Pure-water membrane electrode assemblies (MEAs) represent a promising strategy to eliminate (bi)carbonate salt precipitation for electrochemical CO2 reduction (CO2R). However, the absence of alkali metal cations fundamentally restricts CO2 activation and intermediate stabilization, thereby reducing catalytic performance. Here, we overcome this limitation by identifying the ionomer charge density as a key molecular-level parameter associated with pure-water CO2R. By comparing anion-exchange ionomers with varying charge characteristics, we reveal that high-charge-density ionomer (HCDI) introduces a favorable catalyst–membrane interfacial environment, enabling superior macroscopic CO2R performance. HCDI-enabled MEAs achieve >99% CO Faradaic efficiency at 100 mA cm–2 and sustain ∼92% at 1000 mA cm–2. In situ diagnosis and electrochemical characterization reveal that the HCDI-functionalized interface produces a substantial *CO signal, while concurrently suppressing hydrogen evolution. By decoupling cation effects from liquid electrolytes, these findings support interfacial ionomer charge density as a useful comparative parameter for pure-water CO2 MEA electrolyzers.
纯水膜电极组件（MEAs）是一种很有前途的策略，以消除（双）碳酸盐岩沉淀的电化学二氧化碳还原（CO2R）。然而，碱金属阳离子的缺乏从根本上限制了CO2的活化和中间稳定，从而降低了催化性能。在这里，我们克服了这一限制，将离子单体电荷密度确定为与纯水CO2R相关的关键分子水平参数。通过比较具有不同电荷特性的阴离子交换离聚体，我们发现高电荷密度离聚体（HCDI）引入了良好的催化剂-膜界面环境，从而实现了优越的宏观CO2R性能。启用hcdi的mea在100 mA cm-2时可实现高达99%的CO法拉第效率，在1000 mA cm-2时可保持92%的CO法拉第效率。原位诊断和电化学表征表明，hcdi功能化界面产生大量的*CO信号，同时抑制析氢。通过从液体电解质中解耦阳离子效应，这些发现支持界面离聚体电荷密度作为纯水CO2 MEA电解槽的有用比较参数。
{"title":"Charge-Density-Dependent Ionomer Effects in Pure-Water CO2 Electrolysis","authors":"Minqiu Lan,Wenhao Ren,Linsen Huang,Xiaogang Sun,Shi-Zhang Qiao","doi":"10.1021/acsenergylett.6c02712","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02712","url":null,"abstract":"Pure-water membrane electrode assemblies (MEAs) represent a promising strategy to eliminate (bi)carbonate salt precipitation for electrochemical CO2 reduction (CO2R). However, the absence of alkali metal cations fundamentally restricts CO2 activation and intermediate stabilization, thereby reducing catalytic performance. Here, we overcome this limitation by identifying the ionomer charge density as a key molecular-level parameter associated with pure-water CO2R. By comparing anion-exchange ionomers with varying charge characteristics, we reveal that high-charge-density ionomer (HCDI) introduces a favorable catalyst–membrane interfacial environment, enabling superior macroscopic CO2R performance. HCDI-enabled MEAs achieve >99% CO Faradaic efficiency at 100 mA cm–2 and sustain ∼92% at 1000 mA cm–2. In situ diagnosis and electrochemical characterization reveal that the HCDI-functionalized interface produces a substantial *CO signal, while concurrently suppressing hydrogen evolution. By decoupling cation effects from liquid electrolytes, these findings support interfacial ionomer charge density as a useful comparative parameter for pure-water CO2 MEA electrolyzers.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"12 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221517","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 : 2026-10-20DOI: 10.1021/acsenergylett.6c02492
Eunsong Jeon,Gayoung Ham,Jin Su Park,Hoon Kim,Euimin Lee,Donghyun Lee,Hyuna Kim,Jun-Ho Yum,Kevin Sivula,Hyojung Cha,Han-Hee Cho
Integrating alternative oxidation reactions (AORs) into photoelectrochemical (PEC) systems is promising for unassisted hydrogen production and value-added chemical synthesis, yet organic semiconductor (OS) photoanodes suffer from poor charge extraction and short carrier lifetimes. Here, we address this bottleneck by stabilizing long-lived hole polarons through macroporous tin oxide (mcSnO2) interlayers. Transient absorption spectroscopy reveals that accelerated electron extraction through mcSnO2 stabilizes hole polaron states, substantially prolonging carrier lifetimes. Consequently, the optimized organic photoanodes outperform bare counterparts by more than 5.5-fold, retaining 74% of their initial photocurrent over 15 h for iodide oxidation and 61% over 35 h for ascorbic acid oxidation. Furthermore, integrating this robust organic photoanode with an OS-based photocathode enables the first bias-free organic PEC tandem cell coupling hydrogen evolution with AORs, delivering a remarkable solar-to-hydrogen conversion efficiency of 1.4%. These findings establish interfacial carrier lifetime engineering as an effective strategy for realizing high-performance and durable organic PEC systems.
