{"title":"Single-atom catalysts for electrochemical CO2 reduction across concentrated, dilute, and capture-derived (bi)carbonate feed conditions","authors":"Jae Hak Kim,Joonhee Ma,Soo Young Kim","doi":"10.1039/d6ta07869a","DOIUrl":"https://doi.org/10.1039/d6ta07869a","url":null,"abstract":"Single-atom catalysts (SACs) provide a versatile platform for electrochemical CO2 reduction through precise control of isolate metal centers and their surrounding environments. However, their performance depends on the carbon feed, raising questions about the applicability of catalyst design principle developed under conventional conditions to more practical carbon sources. This review discusses SACs across concentrated CO2, dilute CO2, and capture-derived (bi)carbonate electrolysis, emphasizing how changes in feed conditions reshape catalytic requirements. Representative synthesis methods and reaction fundamentals are outlined, follwed by a discussion of catalyst engineering strategies and their relevance to each reaction environment. The relationships among active-site properties, reactant availability, and the local reaction environment are examined across these feed conditions. Current challenges and future directions for practical implementation are also discussed. This review highlights the need to adapt SAC design to carbon-feed characterizations, providing guidance for efficient and practical electrochemical carbon utilization.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"232 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Lewis Acid-Base Regulated Novel Eutectic Electrolyte of 1,4-Butane Sultone and LiTFSI Enables High-Voltage Lithium Metal Batteries via F/S-Rich Interphases","authors":"Yunyun Lei,Huijie Tian,Binyi Chen,Fengyi Liu,Xiang Li,Yejun Qiu,Wei Gan,Qunhui Yuan","doi":"10.1039/d6ta05374b","DOIUrl":"https://doi.org/10.1039/d6ta05374b","url":null,"abstract":"Conventional carbonate electrolytes oxidatively decompose at high voltages, limiting the cycling life of lithium metal batteries (LMBs). Herein, we report a deep eutectic electrolyte (DEE) composed of 1,4-butane sultone (BS) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), in which BS coordinates with Li⁺ through its S=O group via Lewis acid–base interactions to promote LiTFSI dissociation. The sulfonate group in BS enables DEE to exhibit good compatibility with Li and robust oxidative stability under high-voltage operation. Its effective decomposition promotes the formation of F/S-rich interphases with an ultrathin cathode electrolyte interface (CEI) of ~6 nm, synergistically boosting interfacial ionic conductivity and mechanical stability. Consequently, Li||Li symmetric cells sustain stable stripping/plating for over 2,000 hours. LiCoO2||Li cells achieve 81.7% capacity retention after 1,000 cycles at 0.5C with a 4.3 V cutoff. At elevated cutoff voltages of 4.5 V and 4.6 V (1C), the cells retain 83.6% capacity after 500 cycles and 83.2% after 300 cycles, respectively, far outperforming cells with commercial carbonate electrolytes. Even at 50 ℃, the capacity loss remains only 19.2% after 800 cycles. This work highlights the potential of sulfonate-based DEEs for high-voltage, high-temperature and long-life LMBs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"82 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173187","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shengqiang Cui,Jie Zheng,Ruiheng Li,Jubo Tang,Shuangyuan Li,Ran Ang
{"title":"Cu-Doping-Driven Texture and Transport Anisotropy Engineering in n-type Bi2Te3-Based Thermoelectrics","authors":"Shengqiang Cui,Jie Zheng,Ruiheng Li,Jubo Tang,Shuangyuan Li,Ran Ang","doi":"10.1039/d6ta07457j","DOIUrl":"https://doi.org/10.1039/d6ta07457j","url":null,"abstract":"Bi2Te3-based alloys are the only commercially established thermoelectric materials for near-room-temperature applications, yet high-performance texturing of n-type alloys typically requires complex hot deformation, which can cause Te volatilization and performance instability. In this work, we demonstrate a facile Cu-doping strategy to simultaneously regulate carrier transport and enhance texture in Te-rich n-type Bi2Te2.9Se0.3 without post-deformation processing. Cu promotes preferential grain growth along the ab plane and strengthens c-axis orientation, while excess Cu forms Cu-Te secondary phases. Cu doping reverses the electrical conductivity anisotropy, while the enhanced in-plane Seebeck coefficient compensates for the reduced conductivity, yielding an improved power factor. Meanwhile, point defects and interfacial scattering suppress lattice thermal conductivity. Consequently, the optimized Cu0.03Bi2Te2.9Se0.3 achieves a peak in-plane zT of ~1.02 at 350 K and a room-temperature zT of 0.97, representing a ~140% enhancement over the pristine sample. A 7-pair device delivers a conversion efficiency of 5.1% at ΔT = 197 K. This work provides a simple, low-cost route to texture and transport optimization of n-type Bi2Te3-based thermoelectrics.