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Triple Synergistic Modulation via Sn Doping in Tetrahedrites: Electronic Structure, DOS, and Scattering engineering for a High Thermoelectric Performance

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ACS Applied Materials and Interfaces 2025年第19期17卷 28384-28394页

作者： Huang, Lulu Wan, Shanhong Wu, Junyang Wang, Binbin Yu, Hongsong Liu, Yu Zhang, Jinhua Wu, Yucheng Zhang, Xuemei Yan, Jian Zhang, Jian School of Materials Science and Engineering Hefei University of Technology Hefei230009 China Engineering Research Center of High Performance Copper Alloy Materials and Processing Ministry of Education Hefei University of Technology Hefei230009 China Anhui Province Engineering Research Center of Flexible and Intelligent Materials School of Chemistry and Chemical Engineering Hefei University of Technology Hefei230009 China Infrared and Low Temperature Plasma Key Laboratory of Anhui Province College of Electronic Engineering National University of Defense Technology Hefei230037 China School of Physics and Electronic Information Engineering Ningxia Normal University Guyuan756000 China Key Laboratory of Materials Physics Institute of Solid State Physics Chinese Academy of Sciences Hefei230031 China

Achieving a high power factor and low lattice thermal conductivity is crucial for improving the thermoelectric performance. The eco-friendly Cu12Sb4S13 tetrahedrite inherently exhibits a high power factor (∼10-14 μW cm-1 K-2) and low thermal conductivity (0.5-1.00 W m-1 K-1), but these properties also impose significant limitations for further performance enhancement. To overcome these challenges, researchers have explored strategies such as codoping/synergistic element doping and nanocomposites. In this work, we demonstrate that Sn doping at the Sb site in Cu12Sb4S13 (without the use of nanocomposites) enables the synergistic modulation of both the electronic and thermal properties. The Sn doping increases the hole concentration and enhances the density of states (DOS), leading to a marked improvement in the power factor (at 750 K), 12 μW cm-1 K-2 for x = 0 to 16 μW cm-1 K-2 for x = 0.04. Simultaneously, Sn doping induces strong phonon scattering, which lowers thermal conductivity by ∼69% (at 750 K). This synergistic modulation of the electronic structure, DOS, and scattering mechanisms results in a significant enhancement in the thermoelectric performance. The optimized Cu12Sb3.96Sn0.04S13 sample exhibits an exceptional figure of merit (ZT) of 1.26 at 750 K, representing a 126% increase compared to pristine Cu12Sb4S13. These findings demonstrate the effectiveness of Sn doping in simultaneously optimizing the electrical and thermal properties of Cu12Sb4S13 through the synergistic modulation of the electronic structure, density of states, and phonon scattering mechanisms. © 2025 American chemical Society.

关键词： Phonon scattering

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Enhancing compatibility of waste tire rubber powder in asphalt: A comparative study of acid surface activation and molecular dynamics insights

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Construction and Building Materials 2025年 478卷

作者： Jin, Xin Ren, Denghui Wu, Haisheng Kong, Hao Yang, Qingzhao Zhou, Tao Zhao, Zhenxia Li, Jing School of Chemistry and Chemical Engineering Guangxi University Nanning530004 China Key Laboratory of New Low-carbon Green Chemical Technology Education Department of Guangxi Zhuang Autonomous Region Nanning530004 China

Waste tire management remains an environmental challenge due to low recycling rates and the inert nature of rubber powder (RP) in asphalt applications. This study systematically investigates the surface activation of RP using five acids—gallic acid, oleic acid, palmitic acid, stearic acid, and tannic acid—and evaluates their effects on asphalt modification. Among these, gallic acid-activated rubber powder (GA-RP) exhibited the most significant enhancements in rheological properties and anti-aging performance. Compared to unmodified asphalt, GA-RP-modified asphalt demonstrated a 126.76 % increase in complex modulus, a 173.12 % increase in storage modulus, and a 107.18 % increase in loss modulus at 46°C, reflecting improved elasticity and high-temperature stability. The MSCR test revealed an 82.98 % reduction in strain under 0.1 kPa stress, indicating superior resistance to permanent deformation, while the LAS test demonstrated a 7.52-fold increase in fatigue life at 2.5 % strain, confirming enhanced durability. Molecular dynamics simulations provided further insights into the improved compatibility of GA-RP with the asphalt matrix. The solubility parameter difference between GA-RP and asphalt was reduced to 1.69, the smallest among all modified asphalts, suggesting superior molecular affinity. Mean square displacement analysis showed that the diffusion coefficient difference between GA-RP and asphalt was only 0.00038 Å²/s, significantly lower than that of unmodified RP (0.00086 Å²/s), confirming enhanced stability and reduced phase separation. Additionally, GA-RP-modified asphalt exhibited the lowest softening point difference (2.1°C) in storage stability tests, further validating the effectiveness of gallic acid modification. These findings establish an optimized strategy for sustainable waste tire utilization, offering an effective and environmentally friendly solution for high-performance asphalt modification. © 2025 Elsevier Ltd

