Qiu,Hanci Chen,Mengqi Zhu,Guowen Dong,Jeng-Han Wang,Xianhui Zhang,Wenwu Li,Zaiping Guo,Ho Seok Park
Here, we report a composite additive strategy that integrates sodium hexametaphosphate (SHMP) and sodium molybdate (NMO) to achieve cooperative regulation of the electrolyte bulk chemistry and the Zn–electrolyte interface. SHMP reconstructs the Zn2+ solvation structure through controlled coordination, while NMO mitigates overchelation via pH buffering and preferential interfacial adsorption. Their cooperation induces the in situ formation of a chemically coupled Mo/P-rich interphase, which regulates ion flux, limits proton-driven side reactions, and maintains Zn deposition kinetics. Comprehensive experiments and theoretical calculations elucidate the bulk–interface coupling governing Zn2+ transport and reversibility. Consequently, the resulting electrolyte enables 3700 h reversible cycling in Zn||Zn cells, 99.85% average Coulombic efficiency over 5100 cycles in Zn||Cu cells, and 78.9% capacity retention after 2500 cycles in Zn||MnO2 cells. This work presents a general dual-regulation paradigm for Zn electrolyte design and provides mechanistic insights into developing aqueous zinc-ion batteries.
{"title":"Protective Solid Interphase via Composite Additives for Long-Life Aqueous Zinc Batteries","authors":"Xianting Zhao,Di Liu,Kuang-Yen Chiu,Xinya Qiu,Hanci Chen,Mengqi Zhu,Guowen Dong,Jeng-Han Wang,Xianhui Zhang,Wenwu Li,Zaiping Guo,Ho Seok Park","doi":"10.1021/acsenergylett.5c03837","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03837","url":null,"abstract":"Here, we report a composite additive strategy that integrates sodium hexametaphosphate (SHMP) and sodium molybdate (NMO) to achieve cooperative regulation of the electrolyte bulk chemistry and the Zn–electrolyte interface. SHMP reconstructs the Zn2+ solvation structure through controlled coordination, while NMO mitigates overchelation via pH buffering and preferential interfacial adsorption. Their cooperation induces the in situ formation of a chemically coupled Mo/P-rich interphase, which regulates ion flux, limits proton-driven side reactions, and maintains Zn deposition kinetics. Comprehensive experiments and theoretical calculations elucidate the bulk–interface coupling governing Zn2+ transport and reversibility. Consequently, the resulting electrolyte enables 3700 h reversible cycling in Zn||Zn cells, 99.85% average Coulombic efficiency over 5100 cycles in Zn||Cu cells, and 78.9% capacity retention after 2500 cycles in Zn||MnO2 cells. This work presents a general dual-regulation paradigm for Zn electrolyte design and provides mechanistic insights into developing aqueous zinc-ion batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138977","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}
引用次数: 0
Taming Chemical Reactions in Batteries by Noncovalent Interactions 通过非共价相互作用控制电池中的化学反应
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-09 DOI: 10.1021/acsenergylett.5c04024
Tianyue Wang,Zhizun Wu,Zhenqing Jiang,Guangjian Hu,Huicong Yang,Feng Li,Hui-Ming Cheng
Battery performance is governed not only by electrochemical reactions but also by parasitic and unavoidable chemical reactions, such as the hydrolysis of LiPF6 by trace H2O. Rather than conventional H2O/HF scavenging, we suggest a strategy for taming these reactions via noncovalent interactions. Hydrogen bonds are designed to deactivate H2O molecules, thereby suppressing LiPF6 hydrolysis during battery operation. This example illustrates the precise control of the reactivity of chemical reactions by noncovalent interactions. “Competition” based on the strength of different noncovalent interactions is the key in this strategy. This concept is generalized to control other key chemical reactions and equilibria in batteries, including salt dissolution and solvation structure change, enabling control of ion transport and interface chemistry. This paradigm opens a new way to manipulate chemical reactions without breaking covalent bonds, not only in batteries but also in broad applications such as electrocatalysis and chemical reactions.