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"33 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173185","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Highly-efficient and rapidly-fabricated dye-sensitized solar cells through molecular design of the Cu-complex hole-transport material","authors":"Meiyi Chen,Yue Hu,Neil Robertson","doi":"10.1039/d6ta07596g","DOIUrl":"https://doi.org/10.1039/d6ta07596g","url":null,"abstract":"Solid-state dye-sensitized solar cells (ssDSSCs) are promising for indoor energy harvesting, yet their fabrication and performance are limited by their coordination-complex hole-transport materials (HTMs). The effects of intermolecular packing and inner-sphere reorganization during redox both arise from the structural design of the coordination environment. Here, we show that ligand steric engineering provides a strategy to control these structural effects. By extending the 6,6′-substituents from methyl to butyl in a Cu(I)/Cu(II) diimine redox couple crystallization is inhibited, while coordination-sphere flexibility is also suppressed, leading to reduced geometric distortion upon oxidation. Thin-film diffraction and microscopy demonstrate the formation of amorphous, uniformly infiltrated networks under device-relevant conditions. This enables uniquely rapid and simple fabrication of efficient ssDSSCs, exhibiting power conversion efficiencies exceeding 10% under one-sun illumination and approximately 34% at 1000 lux under indoor illumination. These results establish steric control of intermolecular interactions as a transformative approach in coordination-complex HTMs and open up a new phase of ssDSSC development and application.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"90 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173181","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bolun Zhang,Dongliang Jia,Hongtao Yan,Xinming Guo,Dan Tan
{"title":"Flexoelectric Modulation of Photovoltaic Performance in Two-Dimensional CuInPS: Enhanced Shift Current, Carrier Separation, and Power Conversion Efficiency","authors":"Bolun Zhang,Dongliang Jia,Hongtao Yan,Xinming Guo,Dan Tan","doi":"10.1039/d6ta06229f","DOIUrl":"https://doi.org/10.1039/d6ta06229f","url":null,"abstract":"Two-dimensional ferroelectrics hold exceptional promise for photovoltaic energy conversion owing to their intrinsic bulk photovoltaic effect, yet effective strategies for continuously tuning their photovoltaic performance remain limited. Here, we demonstrate that mechanical bending through the flexoelectric coupling between strain gradients and polarization provides a continuous and reversible strategy for enhancing the photovoltaic functionality of monolayer CuInP2S6 (CIPS). We develop an analytical model for the flexoelectric polarization and quantitatively determine the dominant flexoelectric coefficient. Using density functional theory and Wannier interpolation, we show that uniaxial bending generates an in-plane flexoelectric polarization that amplifies the shift-current conductivity σ^yyy by factors of 1.66–2.23 across the visible-to-ultraviolet spectrum, associated with bending-induced modifications of the Bloch wavefunctions and momentum-resolved interband optical response, accompanied by a pronounced redistribution of the Berry curvature. Meanwhile, the flexoelectric field generates an electrostatic asymmetry between the compressive and tensile surfaces that compresses the conduction band offset from 0.20 to 0.14 eV and establishes a type-II band alignment, promoting spatial separation of photogenerated carriers, while the strain-gradient-modulated band dispersion enhances carrier mobility, particularly for holes (by up to 32%). Separately, a modified Scharber-type estimate based on the PBE bandgap and effective surface-to-surface conduction-band offset yields a comparative PCE proxy that increases to 12.2% with bending. This estimate does not explicitly incorporate the intrinsic shift-current response. This work identifies flexoelectricity as a versatile tuning strategy for the photovoltaic performance of two-dimensional ferroelectrics and provides quantitative materials design guidance for strain-gradient-engineered optoelectronic devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"13 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173180","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"DFT-assisted multiscale descriptor analysis of gas adsorption behavior on rare-earth-doped SnO","authors":"Yufei Li,Mingyang Shi,Tao Wu,Tao