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Ultrafast Interphase Exciton Funneling in Alternating-Cation 2D Perovskites through Förster-Type Energy Transfer 通过Förster-Type能量传递在交替阳离子二维钙钛矿中的超快间相激子漏斗
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc06761a
SUPRIYA GHOSH,Bapi Pradhan,Johan Hofkens,Tönu Pullerits,Christian Sternemann,Peiran Wang,Heinz Amenitsch,Sumea Klokic,Pavel Chábera
{"title":"Ultrafast Interphase Exciton Funneling in Alternating-Cation 2D Perovskites through Förster-Type Energy Transfer","authors":"SUPRIYA GHOSH,Bapi Pradhan,Johan Hofkens,Tönu Pullerits,Christian Sternemann,Peiran Wang,Heinz Amenitsch,Sumea Klokic,Pavel Chábera","doi":"10.1039/d6sc06761a","DOIUrl":"https://doi.org/10.1039/d6sc06761a","url":null,"abstract":"Efficient exciton transport is central to the development of low-dimensional semiconductors for optoelectronic applications. Layered metal halide perovskites provide a versatile platform for regulating excitonic interactions through spacer-layer engineering. Here, we demonstrate that alternating-cation-in-interlayer (ACI) perovskites exhibit markedly rapid interphase exciton funneling compared with conventional Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) architectures. Using femtosecond transient absorption and time-resolved photoluminescence spectroscopy, complemented by full-spectrum global analysis, we reveal rapid exciton transfer from lower-n toward higher-n quantum wells. The concomitant decay of lower-n excitonic signals and growth of higher-n features, together with the species-associated spectral evolution, are consistent with a predominantly Förster-type interphase energy-transfer mechanism. The characteristic early-time dynamics correlate with shorter interlayer spacing along the stacking direction, suggesting that spacer-layer architecture contributes to modulation of interphase excitonic coupling. While differences in phase distribution, spectral overlap, and domain morphology may additionally influence the measured dynamics, these results establish spacer-layer engineering as an effective strategy for regulating ultrafast energy flow in layered excitonic semiconductors.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"1 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc06148f
Denis Hartmann,Artemijs Krimovs,Oussama Errida,Tiberiu-M Gianga,Giuliano Siligardi,Robert Pal,Timothy Andrew Barendt
{"title":"","authors":"Denis Hartmann,Artemijs Krimovs,Oussama Errida,Tiberiu-M Gianga,Giuliano Siligardi,Robert Pal,Timothy Andrew Barendt","doi":"10.1039/d6sc06148f","DOIUrl":"https://doi.org/10.1039/d6sc06148f","url":null,"abstract":"The self-assembly of chiral organic dyes provides an effective route to strongly chiral optical materials. Herein, we report a novel coronene diimide derivative with point-chiral imide groups derived from L/D-valinol. This chiral chromophore shows solvent-dependent aggregation and readily self-assembles via π-stacking into strongly chiroptically active materials, effectively translating point chirality into supramolecular chirality in the assembly. These properties are retained in the solid state, with thin films of these molecules showing strong circular dichroism (CD) and circularly polarised luminescence (CPL), realising easily accessible point chirality as a structural element for chiroptical materials.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"471 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152719","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Persistent Functionalized Triarylmethyl Radicals: when Spin meets Chirality 持续功能化三芳基甲基自由基:当自旋遇到手性时
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc06418c
Imma Ratera,Jaume Veciana,Paula Mayorga-Burrezo