{"title":"Taming Chemical Reactions in Batteries by Noncovalent Interactions","authors":"Tianyue Wang,Zhizun Wu,Zhenqing Jiang,Guangjian Hu,Huicong Yang,Feng Li,Hui-Ming Cheng","doi":"10.1021/acsenergylett.5c04024","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04024","url":null,"abstract":"Battery performance is governed not only by electrochemical reactions but also by parasitic and unavoidable chemical reactions, such as the hydrolysis of LiPF6 by trace H2O. Rather than conventional H2O/HF scavenging, we suggest a strategy for taming these reactions via noncovalent interactions. Hydrogen bonds are designed to deactivate H2O molecules, thereby suppressing LiPF6 hydrolysis during battery operation. This example illustrates the precise control of the reactivity of chemical reactions by noncovalent interactions. “Competition” based on the strength of different noncovalent interactions is the key in this strategy. This concept is generalized to control other key chemical reactions and equilibria in batteries, including salt dissolution and solvation structure change, enabling control of ion transport and interface chemistry. This paradigm opens a new way to manipulate chemical reactions without breaking covalent bonds, not only in batteries but also in broad applications such as electrocatalysis and chemical reactions.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"34 24 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138979","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}
引用次数: 0
Beyond Hole Transportation: Substrate-Engineered Sb2Se3 Photocathodes 超越空穴传输:衬底工程Sb2Se3光电阴极
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-08 DOI: 10.1021/acsenergylett.5c04281
Ziying Zhang,Guanghui Zhu,Yuchen Dong,Sanghyun Bae,Thomas Moehl,Yongping Gan,S. David Tilley,Xiangjiu Guan,Liejin Guo
While antimony selenide (Sb2Se3) has emerged as a promising absorber for photoelectrochemical water splitting, the critical role of the hole transport layer (HTL) for back-contact remains underexplored. We introduced solution-processed NiOx nanocrystals as noble metal-free HTL that synergistically enable: (1) Thermodynamic-stability-driven [hk1]-oriented Sb2Se3 growth with the lowest interfacial formation energy and (2) Electron-blocking functionality through a 2.16 eV conduction band offset at the back contact interface. Therefore, the optimized NiOx-based photocathode achieved a photocurrent density of −17 mA cm–2 at 0 V versus reversible hydrogen electrode (RHE) and 214 mV photovoltage, outperforming Au-based and HTL-free-based counterparts. This dual functionality-crystallographic templating and hole-selective transport not only improve the crystal growth of the absorber but also suppress electron back flowing. This work establishes NiOx nanocrystals as a design paradigm for chalcogenide photoelectrodes, emphasizing concurrent interfacial lattice matching and electronic alignment optimization for solar-fuel generation.
{"title":"Beyond Hole Transportation: Substrate-Engineered Sb2Se3 Photocathodes","authors":"Ziying Zhang,Guanghui Zhu,Yuchen Dong,Sanghyun Bae,Thomas Moehl,Yongping Gan,S. David Tilley,Xiangjiu Guan,Liejin Guo","doi":"10.1021/acsenergylett.5c04281","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04281","url":null,"abstract":"While antimony selenide (Sb2Se3) has emerged as a promising absorber for photoelectrochemical water splitting, the critical role of the hole transport layer (HTL) for back-contact remains underexplored. We introduced solution-processed NiOx nanocrystals as noble metal-free HTL that synergistically enable: (1) Thermodynamic-stability-driven [hk1]-oriented Sb2Se3 growth with the lowest interfacial formation energy and (2) Electron-blocking functionality through a 2.16 eV conduction band offset at the back contact interface. Therefore, the optimized NiOx-based photocathode achieved a photocurrent density of −17 mA cm–2 at 0 V versus reversible hydrogen electrode (RHE) and 214 mV photovoltage, outperforming Au-based and HTL-free-based counterparts. This dual functionality-crystallographic templating and hole-selective transport not only improve the crystal growth of the absorber but also suppress electron back flowing. This work establishes NiOx nanocrystals as a design paradigm for chalcogenide photoelectrodes, emphasizing concurrent interfacial lattice matching and electronic alignment optimization for solar-fuel generation.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"385 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138863","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}
引用次数: 0
Solvation Sheath Exchange with Weak-Solvent Molecules Enables the Development of Sodium Dual-Ion Pouch Cells 与弱溶剂分子的溶剂化鞘交换使钠双离子袋状电池的发展成为可能
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acsenergylett.5c03388
Sanjaykumar C, Soumyashree Das Adhikari, Mahesh Chandra, Kundan Kumar Mishra, Sungjemmenla, Rahul Singh, S. K. Vineeth, Hemant Kumar, Sanjeev Kumar Chauhan, Rajendra Singh, Vipin Kumar
This study introduces a new electrolyte formulation enabling low-potential intercalation of PF6 anions. The electrolyte consists of an optimized mixture of ethyl methyl carbonate (EMC, a primary solvating medium) and trimethyl phosphate (TMP, a weakly solvating medium). While solvation in either EMC or TMP alone is unstable, adding TMP to EMC modifies the solvation sheath and enhances the solvation dynamics. Theoretical calculations reveal that a favorable solvation environment can be achieved through a balanced exchange of EMC with TMP molecules, thereby improving the overall stability and electrochemical performance of the cell. Sodium dual-ion cells, comprising sodium metal and synthetic graphite as the anode and cathode, respectively, exhibit an impressive cycling stability and high Coulombic efficiency when paired with the optimized electrolyte system. We believe that the strategy of solvation-shell exchange using weakly solvating solvents to modulate solvation dynamics could pave the way for the design of next-generation electrolyte systems for high-performance sodium dual-ion batteries.