Gao","doi":"10.1039/d6ta07449a","DOIUrl":"https://doi.org/10.1039/d6ta07449a","url":null,"abstract":"Gas sensors play a critical role in environmental monitoring, industrial safety, and medical diagnostics, highlighting the need for efficient and cost-effective sensing materials. By combining machine learning (ML) with density functional theory (DFT), we systematically investigated the adsorption mechanisms of target gases (CH4, H2, CO, and NH3) on rare-earth-doped SnO2 surfaces (Ln-SnO2). Our work successfully predicted the adsorption energies of target gases across various doped systems and identified the important electronic and structural factors influencing adsorption strength based on a random forest model. Furthermore, equations derived from the sure independence screening and sparsifying operator (SISSO) provided clear and interpretable structure-energy relationships. The results indicate that adsorption strength is jointly determined by molecular charge transfer and geometric relaxation under the constraint of the surface work function (Wf). Through analyses of recovery time and sensitivity, we clarified the response behaviors of rare-earth dopants toward different target gases. These findings deepen our understanding of Ln–SnO2–gas interactions.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"293 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173192","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Modulation of the Structural and Photophysical Properties of 2D-RP Perovskites with Nitrogenous-Heteroaromatic Molecules","authors":"Soumi Dutta,Biplove Kumar,Priyanka Dubey,Mustafa Maqbool,Neeladri Das,Manas Kumar Sarangi","doi":"10.1039/d6ta06639a","DOIUrl":"https://doi.org/10.1039/d6ta06639a","url":null,"abstract":"Two-dimensional lead halide Ruddlesden-Popper (2D-RP) perovskites have emerged as promising optoelectronic materials owing to their facile solution-based synthesis, ligand-engineered stability enhancement, and excellent photophysical properties. Structure-induced property changes like crystal patterns, defect density, phase purity, and optical properties in layered 2D-RP perovskites are underexplored and are mostly governed by Lewis acid-base ligand chemistry. In this manuscript, two Phenyl-ethyl-amine (PEA) based 2D-RP perovskites are studied, namely (PEA)2PbBr4 (PEPB) and (PEA)2PbI4 (PEPI) and systematically probe their photo-induced structural changes in the presence of Pyridine (PY), N, Nʹ-Dimethylaniline (DMA), and their functionalized derivatives. The nature and position of the functional groups in these nitrogenous-Lewis bases may significantly influence their interactions with the spacer cations, the Pb(II)-octahedra, surface passivation, etc., in the layered structures through supramolecular interactions like inter/intra-molecular hydrogen-bonding, ion-π, and π-π. PY, 2-Aminopyridine, and DMA induced only minor structural changes in PEPB and PEPI, whereas 3-Aminopyridine and N, Nʹ-dimethyl-3-aminopyridine cause moderate structural perturbations, only in PEPI. In contrast, the para-substituted molecules, 4-Aminopyridine and N, Nʹ-Dimethyl-4-aminopyridine, causes significant structural distortions in both 2D-RP perovskites. These observations open-up new insight in tailoring the structural and photophysical properties of 2D-RP perovskites with nitrogenous-heteroaromatic molecules as effective surface passivator or linkers for optoelectronic-device applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"191 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dan Kaplun,Boris Biniaminov,Joanna Dehnel,Michelle Sykes Akerman,Ido Zemer,Igal Levine
{"title":"Identifying deep hole traps as the origin of reduced carrier separation in Sb-alloyed CsAgBiBr double perovskites","authors":"Dan Kaplun,Boris Biniaminov,Joanna Dehnel,Michelle Sykes Akerman,Ido Zemer,Igal Levine","doi":"10.1039/d6ta04613d","DOIUrl":"https://doi.org/10.1039/d6ta04613d","url":null,"abstract":"Lead-free double perovskites, such as Cs2AgBiBr6, are promising low-toxicity alternatives for photovoltaic (PV) applications, and bandgap engineering through antimony (Sb) alloying has been extensively investigated to optimize their performance. This study uses advanced modulated and time-resolved surface photovoltage (SPV) spectroscopy to investigate how the degree of Sb incorporation in Cs2Ag(SbxBi1−x)Br6 (x = 0–1) films affects their optoelectronic properties and the distribution of defects within the films. Structural characterization confirms phase purity across the composition range and modulated SPV reveals that the indirect bandgap remains nearly constant at ∼2.25 eV for most mixed compositions, directly contradicting previous reports of bandgap bowing. The results of this study demonstrate that the addition of Sb to Cs2AgBiBr6 films significantly reduces the charge separation efficiency. Using modulated SPV, three deep defect levels situated at 0.67, 1.44, and 1.74 eV from the band edges were identified. Time-resolved SPV analysis indicates that these negatively charged defects act as surface hole traps, leading to the accumulation of trapped holes near the surface. Exciton formation in the Sb-alloyed films results in localized excitons that fail to generate free charge carriers, leading to severe signal quenching. Here, it is demonstrated that alloying double perovskites with Sb introduces deep defect states that act as non-radiative recombination centers, degrading the optoelectronic quality of the alloyed double perovskites.