{"title":"Persistent Functionalized Triarylmethyl Radicals: when Spin meets Chirality","authors":"Imma Ratera,Jaume Veciana,Paula Mayorga-Burrezo","doi":"10.1039/d6sc06418c","DOIUrl":"https://doi.org/10.1039/d6sc06418c","url":null,"abstract":"For decades, persistent trityl radical derivatives have been the object of intense research in a wide variety of disciplines, ranging from fundamental to applied science, thanks to the versatility of their properties (magnetic, optical, redox, etc.) and their potential as multifunctional open-shell building blocks. Nonetheless, far from becoming less appealing after such extensive study, these propeller-shaped radicals are nowadays gaining momentum thanks to their intrinsic chirality, which arises from the clockwise or counterclockwise torsion of their aryl rings. Indeed, increasing attention is being devoted to the implications of combining this feature with other properties, such as magnetism, enabling applications such as EPR probes, spin-dependent electronic transport through the CISS effect, and quantum technologies. From an optical perspective, their performance as circularly polarized light emitters has emerged as one of the most promising research directions. In this review, we present the advances made in understanding and exploiting the handedness of trityl-based radicals, from tetrathiatriarylmethyl radicals to halogen-shielded derivatives, covering the evolution from intrinsic propeller chirality to more complex diastereomeric systems resulting from their functionalization with additional chiral centers, axes, and planes, as well as the incorporation of additional propeller units into multipropeller architectures or their involvement in chiral supramolecular assemblies. Finally, we discuss how these advances are shaping emerging applications.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"49 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc03126a
Karen Lizbeth Valadez-Villalobos,Rodrigo Garcia Rodriguez,Rhys Gareth Charles,Matthew L Davies
{"title":"","authors":"Karen Lizbeth Valadez-Villalobos,Rodrigo Garcia Rodriguez,Rhys Gareth Charles,Matthew L Davies","doi":"10.1039/d6sc03126a","DOIUrl":"https://doi.org/10.1039/d6sc03126a","url":null,"abstract":"The sustainability of photovoltaic technologies cannot be assessed independently of their absorber chemistry. In this Perspective, we compare crystalline silicon (c-Si), cadmium telluride (CdTe) and halide perovskites, tracing how their fundamental optoelectronic and chemical properties shape material demand, manufacturing, operational stability and end-of-life pathways. Silicon has an indirect bandgap and limited defect tolerance which necessitates thick wafers, ultra-high-purity feedstocks and energy- and capital-intensive processing. Its chemically robust and insoluble structure supports long operational lifetimes but complicates material recovery. By contrast, the strong absorption and greater defect tolerance of CdTe and halide perovskites enable thin-film architectures, lower absorber-material requirements and potentially less intensive manufacturing and recovery processes. These advantages are accompanied by distinct challenges, including tellurium criticality and cadmium toxicity for CdTe, and limited stability and lead management for perovskites. No absorber choice is intrinsically sustainable: progress requires the coordinated optimisation of performance, durability, resource availability, manufacturing and circularity across the complete photovoltaic lifecycle.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"3 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Engineering peroxygenases for pharmaceutical applications: recent advances and future perspectives 工程过氧酶在制药中的应用:最新进展和未来展望
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc04536g
Lilin Feng,Atul Kumar,Ulrich Schwaneberg,Marisa Sárria Pereira de Passos
{"title":"Engineering peroxygenases for pharmaceutical applications: recent advances and future perspectives","authors":"Lilin Feng,Atul Kumar,Ulrich Schwaneberg,Marisa Sárria Pereira de Passos","doi":"10.1039/d6sc04536g","DOIUrl":"https://doi.org/10.1039/d6sc04536g","url":null,"abstract":"Selective oxidation is a cornerstone process in pharmaceutical biosynthesis, as it enables the conversion of inert C–H bonds into valuable functional groups such as alcohols, ketones, epoxides, and carboxylic acids, which serve as important intermediates in drug synthesis. Peroxygenases, including unspecific peroxygenases and P450 peroxygenases, have emerged as powerful biocatalysts for enzymatic oxidation, with growing applications in metabolite synthesis, late-stage