关键词： Waste management

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The construction of flocculation-to-extraction coupled system with a novel dual-functional polymer for dye wastewater treatment and reuse

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Environmental Research 2025年 278卷 121725页

作者： Bai, Guochen Liu, Guo Ran, Tingmin Shi, Yulin State Key Laboratory Incubation Base for Green Processing of Chemical Engineering School of Chemistry and Chemical Engineering Shihezi University Shihezi832000 China State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources School of Chemical Engineering and Technology Xinjiang University Urumqi830017 China

The construction of novel materials with multiple functions for water treatment has received wide attention in the field of environmental science. Herein, a dual-functional polymer (DFP) was prepared through the etherification reaction of starch with isopropyl glycidyl ether and 2-chloro-4-dimethylamine-6-diethylamine-[1,3,5]-triazine. DFP exhibited controlled thermo-irreversible on/off properties, and the changes in water solubility could be observed in response to slight stimuli from the external environment. This made DFP a promising candidate for the treatment of dye wastewater through flocculation or extraction. The results showed that the maximum dye uptake capacity and the decoloration efficiency reached 976 mg/g and 97.2 %, respectively, under the optimal flocculation conditions. Moreover, the extraction rate was 94.5 % under the optimal extraction conditions. Excitingly, the heat-triggered flocculation-to-extraction behavior of DFP could be realized with a coupled system, which then minimized the drawbacks of a single unit. In this coupled system, the extraction mechanism changed from chemical extraction to physical extraction, which avoided unnecessary loss of decolorization rate. Furthermore, the recycling and reuse of waste resources could be achieved through stripping and the next round of direct dye baths. Therefore, this work provided a new methodology for the development of novel pollutant removal systems with dual-functional materials, achieving the reuse of waste resources and improving the quality of treated water. © 2025 Elsevier Inc.

关键词： Water recycling

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Modulating Cu-O-Zr interfaces on high-roughness MgO surface for reinforced hydrogen production from sorption-enhanced steam reforming of methanol

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Nano Energy 2025年 141卷

作者： Sun, Zhao Wang, Huicai Wang, Xingxu Zhang, Riguang Sun, Zhiqiang Hunan Engineering Research Center of Clean and Low-Carbon Energy Technology School of Energy Science and Engineering Central South University Changsha410083 China State Key Laboratory of Clean and Efficient Coal Utilization College of Chemical Engineering and Technology Taiyuan University of Technology Taiyuan030024 China

Sorption-enhanced steam reforming of methanol (SE-SRM) offers a promising route for high-quality hydrogen production with in situ CO2 capture;however, achieving an optimal balance between catalytic activity and CO2 uptake capability, while ensuring catalyst stability, remains a significant challenge. In this study, a series of Zr-doped (0 wt%, 5 wt%, 15 wt%, 25 wt%) Cu-MgO catalytic sorbents are synthesized for SE-SRM. At 180℃, the hydrogen concentration and yield reach nearly 100 % and 10.35 μmol·g−1·s−1. Moreover, the catalytic sorbent basically retains its catalytic activity and CO2 uptake capacity after 30 cycles with merely slight deactivation. Results demonstrate that the doped Zr, presents as tetragonal ZrO2, enhances metal-support interactions with the formation of a Cu-O-Zr interfacial structure, promoting Cu nanocluster dispersion and altering the Cu+/Cu0 distributions. Zr doping also enables the modulation of the medium-strong basic sites. Moreover, the AFM and TEM confirmed the formation of high-roughness MgO surface on the substrate, thereby facilitating CO2 diffusion and adsorption. DFT calculation results further confirm the advantages of Zr-doped Cu-MgO catalytic sorbents due to its stronger capability on CH3OH activation and CO2 adsorption. © 2025 Elsevier Ltd