{"title":"Macroporous Interlayers Stabilize Long-Lived Hole Polarons in Organic Semiconductor Photoanodes","authors":"Eunsong Jeon,Gayoung Ham,Jin Su Park,Hoon Kim,Euimin Lee,Donghyun Lee,Hyuna Kim,Jun-Ho Yum,Kevin Sivula,Hyojung Cha,Han-Hee Cho","doi":"10.1021/acsenergylett.6c02492","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02492","url":null,"abstract":"Integrating alternative oxidation reactions (AORs) into photoelectrochemical (PEC) systems is promising for unassisted hydrogen production and value-added chemical synthesis, yet organic semiconductor (OS) photoanodes suffer from poor charge extraction and short carrier lifetimes. Here, we address this bottleneck by stabilizing long-lived hole polarons through macroporous tin oxide (mcSnO2) interlayers. Transient absorption spectroscopy reveals that accelerated electron extraction through mcSnO2 stabilizes hole polaron states, substantially prolonging carrier lifetimes. Consequently, the optimized organic photoanodes outperform bare counterparts by more than 5.5-fold, retaining 74% of their initial photocurrent over 15 h for iodide oxidation and 61% over 35 h for ascorbic acid oxidation. Furthermore, integrating this robust organic photoanode with an OS-based photocathode enables the first bias-free organic PEC tandem cell coupling hydrogen evolution with AORs, delivering a remarkable solar-to-hydrogen conversion efficiency of 1.4%. These findings establish interfacial carrier lifetime engineering as an effective strategy for realizing high-performance and durable organic PEC systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"87 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221616","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}
Buried-interface engineering is critical for inverted perovskite solar cells, yet integrating anchoring, charge transport, electrostatic regulation, and defect passivation within single molecular systems often creates intrinsic trade-offs. Here, we use cavity-selective host–guest recognition to construct a modular, recognition-directed interface. The cavity of dipolar 4-tert-butylsulfonylcalix[4]arene (tBSCA) selectively accommodates the terminal phenyl group of substrate-anchored Ph-4PACz. Comparisons with a structurally related calixarene analogue and competing inclusion orientations identify a thermodynamically preferred Ph-4PACz-tBSCA configuration, distinguishing cavity-selective association from nonspecific interactions. This preferred configuration underpins a preferentially organized dipolar interface that retains Ph-4PACz-mediated anchoring and charge transport while enabling tBSCA to regulate interfacial electrostatics, reduce interfacial defect sites, and suppress defect-assisted halide migration and interfacial accumulation. The resulting devices achieve a PCE of 27.36% (certified at 26.74%), and a 110 cm2 module delivers a certified efficiency of 22.61%. These results demonstrate configuration-selective molecular recognition as a strategy for the modular organization of complementary functions at buried perovskite interfaces.