C–H functionalization, and the preparation of enantioenriched intermediates for pharmaceutical development. In this review, we present the latest advances in peroxygenases engineering for pharmaceutical applications. We summarize pharmaceutical drug candidates that can serve as substrates for peroxygenases, discuss the enzymatic oxidation pathways mediated by peroxygenases for these substrates, and outline protein engineering strategies employed to improve the catalytic performance and properties of peroxygenases in pharmaceutical biosynthesis. We also discuss the potential of emerging artificial intelligence (AI) strategies for multi-dimensional peroxygenase engineering including catalytic activity, thermostability, hydrogen peroxide tolerance, heterologous expression, substrate scope, regioselectivity, and enantioselectivity. Overall, continued progress in peroxygenase engineering will drive the transformation of these biocatalysts for versatile industrial applications, thereby enabling sustainable drug synthesis, efficient metabolite production, and innovative therapeutic strategies.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"7 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152730","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Accelerating the Discovery of Nanoporous Gas Separation Materials via Coulomb-Enhanced Classical Density Functional Theory 利用库仑增强经典密度泛函理论加速纳米多孔气体分离材料的发现
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc04283j
Yong Qiu,Yun Tian,Yu Liu,Weiqiang Tang,Zhen Zhou
{"title":"Accelerating the Discovery of Nanoporous Gas Separation Materials via Coulomb-Enhanced Classical Density Functional Theory","authors":"Yong Qiu,Yun Tian,Yu Liu,Weiqiang Tang,Zhen Zhou","doi":"10.1039/d6sc04283j","DOIUrl":"https://doi.org/10.1039/d6sc04283j","url":null,"abstract":"The design of advanced nanoporous materials for gas separations, such as carbon capture and alkyne purification, is increasingly driven by high-throughput screening. However, the accurate description of electrostatic interactions in porous frameworks remains challenging and can introduce sizable deviations between predicted and experimental performance, thereby hindering rational materials design. To address this gap, we present a computational framework, compatible with standard force fields under appropriate charge assignments, that explicitly incorporates a point-charge model to capture adsorbate-framework long-range Coulomb interactions via the Ewald summation technique within the external potential of classical density functional theory (cDFT), enabling adsorption prediction for common polar or quadrupolar gas molecules. The resulting Coulomb-enhanced cDFT (QcDFT) shows closer agreement with GCMC and experimental adsorption data than existing cDFT variants, and was applied to 690 CO2/MOF adsorption cases and nearly 10,000 CoRE MOF 2019 structures for C2H2/CO2 screening. By further integrating the string method, QcDFT allows for efficient prediction of adsorption selectivity and rapid estimation of self-diffusion coefficients, achieving up to three orders of magnitude acceleration relative to conventional molecular dynamics simulations. This combination of speed and accuracy makes QcDFT well suited to large-scale nanoporous materials screening, bridging atomic-scale adsorption mechanisms with separation-relevant candidate selection.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"232 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152727","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mesoporous AgSe as a model n-type thermoelectric: soft-templated synthesis and thermal transport engineering 介孔AgSe作为模型n型热电材料:软模板合成与热输运工程
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc05923f
Zihao Yang,Minsu Han,Jihyun Kim,Ho Ngoc Nam,Quan Manh Phung,Young Jun Lee,Norman C.-R. Chen,Xiangyang Liu,Yuqi Guo,Yingji Zhao,Yunqing Kang,Kevin C.-W. Wu,Yusuke Asakura,Byeonggwan Kim,Yusuke Yamauchi