关键词： Water absorption

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Ti deficiency and its effect on synthesizing all-d-metal Heusler alloy powders via mechanical alloying

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Materials Characterization 2025年 224卷

作者： Zhang, Hongguo Shi, Jinhao Zhang, Zhentao Wang, Xiangming Yue, Ming College of Materials Science and Engineering State Key Laboratory of Materials Low-Carbon Recycling Key Laboratory of Advanced Functional Materials Ministry of Education Beijing University of Technology Beijing100124 China Hefei230031 China

This study proposes and realizes the synthesis of powder and bulk Ni-Co-Mn-Ti-based all-d-metal Heusler alloys through mechanical alloying and powder metallurgy. Ti deficiency was found and recognized as a critical factor for the phase formation in similar compounds. By adjusting the Ti content, alloying and heat treatment process, L10, B2, and 5 M martensitic phases can be obtained. Martensitic phase transformation temperatures can also be adjusted through various factors involved in the process. The absence of a metamagnetic transition up to 3 T was observed in the bulk samples, which is related to the small magnetization difference during the phase transformation. A maximum magnetic entropy change comparable to alloys produced via rapid quenching was achieved. The present method is an effective and flexible route to fabricating powders of all-d-metal alloys with tailored structural and magnetic properties. It can serve as a pre-process for advanced manufacturing and provide new phase control choices in related systems. © 2025 Elsevier Inc.

关键词： Titanium alloys

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Research on the induced crystallization behavior of high-performance thermoplastics resin-based composites

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Fuhe Cailiao Xuebao/Acta Materiae Compositae Sinica 2025年第5期42卷 2331-2348页

作者： Yu, Kun Yao, Jianan Zhang, Daijun Liu, Gang Liu, Hao Chen, Chunhai Center for Advanced Low-dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Shanghai201620 China AECC Beijing Institute of Aeronautical Materials Beijing100095 China National Key Laboratory of Advanced Composites Beijing100095 China Institute of Advanced Technology and Equipment Beijing University of Chemical Technology Beijing100029 China

In thermoplastic resin-based composites, optimizing interfacial properties is crucial for enhancing the overall characteristics of the composites. When carbon fibers (CF) are employed as the reinforcement, combined with semi-crystalline high-performance thermoplastic resins such as polyetheretherketone (PEEK), polyaryletherketone (PAEK), or polyphenylene sulfide (PPS) as the matrix, the induced crystallization phenomenon at the fiber/resin interface significantly impacts the interfacial properties of the composite. Taking the issue of induced crystallization in the study of high-performance thermoplastic resin-based composites as the starting point, this article comprehensively reviews the research progress in this area. The article covers the entire process from the preparation methods of induced crystallization samples to their final performance changes, analyzes the classification and influencing factors of induced crystallization, and describes several typical transcrystallinity (TC) morphologies in high-performance thermoplastic resins. Additionally, this article focuses on discussing the specific impact of TC on the interfacial properties of high-performance thermoplastic resin-based composites, and proposes the existing problems and challenges in this field. © 2025 Beijing University of Aeronautics and Astronautics (BUAA). All rights reserved.

关键词： carbon fibers

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An experimental and computational investigation on structural evolution of the In₂O₃ catalyst during the induction period of CO₂ hydrogenation

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Chinese Journal of Catalysis 2025年 72卷 301-313页

作者： Wei, Zhangqian Wang, Mingxiu Lu, Xinnan Zhou, Zixuan Tang, Ziqi Chang, Chunran Yang, Yong Li, Shenggang Gao, Peng Center for Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 China University of the Chinese Academy of Sciences Beijing 100049 China School of Physical Science and Technology Shanghai Tech University Shanghai 201210 China State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 China Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering and Technology Xi'an Jiaotong University Shaanxi Xi'an 710049 China

As one of the most important industrially viable methods for carbon dioxide (CO2) utilization, methanol synthesis serves as a platform for production of green fuels and commodity chemicals. For sustainable methanol sy... 详细信息