{"title":"Cavity-Selective Host–Guest Assembly for Modular Buried-Interface Engineering in Perovskite Solar Cells","authors":"Yunjia Wu,Sihao Huang,Yude Wei,Jiayan Wang,Qiuju Liu,Wenqi Ge,Zhiyang Yan,Yinping Zeng,Yang An,Chaocheng Zhou,Jie Bai,Weihai Sun,Hua Bai","doi":"10.1021/acsenergylett.6c02392","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02392","url":null,"abstract":"Buried-interface engineering is critical for inverted perovskite solar cells, yet integrating anchoring, charge transport, electrostatic regulation, and defect passivation within single molecular systems often creates intrinsic trade-offs. Here, we use cavity-selective host–guest recognition to construct a modular, recognition-directed interface. The cavity of dipolar 4-tert-butylsulfonylcalix[4]arene (tBSCA) selectively accommodates the terminal phenyl group of substrate-anchored Ph-4PACz. Comparisons with a structurally related calixarene analogue and competing inclusion orientations identify a thermodynamically preferred Ph-4PACz-tBSCA configuration, distinguishing cavity-selective association from nonspecific interactions. This preferred configuration underpins a preferentially organized dipolar interface that retains Ph-4PACz-mediated anchoring and charge transport while enabling tBSCA to regulate interfacial electrostatics, reduce interfacial defect sites, and suppress defect-assisted halide migration and interfacial accumulation. The resulting devices achieve a PCE of 27.36% (certified at 26.74%), and a 110 cm2 module delivers a certified efficiency of 22.61%. These results demonstrate configuration-selective molecular recognition as a strategy for the modular organization of complementary functions at buried perovskite interfaces.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"56 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221518","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 : 2026-10-19DOI: 10.1021/acsenergylett.6c01299
Yinggang Qu,Peixue Jiang,Yufan Weng,Ruina Xu
Polymer film capacitors are fundamental to modern power electronics, yet low permittivity restricts their energy density. Although poly(vinylidene fluoride) (PVDF) possesses high intrinsic permittivity, stabilizing its polar structure remains thermodynamically challenging. Here, we report a scalable physical processing strategy to optimize PVDF-based films via a specialized shear-imposed coating methodology. By employing a micro-structured blade, we generate intense local shear flow fields that exert hydrodynamic tension to drive a coil-stretch transition. This process drives an α-to-β phase transition and templates the growth of oriented, polar-phase-rich crystal structures. Furthermore, we develop a stage-wise regulation strategy using binary solvents to orchestrate evaporation dynamics, effectively trapping these metastable shear-induced conformations before relaxation. Effective across the PVDF copolymer family, this method enables P(VDF-HFP) films to achieve a high energy density of 20.05 J/cm3, a 44% improvement over conventional casting. This work provides a general, non-chemical pathway for manufacturing high-performance functional polymers through multi-physical field synergistic regulation.
{"title":"Shear-Driven Structural Ordering Enables High Energy Density in Ferroelectric Polymer Capacitors","authors":"Yinggang Qu,Peixue Jiang,Yufan Weng,Ruina Xu","doi":"10.1021/acsenergylett.6c01299","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01299","url":null,"abstract":"Polymer film capacitors are fundamental to modern power electronics, yet low permittivity restricts their energy density. Although poly(vinylidene fluoride) (PVDF) possesses high intrinsic permittivity, stabilizing its polar structure remains thermodynamically challenging. Here, we report a scalable physical processing strategy to optimize PVDF-based films via a specialized shear-imposed coating methodology. By employing a micro-structured blade, we generate intense local shear flow fields that exert hydrodynamic tension to drive a coil-stretch transition. This process drives an α-to-β phase transition and templates the growth of oriented, polar-phase-rich crystal structures. Furthermore, we develop a stage-wise regulation strategy using binary solvents to orchestrate evaporation dynamics, effectively trapping these metastable shear-induced conformations before relaxation. Effective across the PVDF copolymer family, this method enables P(VDF-HFP) films to achieve a high energy density of 20.05 J/cm3, a 44% improvement over conventional casting. This work provides a general, non-chemical pathway for manufacturing high-performance functional polymers through multi-physical field synergistic regulation.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"16 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218850","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}
Leveraging oxygen redox in lithium-rich layered oxides paves the way for increasing the energy density of lithium-ion batteries, whose practical implementation is plagued by poor stability. Although a uniform Li2MnO3-like domain dispersion is suggested to improve cycle stability, the synthesis–structure relationship governing domain formation remains underexplored. Here, we show that Li2MnO3-like domain dispersion is derived by the precursor structure according to the degree of transition-metal separation. Through a comparative investigation of the synthesis mechanism, we reveal the templating effect that more clustered transition-metal oxide precursors lead to more localized Li2MnO3-like ordering in the final cathodes, a tendency also observed with a different lithium source. Furthermore, it is corroborated that cathodes with more dispersed Li2MnO3-like ordering derived from less-ordered precursors exhibit improved electrochemical stability with a mitigated voltage decay. Our findings highlight the significance of precursor design and engineering for structural regulation of high-performance lithium-rich layered oxide cathodes.