{"title":"Mesoporous AgSe as a model n-type thermoelectric: soft-templated synthesis and thermal transport engineering","authors":"Zihao Yang,Minsu Han,Jihyun Kim,Ho Ngoc Nam,Quan Manh Phung,Young Jun Lee,Norman C.-R. Chen,Xiangyang Liu,Yuqi Guo,Yingji Zhao,Yunqing Kang,Kevin C.-W. Wu,Yusuke Asakura,Byeonggwan Kim,Yusuke Yamauchi","doi":"10.1039/d6sc05923f","DOIUrl":"https://doi.org/10.1039/d6sc05923f","url":null,"abstract":"Mesoporous structuring is a promising route to suppress thermal conductivity in thermoelectrics by enhancing phonon scattering, yet mesoporous thermoelectric materials remain scarcely explored. Here, we report the synthesis and thermoelectric evaluation of mesoporous Ag2Se as a model n-type system. Mesoporous Ag2Se thin films are obtained by block-copolymer-directed soft-templated electrodeposition using PS-b-PEO micelles, which interact with Ag+ and Se(iv) species and direct the formation of orthorhombic β-Ag2Se frameworks with a high density of mesopores. By tuning the molecular weight of copolymers and applying an optimized deposition potential of −0.48 V vs. Hg/Hg2SO4 (saturated K2SO4), we realize narrowly distributed pore diameters of 8, 12, and 16 nm and a concomitant deposition in crystallite size. The films are delaminated from ITO substrates and pressed into pellets while preserving both the mesoporous architecture and the β-Ag2Se lattice. For the Ag2Se-12 nm sample, the thermal conductivity at room temperature is reduced from 0.93 W m−1 K−1 for nonporous Ag2Se to 0.40 W m−1 K−1, with moderate degradation of the power factor, resulting in a room-temperature zT of 0.98 (56% enhancement). These results establish mesostructural engineering in Ag2Se as an effective strategy to reduce the thermal conductivity, providing a design principle for next-generation thermoelectrics.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"11 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152729","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
When carbonyls beat aromaticity: An additive framework for predicting tautomeric preferences 当羰基击败芳香性:预测互变异构偏好的加性框架
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc03354g
Felipe Fantuzzi,Pierre Mothe Esteves,Lucas Araujo,Thiago M. Cardozo
{"title":"When carbonyls beat aromaticity: An additive framework for predicting tautomeric preferences","authors":"Felipe Fantuzzi,Pierre Mothe Esteves,Lucas Araujo,Thiago M. Cardozo","doi":"10.1039/d6sc03354g","DOIUrl":"https://doi.org/10.1039/d6sc03354g","url":null,"abstract":"Aromatic structures are often regarded as privileged stabilising motifs, generally retained even when competing structural effects are present. Here, we show that functional-group energetics can overturn this expectation in heteroaromatic tautomerism. Analysis of the 2-hydroxypyridine/2-pyridone equilibrium reveals a near-cancellation between carbonyl stabilisation and the energetic penalty associated with perturbing the aromatic ring framework, accounting for the small experimental energy gap. Extending this approach to pyridines, diazines, and triazines reveals a simple additive pattern: hydroxy/carbonyl exchange favours carbonylated, non-aromatic tautomers, typically requiring two C=O/N–H units to invert the preference, whereas amino/imine and methyl/methylidene exchanges reinforce aromatic tautomers. Spin-coupled generalised valence bond (SCGVB) calculations analysed within the GPF-EP energy decomposition scheme show that the quasi-classical component favours the aromatic 6c–6e π framework, whereas quantum interference favours localised 2c–2e bonds, especially C=O. This provides an energy-decomposition expression of π-distortivity: without interference, the aromatic tautomers would predominate across all series. Complementary NBO analysis suggests that this trend reflects stronger lactam-type donor--acceptor delocalisation in carbonylated $N$-heteroaromatic tautomers than in the corresponding imine, methylidene, or all-carbon benzenoid keto analogues. The model rationalises benzenoid phenols as boundary cases and predicts tautomeric preferences along the deamination pathway from melamine to cyanuric acid. These results establish a framework for predicting tautomeric preferences and clarify how aromatic-ring stabilisation is balanced against functional-group energetics.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"37 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Facile Synthesis of Closed-loop Recyclable and Crystalline Stereoregular Poly(ether--ester)s from Bio-based Commodity Chemicals 基于生物基商品化学品的闭环可回收结晶立体规则聚醚酯的简易合成