As one of the most important industrially viable methods for carbon dioxide (CO₂) utilization, methanol synthesis serves as a platform for production of green fuels and commodity chemicals. For sustainable methanol synthesis, In₂O₃ is an ideal catalyst and has garnered significant attention. Herein, cubic In₂O₃ nanoparticles were prepared via the precipitation method and evaluated for CO₂ hydrogenation to produce methanol. During the initial 10 h of reaction, CO₂ conversion gradually increased, accompanied by a slow decrease of methanol selectivity, and the reaction reached equilibrium after 10-20 h on stream. This activation and induction stage may be attributed to the sintering of In₂O₃ nanoparticles and the creation of more oxygen vacancies on In₂O₃ surfaces. Further experimental studies demonstrate that hydrogen induction created additional oxygen vacancies during the catalyst activation stage, enhancing the performance of In₂O₃ catalyst for CO₂ hydrogenation. Density functional theory calculations and microkinetic simulations further demonstrated that surfaces with higher oxygen vacancy coverages or hydroxylated surfaces formed during this induction period can enhance the reaction rate and increase the CO₂ conversion. However, they predominantly promote the formation of CO instead of methanol, leading to reduced methanol selectivity. These predictions align well with the above-mentioned experimental observations. Our work thus provides an in-depth analysis of the induction stage of the CO₂ hydrogenation process on In₂O₃ nano-catalyst, and offers valuable insights for significantly improving the CO₂ reactivity of In₂O₃-based catalysts while maintaining long-term stability. © 2025 Dalian Institute of chemical Physics, the Chinese Academ

关键词： In2O3CO2 hydrogenation Induction and activation Methanol production Structural evolution

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Magnetic tuning of optical anisotropy in 2D materials: Insights from antiferromagnetic-TMDC interfaces

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Nano Research 2025年第2期18卷 869-877页

作者： Miaoxia Gao Xing Xie Junying Chen Junnan Ding Fangping Ouyang Zongwen Liu Jian-Tao Wang Jun He Yanping Liu Institute of Quantum Physics School of PhysicsCentral South UniversityChangsha 410083China State Key Laboratory of Precision Manufacturing for Extreme Service Performance Central South UniversityChangsha 410083China School of Physics and Technology State Key Laboratory of Chemistry and Utilization of Carbon Based Energy ResourcesXinjiang UniversityUrumqi 830046China School of Chemical and Biomolecular Engineering The University of SydneyNSW 2006Australia The University of Sydney Nano Institute The University of SydneyNSW 2006Australia Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China Songshan Lake Materials Laboratory Dongguan 523808China

Atomically thin two-dimensional(2D)magnetic materials offer unique opportunities to enhance interactions between electron spin,charge,and lattice,leading to novel physical properties at low-dimensional *** extensive research has explored how breaking three-fold(Cs)rotational symmetry in transition metal dichalcogenides(TMDC)can induce optical anisotropy at heterointerfaces,the role of magnetism in modulating these anisotropic optical properties ***,engineerwe antiferromagnet/semiconductor heterostructure by coupling isotropic MoWSe_(2) with the low-symmetric antiferromagnet NiPSs,introducing in-plane anisotropy in the MoWSe_(2) ***-temperature photoluminescence(PL)measurements reveal a pronounced linear polarization-dependent exciton emission intensity at the MoWSe_(2)/NiPS interface,with anisotropy ratios of 1.09 and 1.07 for charged and neutral excitons,***,applying an out-of-plane magnetic field results in a dramatic rotation of the exciton polarization direction by up to 90°at 9 T,significantly exceeding the previously reported maximum deflection of around 27°.This pronounced polarization rotation is not solely attributed to valley coherence,indicating a strong influence of the magnetic order in *** findings provide new insights into the role of magnetic ordering in tuning optical anisotropy in 2D materials,paving the way for the development of advanced polarization-sensitive optoelectronic and magneto-optic devices.