{"title":"Manipulating Li2MnO3-Like Domain Dispersion in Lithium-Rich Layered Oxides Inherited from Precursor","authors":"Woonbae Sohn,Minji Kim,Jin-Hee Bae,Minseo Choi,Hwa-Jung Kim,Yong-Il Kim,Jun-Hyuk Song,Byongyong Yu,Su-Hyun Lee,Hionsuck Baik,Seung-Wook Baek,Seokhee Lee,Hyeokjun Park","doi":"10.1021/acsenergylett.6c02547","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02547","url":null,"abstract":"Leveraging oxygen redox in lithium-rich layered oxides paves the way for increasing the energy density of lithium-ion batteries, whose practical implementation is plagued by poor stability. Although a uniform Li2MnO3-like domain dispersion is suggested to improve cycle stability, the synthesis–structure relationship governing domain formation remains underexplored. Here, we show that Li2MnO3-like domain dispersion is derived by the precursor structure according to the degree of transition-metal separation. Through a comparative investigation of the synthesis mechanism, we reveal the templating effect that more clustered transition-metal oxide precursors lead to more localized Li2MnO3-like ordering in the final cathodes, a tendency also observed with a different lithium source. Furthermore, it is corroborated that cathodes with more dispersed Li2MnO3-like ordering derived from less-ordered precursors exhibit improved electrochemical stability with a mitigated voltage decay. Our findings highlight the significance of precursor design and engineering for structural regulation of high-performance lithium-rich layered oxide cathodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"37 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218852","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 rational combination of multiple electrolyte additives is a promising strategy for constructing stable interphases in lithium-ion batteries. However, unintended additive interactions can alter the preferential reduction/oxidation pathways at electrode surfaces, compromising cell performance. In this study, we identify a detrimental interaction between succinonitrile (SN) and lithium bis(oxalato)borate (LiBOB) on a graphite-silicon (Gr-Si) anode. Specifically, an electron-deficient boron-embedded solid electrolyte interphase (SEI) derived from LiBOB promotes the reduction of the electron-rich nitrile moieties of SN, disrupting fluoroethylene carbonate (FEC)-driven SEI construction. Based on this mechanism, SN was replaced with triisopropanolamine borate (TPAB), which mitigates transition metal dissolution through its amine moiety while forming a robust borate-based cathode electrolyte interphase. Moreover, TPAB combined with LiBOB avoided detrimental side reductions at the anode–electrolyte interface. The FEC-LiBOB-TPAB combination creates thermally stable interphases on the Gr-Si anode and LiNi0.91Co0.08Al0.01O2 cathode (4.8 mAh cm–2), enabling 68.7% capacity retention after 300 cycles at 45 °C and 1C.
多种电解质添加剂的合理组合是构建锂离子电池稳定界面的一种很有前途的策略。然而，意想不到的添加剂相互作用会改变电极表面的优先还原/氧化途径，从而影响电池性能。在这项研究中，我们在石墨硅（Gr-Si）阳极上发现了丁二腈（SN）和硼酸锂（LiBOB）之间的有害相互作用。具体来说，LiBOB衍生的缺电子硼嵌入固体电解质界面（SEI）促进了SN中富电子腈部分的还原，破坏了氟碳酸乙烯（FEC）驱动的SEI结构。基于这一机制，SN被三异丙醇胺硼酸盐（TPAB）取代，TPAB通过其胺部分减轻了过渡金属的溶解，同时形成了坚固的硼酸盐基阴极电解质界面。此外，TPAB与LiBOB的结合避免了阳极-电解质界面的有害侧减少。FEC-LiBOB-TPAB组合在Gr-Si阳极和lini0.91 co0.08 al0.010 o2阴极（4.8 mAh cm-2）上形成热稳定的界面，在45°C和1C下循环300次后，容量保持率达到68.7%。
{"title":"Rational Integration of Multiple Additives for High-Temperature Lithium-Ion Batteries","authors":"Gihoon Lee,Seung Hee Han,Jiwon Seo,Jaehyuk Choi,Sanggil Park,Junyoung Kim,Jae-Seung Kim,Junghyo Lee,Myung-Hoon Kim,Arum Amy Yu,Seungbum Hong,Dong-Hwa Seo,Nam-Soon Choi","doi":"10.1021/acsenergylett.6c02555","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02555","url":null,"abstract":"The rational combination of multiple electrolyte additives is a promising strategy for constructing stable interphases in lithium-ion batteries. However, unintended additive interactions can alter the preferential reduction/oxidation pathways at electrode surfaces, compromising cell performance. In this study, we identify a detrimental interaction between succinonitrile (SN) and lithium bis(oxalato)borate (LiBOB) on a graphite-silicon (Gr-Si) anode. Specifically, an electron-deficient boron-embedded solid electrolyte interphase (SEI) derived from LiBOB promotes the reduction of the electron-rich nitrile moieties of SN, disrupting fluoroethylene carbonate (FEC)-driven SEI construction. Based on this mechanism, SN was replaced with triisopropanolamine borate (TPAB), which mitigates transition metal dissolution through its amine moiety while forming a robust borate-based cathode electrolyte interphase. Moreover, TPAB combined with LiBOB avoided detrimental side reductions at the anode–electrolyte interface. The FEC-LiBOB-TPAB combination creates thermally stable interphases on the Gr-Si anode and LiNi0.91Co0.08Al0.01O2 cathode (4.8 mAh cm–2), enabling 68.7% capacity retention after 300 cycles at 45 °C and 1C.