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"10 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173193","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chunrong Li,Mark Robert James Elsegood,Yibing Peng,Hongxu Guo,Yi Liu,Chuntao Zhang,Huaiyu Yang
{"title":"Reversible Thermosalient Effect of Butyl Paraben Cocrystal for Thermal to Mechanical Energy Conversion","authors":"Chunrong Li,Mark Robert James Elsegood,Yibing Peng,Hongxu Guo,Yi Liu,Chuntao Zhang,Huaiyu Yang","doi":"10.1039/d6ta06574k","DOIUrl":"https://doi.org/10.1039/d6ta06574k","url":null,"abstract":"Thermosalient crystals that exhibit reversible mechanical motion during temperature changes and phase transitions have potential for application in smart sensors, actuators, or drug delivery. During the phase transition of thermosalient crystals, energy conversion occurs, while thermomorphism produces physical work through continuous and nearly instantaneous directed forces. Here, we report for the first time a reversible, single crystal to single crystal phase transition from one polymorph to another of a butyl paraben cocrystal formed with isonicotinamide. This crystal exhibited highly anisotropic lattice changes and reversible crystal shape deformation by the rotation of functional groups in one component, and the stretching of hydrogen bonds between the two components. The slip, molecular rotation, and hydrogen bond stretching caused significant modulation between layers before and after the phase transition, accompanied by anisotropic changes in the crystal unit cells. These changes lead to crystal movements of rotating, splitting, and jumping. In addition, we succeeded in preparing a reversible thermomechanical actuator that generated a push force more than 450 times greater than the weight of the crystal, thereby enabling the cocrystal to act as an actuator for the reversible movement of the glass plate. When the temperature became over 373.15 K, the crystal expanded instantaneously to approximately 2.7% of its original length. When the temperature dropped below 353.15 K, the crystal contracted back to its original length. This cyclic process can rapidly display temperature changes by current. The structural changes during thermosalience processes helps to understand thermo-responsive molecular crystals.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"53 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173183","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A TiCT MXene/SmVO composite electrode enabling high-performance asymmetric supercapacitors","authors":"Arjun Singh,Sonia Nain","doi":"10.1039/d6ta06559g","DOIUrl":"https://doi.org/10.1039/d6ta06559g","url":null,"abstract":"A facile hydrothermal strategy was used to synthesize SmVO4/Ti3C2Tx (SMX) heterostructures by uniformly anchoring SmVO4 (SV) nanoparticles on conductive Ti3C2Tx MXene (MX) nanosheets. The successful formation of the heterostructured composites was confirmed through detailed structural, morphological, and surface analyses. Cyclic voltammetry (CV), galvanostatic charge–discharge (GCD), and electrochemical impedance spectroscopy (EIS) measurements in a 1 M H2SO4 electrolyte were used to systematically examine the electrochemical performance of the SMX series. With a specific capacitance of 975.13 F g−1 (CV) and 972.53 F g−1 (GCD) at 0.5 A g−1 and 92.34% capacitance retention after 10 000 cycles, the optimised SMX3 electrode demonstrated the best electrochemical performance. The optimized SMX3 electrode had an energy density of 86.00 Wh kg−1 at a power density of 200 W kg−1 in the three-electrode configuration. Further practical energy-storage performance was investigated using an SMX3//AC asymmetric supercapacitor device, which achieved a maximum energy density of 58.59 Wh kg−1 at a power density of 193.69 W kg−1. The present study shows the feasibility of the designed composite for further development in advanced electrochemical energy storage devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"169 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}