关键词： transition metal dichalcogenides(TMDC) optical anisotropy symmetry engineering antiferromagnetic NiPS_(3)

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Applications of CeO_(2)-based heterojunctions in photocatalytic bactericidal and antitumor therapy

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Journal of Rare Earths 2025年第3期43卷 441-452,I0002页

作者： Chengzhang Zhu Qihang Tian Binghan Wang Jiahui Liu Jiaao Han Shukun Le Peipei Liu Yang Wu Haitao Xu School of Environmental Science and Engineering Nanjing Tech UniversityNanjing210009China Inner Mongolia Key Laboratory of High-Value Functional Utilization of Low Rank Carbon Resources Chemical Engineering CollegeInner Mongolia University of TechnologyHohhot010050China National Institute of Scientific Research-Energy Materialsand TelecommunicationsJ3X 1P7QCCanada National Observation and Research Station of Coastal Ecological Environments in Macao Macao Environmental Research InstituteMacao University of Science and TechnologyMacao SAR999078China Nanjing Gekof Institute of Environmental Protection Technology&Equipment Co. Ltd.Nanjing211100China

The rapid development of rare earth metal elements in the field of photocatalysis is due to their excellent optical and physicochemical *** from the unique external electronic structure of 4f_15d_16S_2,superior electronegativity of the 4f orbitals,and strong oxygen storage-release ability in Ce^(4+)/Ce^(3+)reversible pairs,cerium dioxide(CeO_(2))has attracted increasing interest from ***,the fast recombination of photoinduced electron-hole pairs and wide energy band gap of bare CeO_(2)significantly limit its practical *** overcome the above drawbacks,the construction of heterojunctions has been developed to broaden the absorption spectrum and accelerate the charge *** review presents a mini-review of the synthesis of CeO_(2)-based heterojunctions including typeⅡ,Z-scheme,and S-scheme photocatalysts,as well as the corresponding applications in photocatalytic bactericidal and antitumor ***,the latest advancements and potential perspectives on their future development are also discussed.

关键词： Rare earths Heterojunction Photocatalysis Bacteriostasis Antitumor therapy

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A dual-excitation-driven full-component-responsive lanthanide-basedmetal-organic framework for switchable profiling of multi-diseasemarkers

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Science China Materials 2025年第2期68卷 666-676页

作者： Guoli Chen Bin Dai Ji-Na Hao Yongsheng Li Lab of Low-Dimensional Materials Chemistry Key Laboratory for Ultrafine Materials of Ministry of EducationFrontier Science Center of the Materials Biology and Dynamic ChemistryShanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China School of Chemistry and Chemical Engineering State Key Laboratory Incubation Base for Green Processing of Chemical EngineeringShihezi UniversityShihezi 832003China

Accurate detection of multiple small end-metabolic biomarkers is more sensitive than large biomoleculesto provide real-time feedbacks of physiological/pathologicalstate, but is more challenging due to lack of specific identifyinggroups. Current optical platforms suffer from unsatisfactoryresolutions to differentiate each target because they producesimilar output to different targets using a single excitation,and inevitably involve non-functional components that increase chances of interacting with non-target ***, by taking full advantage of each building unit’sfunctionality to integrate multivariate recognition elements inone interface, a dual-excitation-driven full-component-responsive metal-organic framework (MOF)-based luminescentprobe, namely CeTMA-TMA-Eu, is successfully custom-tailored for detecting both pseudouridine (Ψ) and N-acetylaspartate (NAA), the diagnostic hallmarks of cancer andneurodegenerative disorder. Remarkably, Ψ interacts withMOF’s organic building unit (trimesic acid, TMA) and filtersout its absorptions of 262 nm-light to reduce its energytransferred to Eu^(3+), while NAA induces the valence transitionof Ce^(4+)/Ce^(3+) nodes to improve the cooperative energy transferefficacy from TMA and Ce^(3+) to Eu^(3+). As a result, this platformexhibits completely reverse photoresponses towards Ψ(“switch-off” at 262 nm excitation) and NAA (“switch-on”upon 296 nm excitation), and demonstrates excellent selectivity and sensitivity in complex biofluids, with low detection limits of 0.16 and 0.15 μM, and wide linear ranges of0–180 and 0–100 μM, respectively. Such full-componentresponsive probe with dual-excitation-mediated reverse responses for multi-small targets intrinsically minimizes its interaction with non-target molecules and amplifies resolutionto discriminate each target, providing a new strategy for improving assay accuracy of multi-small biomarkers in diagnostics.

关键词： luminescent probes lanthanide-based metal-organic frameworks dual-excitation regulation multi-disease markers detection

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