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218851","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 : 2026-10-19DOI: 10.1021/acsenergylett.6c02629
Longyuan Guo,Jiayan Luo
Rechargeable magnesium (Mg) metal batteries are promising high-energy-density alternatives to lithium-ion systems, yet sluggish cathode kinetics hinder their development. Departing from the conventional host-centric view, we demonstrate that reversibility in Mg batteries can be governed by electrolyte-derived reaction chemistry. Here, we harness trace water to impart controlled electrolyte reactivity, enabling electrolyte-derived Mg/Cl-containing species to participate in cathode activation. In tunnel-type MnO2, the regulated electrolyte induces lattice expansion and improves electrochemical reversibility. In organic cathodes, improved rechargeability is consistent with a stabilizing role of Cl– in anion-coupled redox. Because polar-solvent chemistry can irreversibly passivate Mg metal, a Sn/MgCl2 artificial interface suppresses parasitic anode reactions while preserving cathode activation. This strategy enables reversible electrochemistry across oxide, organic, and conversion cathodes, including α/γ-MnO2, methylphenothiazine, tetrathiafulvalene, and hybrid I2/O2 systems. These findings establish electrolyte-derived chemical activation as a guiding principle for regulating cathode reaction pathways in magnesium batteries.
{"title":"Electrolyte-Derived Chemical Activation Enables Reversible Cathode Chemistry in Magnesium Batteries","authors":"Longyuan Guo,Jiayan Luo","doi":"10.1021/acsenergylett.6c02629","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02629","url":null,"abstract":"Rechargeable magnesium (Mg) metal batteries are promising high-energy-density alternatives to lithium-ion systems, yet sluggish cathode kinetics hinder their development. Departing from the conventional host-centric view, we demonstrate that reversibility in Mg batteries can be governed by electrolyte-derived reaction chemistry. Here, we harness trace water to impart controlled electrolyte reactivity, enabling electrolyte-derived Mg/Cl-containing species to participate in cathode activation. In tunnel-type MnO2, the regulated electrolyte induces lattice expansion and improves electrochemical reversibility. In organic cathodes, improved rechargeability is consistent with a stabilizing role of Cl– in anion-coupled redox. Because polar-solvent chemistry can irreversibly passivate Mg metal, a Sn/MgCl2 artificial interface suppresses parasitic anode reactions while preserving cathode activation. This strategy enables reversible electrochemistry across oxide, organic, and conversion cathodes, including α/γ-MnO2, methylphenothiazine, tetrathiafulvalene, and hybrid I2/O2 systems. These findings establish electrolyte-derived chemical activation as a guiding principle for regulating cathode reaction pathways in magnesium batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"28 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218855","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 : 2026-10-19DOI: 10.1021/acsenergylett.6c02922
Gauri Sharma,Rahul Mahavir Varma,Shruti Singh,Suman Kundu,Rachna Singh,Rajdeep Das,Debarjya Ganguly,Ushita Roy,Rupam Ghosh,Sasank Pattnaik,Frans P. Widdershoven,Håkan Rensmo,Arindam Chowdhury,Sameer Sapra,Pralay K. Santra
A modified colloidal atomic layer deposition at room temperature grows a vacancy-ordered Cs2SnCl6 shell epitaxially on CsPbCl3 nanocrystals, avoiding the core degradation and parasitic shell nucleation that accompany high-temperature routes. The resulting core–shell nanocrystals achieve an absolute photoluminescence quantum yield of 62% and retain 65% of their emission after six months of ambient storage and 30% after 48 h of exposure to added water.