{"title":"Solvation Sheath Exchange with Weak-Solvent Molecules Enables the Development of Sodium Dual-Ion Pouch Cells","authors":"Sanjaykumar C, Soumyashree Das Adhikari, Mahesh Chandra, Kundan Kumar Mishra, Sungjemmenla, Rahul Singh, S. K. Vineeth, Hemant Kumar, Sanjeev Kumar Chauhan, Rajendra Singh, Vipin Kumar","doi":"10.1021/acsenergylett.5c03388","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03388","url":null,"abstract":"This study introduces a new electrolyte formulation enabling low-potential intercalation of PF<sub>6</sub><sup>–</sup> anions. The electrolyte consists of an optimized mixture of ethyl methyl carbonate (EMC, a primary solvating medium) and trimethyl phosphate (TMP, a weakly solvating medium). While solvation in either EMC or TMP alone is unstable, adding TMP to EMC modifies the solvation sheath and enhances the solvation dynamics. Theoretical calculations reveal that a favorable solvation environment can be achieved through a balanced exchange of EMC with TMP molecules, thereby improving the overall stability and electrochemical performance of the cell. Sodium dual-ion cells, comprising sodium metal and synthetic graphite as the anode and cathode, respectively, exhibit an impressive cycling stability and high Coulombic efficiency when paired with the optimized electrolyte system. We believe that the strategy of solvation-shell exchange using weakly solvating solvents to modulate solvation dynamics could pave the way for the design of next-generation electrolyte systems for high-performance sodium dual-ion batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"31 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129702","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}
引用次数: 0
Weakly Solvated Anions in Electrolytes Boost Cathode Performance for Dual-Ion Batteries and Hybrid Ion Capacitors 电解质中的弱溶剂化阴离子提高双离子电池和混合离子电容器的阴极性能
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acsenergylett.5c04223
Chenglin Zhang, Xueyang He, Shiqi Li, Yulian Dong, Zhijie Lei, Yuhang Ling, Dawei Cao, Huaping Zhao, Yong Lei
Electrochemical anion storage plays a critical role in the development of hybrid ion capacitors and dual-ion batteries. However, the mechanism of the interaction between electrolytes and anion storage remains unknown. Herein, we systematically investigate the electrochemical anion-storage properties of polypyrrole (PPy) cathodes in different chain-length ether-based electrolytes. In dimethyl ether (DME)-based electrolytes, the PPy cathode delivers a specific capacity of 91 mAh g–1 at 100 mA g–1 after 200 cycles and maintained 60 mAh g–1 at 5 A g–1. The shorter-chain DME exhibits weaker anion-solvent interactions, enabling rapid anion desolvation behavior, thus enhancing ion storage kinetics. Further experimental analysis and theoretical computation verify that the shorter-chain solvents exhibit reduced solvation energy barriers and optimized interfacial charge transfer. This work highlights the critical role of solvent molecular structure in regulating anion storage kinetics, providing a strategic electrolyte design for approaching high-performance sodium-ion hybrid capacitors and dual-ion batteries.