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc06571f
tianqi li,Dongfang Zhao,Sifan Ji,Shaofeng Liu,Zheng Li,Zhibo Li
{"title":"Facile Synthesis of Closed-loop Recyclable and Crystalline Stereoregular Poly(ether--ester)s from Bio-based Commodity Chemicals","authors":"tianqi li,Dongfang Zhao,Sifan Ji,Shaofeng Liu,Zheng Li,Zhibo Li","doi":"10.1039/d6sc06571f","DOIUrl":"https://doi.org/10.1039/d6sc06571f","url":null,"abstract":"The microstructure of closed-loop recyclable polyesters, including substituent pattern, stereoregularity, and sequence distribution, plays a pivotal role in determining their thermal and mechanical properties. While stereoregular recyclable polyesters exhibit significantly enhanced overall performance, large-scale access to these materials remains challenging. Herein, we report a scalable one-pot synthesis of enantiopure 3-methyl-1,4-dioxan-2-one (αMDO) from bio-based commodity methyl lactate and ethylene oxide. Further controlled ring-opening polymerization (ROP) of the enantiopure αMDO proceeds with retention of the monomer stereochemistry, yielding semicrystalline closed-loop polyesters with melting temperature up to 100 °C, substantially higher than those of polyesters derived from γ- and δ-substituted MDOs. Moreover, thermodynamic investigations reveal that αMDO exhibits more favorable polymerization thermodynamics than γ- and δ-substituted MDOs, enabling controlled ROP under milder conditions. Crucially, the polyesters enable efficient bulk depolymerization to recover the pristine enantiopure monomer, thus offering a practical pathway toward formation of high-performance, closed-loop recyclable polyesters from sustainable commodity feedstocks.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"10 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152726","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Symmetric dual-interphase design enables stable lithium-metal anodes for high rate ultrahigh-nickel all-solid-state batteries 对称双界面设计为高倍率超高镍全固态电池提供稳定的锂金属阳极
IF 8.4 1区 化学
Chemical Science Pub Date : 2026-10-13 DOI: 10.1039/d6sc06840e
Chen Liu,Zhuolin Zhong,Lin Li,Siwu Li,Qiyue Luo,Haojie Zhang,Xia Chen,Chuang Yu,Kai Jiang
{"title":"Symmetric dual-interphase design enables stable lithium-metal anodes for high rate ultrahigh-nickel all-solid-state batteries","authors":"Chen Liu,Zhuolin Zhong,Lin Li,Siwu Li,Qiyue Luo,Haojie Zhang,Xia Chen,Chuang Yu,Kai Jiang","doi":"10.1039/d6sc06840e","DOIUrl":"https://doi.org/10.1039/d6sc06840e","url":null,"abstract":"Ultrahigh-nickel all-solid-state lithium metal batteries (ASSLMBs) are promising for high-energy storage, yet their high-rate operation is limited by unstable sulfide electrolyte/lithium metal interfaces. The large lithium flux generated by LiNi0.9Mn0.05Co0.05O2 (NCM955) cathodes aggravates interfacial side reactions, nonuniform current distribution, and dendrite-induced short circuits, making stable cycling beyond 1C difficult. Herein, an asymmetric dual-interphase design is developed to regulate the ion-transport and electron-reaction processes at the sulfide/lithium interface. A highly ion-conductive Li–Al alloy is introduced on the electrolyte side to reduce interfacial transport resistance, while an in situ evolved Ta/Li hybrid phase is constructed on the lithium metal side to enhance electronic delocalization, homogenize the current distribution, and regulate lithium deposition. This cooperative interphase design increases the critical current density to 4.8 mA cm−2 and enables stable high-rate cycling of NCM955-based ASSLMBs. The full cell delivers an initial discharge capacity of 193.2 mAh g−1 and operates for 500 cycles at 1.25C without short circuiting; even at 2.5C, it maintains stable cycling for 170 cycles with an initial capacity of 144.3 mAh g−1.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"31 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149152731","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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