{"title":"Colloidal ALD Epitaxial Shelling Enhances Stability and Photoluminescence of Blue Perovskite Nanocrystals","authors":"Gauri Sharma,Rahul Mahavir Varma,Shruti Singh,Suman Kundu,Rachna Singh,Rajdeep Das,Debarjya Ganguly,Ushita Roy,Rupam Ghosh,Sasank Pattnaik,Frans P. Widdershoven,Håkan Rensmo,Arindam Chowdhury,Sameer Sapra,Pralay K. Santra","doi":"10.1021/acsenergylett.6c02922","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02922","url":null,"abstract":"A modified colloidal atomic layer deposition at room temperature grows a vacancy-ordered Cs2SnCl6 shell epitaxially on CsPbCl3 nanocrystals, avoiding the core degradation and parasitic shell nucleation that accompany high-temperature routes. The resulting core–shell nanocrystals achieve an absolute photoluminescence quantum yield of 62% and retain 65% of their emission after six months of ambient storage and 30% after 48 h of exposure to added water.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"55 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218854","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}
Abstract Rational molecular engineering of the perovskite/hole transport layer interface offers a promising route to simultaneously address inefficient charge extraction, defect-mediated recombination, and lead leakage in CsPbI3–xBrx perovskite solar cells. Herein, we introduce 2,2′-dinitro-9,9′-spirobifluorene (DN-SBF) as an interfacial molecular bridge to tackle these challenges. DN-SBF optimizes energy level alignment, establishes π–π interactions, and forms exciplexes with Spiro-OMeTAD, thereby facilitating interfacial charge transport. Meanwhile, DN-SBF passivates undercoordinated Pb2+ through multiple coordination modes, including robust bidentate chelation formed by adjacent nitro groups, effectively passivating defects and suppressing non-radiative recombination. Importantly, multipoint coordination immobilizes leachable Pb2+, substantially mitigating lead leakage and improving film biocompatibility. As a result, DN-SBF-engineered CsPbI3–xBrx devices achieve a champion power conversion efficiency of 22.40% along with significantly enhanced operational and environmental stability. This work highlights the potential of versatile molecular bridges to concurrently enhance performance, stability, and eco-friendliness, which may contribute to the development of more sustainable perovskite photovoltaics.