{"title":"Weakly Solvated Anions in Electrolytes Boost Cathode Performance for Dual-Ion Batteries and Hybrid Ion Capacitors","authors":"Chenglin Zhang, Xueyang He, Shiqi Li, Yulian Dong, Zhijie Lei, Yuhang Ling, Dawei Cao, Huaping Zhao, Yong Lei","doi":"10.1021/acsenergylett.5c04223","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04223","url":null,"abstract":"Electrochemical anion storage plays a critical role in the development of hybrid ion capacitors and dual-ion batteries. However, the mechanism of the interaction between electrolytes and anion storage remains unknown. Herein, we systematically investigate the electrochemical anion-storage properties of polypyrrole (PPy) cathodes in different chain-length ether-based electrolytes. In dimethyl ether (DME)-based electrolytes, the PPy cathode delivers a specific capacity of 91 mAh g<sup>–1</sup> at 100 mA g<sup>–1</sup> after 200 cycles and maintained 60 mAh g<sup>–1</sup> at 5 A g<sup>–1</sup>. The shorter-chain DME exhibits weaker anion-solvent interactions, enabling rapid anion desolvation behavior, thus enhancing ion storage kinetics. Further experimental analysis and theoretical computation verify that the shorter-chain solvents exhibit reduced solvation energy barriers and optimized interfacial charge transfer. This work highlights the critical role of solvent molecular structure in regulating anion storage kinetics, providing a strategic electrolyte design for approaching high-performance sodium-ion hybrid capacitors and dual-ion batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"134 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122254","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}
引用次数: 0
Rapid Laser-Based Deposition of PbI2/CsBr Inorganic Scaffolds for Hybrid Fabrication of Perovskite/Silicon Tandem Solar Cells 快速激光沉积PbI2/CsBr无机支架制备钙钛矿/硅串联太阳能电池
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acsenergylett.5c04010
Suzana Kralj, Kerem Artuk, Marly Nales, Vladyslav Hnapovskyi, Miriam Minguez-Avellan, Badri Vishal, Ahmed Ali Said, Pablo P. Boix, Stefaan De Wolf, Christian M. Wolff, Monica Morales-Masis
Rapid dry deposition of metal halide perovskites and inorganic scaffolds remains a key challenge for scalable vapor-phase fabrication. Here, we demonstrate fast vapor-phase growth of PbI2/CsBr inorganic scaffolds from a single composite target using pulsed laser deposition. Deposition rates exceeding 100 nm min–1, over an order of magnitude higher than comparable co-evaporated scaffolds, enable the deposition of ∼540 nm-thick PbI2/CsBr inorganic scaffolds on textured silicon cells within 5 min. The PbI2/CsBr ratio is moreover maintained from the source target to the film, and the process delivers high material utilization. Proof-of-concept 1 cm2 fully textured perovskite/silicon tandem cells are demonstrated with the rapid PLD scaffolds converted with an organohalide solution to perovskite absorbers and passivated with piperazinium iodide. The material and device characterization demonstrates that laser-based vapor deposition is a promising route for rapid inorganic scaffold fabrication.
{"title":"Rapid Laser-Based Deposition of PbI2/CsBr Inorganic Scaffolds for Hybrid Fabrication of Perovskite/Silicon Tandem Solar Cells","authors":"Suzana Kralj, Kerem Artuk, Marly Nales, Vladyslav Hnapovskyi, Miriam Minguez-Avellan, Badri Vishal, Ahmed Ali Said, Pablo P. Boix, Stefaan De Wolf, Christian M. Wolff, Monica Morales-Masis","doi":"10.1021/acsenergylett.5c04010","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04010","url":null,"abstract":"Rapid dry deposition of metal halide perovskites and inorganic scaffolds remains a key challenge for scalable vapor-phase fabrication. Here, we demonstrate fast vapor-phase growth of PbI<sub>2</sub>/CsBr inorganic scaffolds from a single composite target using pulsed laser deposition. Deposition rates exceeding 100 nm min<sup>–1</sup>, over an order of magnitude higher than comparable co-evaporated scaffolds, enable the deposition of ∼540 nm-thick PbI<sub>2</sub>/CsBr inorganic scaffolds on textured silicon cells within 5 min. The PbI<sub>2</sub>/CsBr ratio is moreover maintained from the source target to the film, and the process delivers high material utilization. Proof-of-concept 1 cm<sup>2</sup> fully textured perovskite/silicon tandem cells are demonstrated with the rapid PLD scaffolds converted with an organohalide solution to perovskite absorbers and passivated with piperazinium iodide. The material and device characterization demonstrates that laser-based vapor deposition is a promising route for rapid inorganic scaffold fabrication.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"161 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135237","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}
引用次数: 0
Short-Wave Infrared InAs Quantum-Dot Light-Emitting Diodes with Tunable Electroluminescence beyond 1.4 μm 超1.4 μm电致发光可调谐短波红外InAs量子点发光二极管
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-04 DOI: 10.1021/acsenergylett.5c03820
Hossein Roshan, Davide Mazza, Satyaprakash Panda, Francesco de Boni, Luca De Trizio, Liberato Manna, Francesco Di Stasio
Short-wave infrared (SWIR) optoelectronics based on colloidal quantum dots (QDs) have been dominated by heavy-metal chalcogenides for many years (e.g., PbS, HgTe). Here, we present Restriction of Hazardous Substances-compliant InAs/ZnSe core/shell QD light-emitting diodes (LEDs) operating in the SWIR spectral range. The InAs cores are synthesized via a tris(dimethylamino)arsine-based continuous-injection method, enabling size control and SWIR spectral tuning. The LEDs employ a hybrid charge-injection stack comprising organic hole-transport layers (poly-TPD/PTAA) and an inorganic ZnMgO electron-transport layer to balance injection into the InAs/ZnSe core/shell QD film. Four different LEDs, with electroluminescence (EL) peaks centered at 1007, 1275, 1300, and 1410 nm, achieve external peak quantum efficiencies of 6.20%, 3.75%, 2.04%, and 1.10%, respectively. This work is the first demonstration of EL from InAs QDs beyond 1100 nm, advancing III–V QDs for SWIR optoelectronic systems in fields such as machine vision and bioimaging.
基于胶体量子点(QDs)的短波红外(SWIR)光电子技术多年来一直被重金属硫族化合物(如PbS、HgTe)所主导。在这里,我们提出了在SWIR光谱范围内工作的符合有害物质的InAs/ZnSe核/壳QD发光二极管(led)的限制。InAs芯通过基于三(二甲胺)胂的连续注入方法合成,实现了尺寸控制和SWIR光谱调谐。led采用混合电荷注入堆叠,包括有机空穴传输层(聚tpd /PTAA)和无机ZnMgO电子传输层,以平衡注入到InAs/ZnSe核/壳QD膜。四种不同的led,其电致发光(EL)峰中心分别为1007、1275、1300和1410 nm,其外峰量子效率分别为6.20%、3.75%、2.04%和1.10%。这项工作是首次从超过1100nm的InAs量子点中展示EL,推进了SWIR光电系统在机器视觉和生物成像等领域的III-V量子点。
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引用次数: 0
Toward Sustainable Electrochemical CO2 Valorization 迈向可持续的电化学CO2增值
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-04 DOI: 10.1021/acsenergylett.5c04160
Gengfeng Zheng
With the continuous accumulation of the atmospheric CO2 level and the substantial cost reduction of renewable electricity generation in the past decade, electrocatalytic CO2 reduction under ambient conditions has been attracting significant research interest worldwide, as it presents potentials of both reducing carbon footprints and producing value-added products. Although many scientific breakthroughs have been reported to contribute to this field, most of those discoveries are still based on laboratory-scale studies, while the implementation of this technology into scalable industrial deployment remains hindered and highly challenging. This Perspective briefly discusses several key challenges in the full electrocatalytic CO2 reduction system, including CO2 capture and direct utilization, catalysts with high stability, surface/interface functionalization, ion-exchange membranes, and electrolytes, which are strongly correlated to the potentials toward sustainable electrochemical CO2 valorization. Furthermore, several important research directions are also proposed, such as developing new catalysts and mechanisms, unconventional reaction conditions, coupling of CO2 electroreduction with other reactants, and tandem catalytic reactions.
近十年来,随着大气CO2水平的不断积累和可再生能源发电成本的大幅降低,环境条件下的电催化CO2还原技术因其具有减少碳足迹和生产增值产品的潜力而引起了世界范围内的极大研究兴趣。尽管许多科学突破已经被报道为该领域做出了贡献,但大多数发现仍然基于实验室规模的研究,而将该技术应用于可扩展的工业部署仍然受到阻碍,并且极具挑战性。本展望简要讨论了全电催化CO2还原系统的几个关键挑战,包括CO2捕获和直接利用,高稳定性催化剂,表面/界面功能化,离子交换膜和电解质,这些与可持续的电化学CO2增值潜力密切相关。提出了开发新型催化剂和机理、非常规反应条件、CO2电还原与其他反应物耦合、串联催化反应等重要研究方向。
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引用次数: 0
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ACS Energy Letters
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