{"title":"Exciplex-Facilitated Charge Extraction and Defect Chelation to Improve Inorganic Perovskite Solar Cells","authors":"Tianxiang Zhou,Wenshi Zhao,Rui Li,Qiyong Chen,Kuo Wang,Guiyong Yin,Hongcan Yu,Qi Zhang,Xianghan Feng,Dong Liang,Yang Liu,Qingwen Tian,Shengzhong (Frank) Liu","doi":"10.1021/acsenergylett.6c01037","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01037","url":null,"abstract":"Abstract Rational molecular engineering of the perovskite/hole transport layer interface offers a promising route to simultaneously address inefficient charge extraction, defect-mediated recombination, and lead leakage in CsPbI3–xBrx perovskite solar cells. Herein, we introduce 2,2′-dinitro-9,9′-spirobifluorene (DN-SBF) as an interfacial molecular bridge to tackle these challenges. DN-SBF optimizes energy level alignment, establishes π–π interactions, and forms exciplexes with Spiro-OMeTAD, thereby facilitating interfacial charge transport. Meanwhile, DN-SBF passivates undercoordinated Pb2+ through multiple coordination modes, including robust bidentate chelation formed by adjacent nitro groups, effectively passivating defects and suppressing non-radiative recombination. Importantly, multipoint coordination immobilizes leachable Pb2+, substantially mitigating lead leakage and improving film biocompatibility. As a result, DN-SBF-engineered CsPbI3–xBrx devices achieve a champion power conversion efficiency of 22.40% along with significantly enhanced operational and environmental stability. This work highlights the potential of versatile molecular bridges to concurrently enhance performance, stability, and eco-friendliness, which may contribute to the development of more sustainable perovskite photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"16 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209875","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}
Abstract Conventional carbonization of semi-coke induces excessive ordering of aromatic skeletons, producing dense graphitic structures that hinder Na+ intercalation and suppress low-potential plateau capacity. Here, we develop a rapid thermomechanical coupling sintering strategy using moderate pressure to drive π–π interactions and topological reconfiguration of aromatic units. This process suppresses excessive graphitization while constructing interconnected, twisted pseudo-graphitic domains with abundant closed nanopores. At 1000 mA g–1, PTR-HC reaches 80% SOC in ≈14.4 min and retains 90.1% of its plateau capacity, enabled by abundant Na+ storage sites and rapid diffusion pathways. Kinetic analyses reveal accelerated Na+ transport and a thin, NaF-rich solid-electrolyte interphase with fewer organic components. In situ XRD and Raman attribute slope capacity to surface/defect adsorption and intercalation and the plateau capacity to quasi-metallic Na clusters in closed pores. This work establishes pressure-driven topological engineering as a promising strategy for upgrading semi-coke into fast-charging hard carbon with high plateau-capacity retention.
半焦的常规炭化会导致芳香骨架过度有序，产生致密的石墨结构，阻碍Na+嵌入，抑制低电位平台容量。在这里，我们开发了一种快速的热-机械耦合烧结策略，使用中等压力来驱动π -π相互作用和芳香单元的拓扑重构。这一过程抑制了过度的石墨化，同时构建了具有丰富封闭纳米孔的相互连接的扭曲伪石墨畴。在1000 mA g-1下，PTR-HC在约14.4 min内达到80%的SOC，并保持了90.1%的平台容量，这得益于丰富的Na+存储位点和快速的扩散途径。动力学分析揭示了加速的Na+传输和薄的富含naf的固体电解质界面，有机成分较少。原位XRD和Raman表征了表面/缺陷吸附和插层的斜坡能力和封闭孔隙中准金属Na团簇的高原能力。这项工作建立了压力驱动的拓扑工程作为一种有前途的策略，将半焦升级为具有高平台容量保留的快速充电硬碳。
{"title":"Pressure-Driven Topological Reconfiguration toward Fast-Charging Hard Carbon with Plateau-Capacity Retention","authors":"Rong-Jie Zhe,Zhen-Yi Gu,Kai-Yang Zhang,Zhi-Zhu Liu,Xin-Yu Wang,Shuo-Hang Zheng,Yu Zhang,Jingping Zhang,Xing-Long Wu","doi":"10.1021/acsenergylett.6c02684","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02684","url":null,"abstract":"Abstract Conventional carbonization of semi-coke induces excessive ordering of aromatic skeletons, producing dense graphitic structures that hinder Na+ intercalation and suppress low-potential plateau capacity. Here, we develop a rapid thermomechanical coupling sintering strategy using moderate pressure to drive π–π interactions and topological reconfiguration of aromatic units. This process suppresses excessive graphitization while constructing interconnected, twisted pseudo-graphitic domains with abundant closed nanopores. At 1000 mA g–1, PTR-HC reaches 80% SOC in ≈14.4 min and retains 90.1% of its plateau capacity, enabled by abundant Na+ storage sites and rapid diffusion pathways. Kinetic analyses reveal accelerated Na+ transport and a thin, NaF-rich solid-electrolyte interphase with fewer organic components. In situ XRD and Raman attribute slope capacity to surface/defect adsorption and intercalation and the plateau capacity to quasi-metallic Na clusters in closed pores. This work establishes pressure-driven topological engineering as a promising strategy for upgrading semi-coke into fast-charging hard carbon with high plateau-capacity retention.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"7 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209878","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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