Chemistry of Materials最新文献

{"title":"Single-Crystal SnSe Film for High-Performance Flexible Thermoelectric Generators","authors":"Xinyu Chen,&nbsp;, ,&nbsp;Jinhong Li,&nbsp;, ,&nbsp;Jianrui Wang,&nbsp;, ,&nbsp;Qiyu Meng,&nbsp;, ,&nbsp;Shangyang Li,&nbsp;, ,&nbsp;Tianpeng Ding,&nbsp;, ,&nbsp;Jianmin Yang,&nbsp;, ,&nbsp;Dasha Mao,&nbsp;, ,&nbsp;Mingyuan Hu*,&nbsp;, and ,&nbsp;Jiaqing He*,&nbsp;","doi":"10.1021/acs.chemmater.5c01587","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01587","url":null,"abstract":"<p >SnSe-based thermoelectric (TE) materials have emerged as promising candidates for wearable devices and flexible electronics due to their exceptional thermoelectric performance. While SnSe single crystals exhibit superior TE properties, their practical applications in flexible electronics have been hindered by mechanical brittleness and complex processing challenges. In this study, we systematically investigated the inherent anisotropic elastic modulus of single-crystalline SnSe and developed a facile tape-peeling method to fabricate high-quality SnSe films. These films exhibited remarkable flexibility, mechanical stability, and a high-power factor of 24 μW cm^–1 K^–2 at 300 K. Furthermore, flexible thermoelectric generators based on SnSe films achieved a high normalized power density of 257.4 W m^–2 under a temperature gradient (Δ<i>T</i>) of 60 K. These results not only demonstrate the immense potential of SnSe films for flexible thermoelectric applications but also provide a scalable fabrication approach that offers an alternative pathway for the development of advanced wearable energy-harvesting technologies.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 18","pages":"7316–7325"},"PeriodicalIF":7.0,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145117378","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":"Strain-Modified Chirality in Selenium-Alloyed Tellurium Nanocrystals","authors":"Bar Reuven,&nbsp;Amram Azulay,&nbsp;Davide Levy,&nbsp;Abdullah Idrees,&nbsp;Amit Kohn and Gil Markovich*,&nbsp;","doi":"10.1021/acs.chemmater.5c01950","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01950","url":null,"abstract":"<p >We investigated the effects of selenium alloying on the shape chirality of colloidal trigonal tellurium nanocrystals (NCs) containing up to ∼6 at. % Se. Circular dichroism spectroscopy shows stronger optical activity in alloyed samples, relative to pure Te NCs, indicating enhanced shape chirality. X-ray diffraction analysis revealed a contraction of the <i>c</i>-axis lattice parameter, attributed to smaller Se atoms substituting for Te, resulting in compressive strain. Furthermore, the average microstrain increases with increasing Se content, along with the development of strong axial strain distribution anisotropy, which is consistent with the intrinsic anisotropy of the Te lattice. Analysis of interplanar spacings from scanning transmission electron microscopy images at atomic-column resolution confirms the existence of heterogeneous intraparticle strain distributions. Hence, these results imply that substitutional Se point defects in Te cause anisotropic strain gradients, which enhance the tendency of chiral Te NCs to form more asymmetric shapes. This study demonstrates how strain engineering by alloying can be employed to tune the structural and optical properties of colloidal NCs.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 17","pages":"6943–6952"},"PeriodicalIF":7.0,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.chemmater.5c01950","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009732","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Inhibition of Metal–Support Interactions by Rare-Earth Doping in Palladium/Ceria Zirconia Three-Way Catalysts","authors":"Lucy Costley-Wood*,&nbsp;, ,&nbsp;Nicolás A. Flores-González,&nbsp;, ,&nbsp;Claire Wilson,&nbsp;, ,&nbsp;Paul Thompson,&nbsp;, ,&nbsp;Sarah Day,&nbsp;, ,&nbsp;Veronica Celorrio,&nbsp;, ,&nbsp;Donato Decarolis,&nbsp;, ,&nbsp;Ruby Morris,&nbsp;, ,&nbsp;Manfred E. Schuster,&nbsp;, ,&nbsp;Huw Marchbank,&nbsp;, ,&nbsp;Timothy I. Hyde,&nbsp;, ,&nbsp;Amy Kolpin,&nbsp;, ,&nbsp;Dave Thompsett,&nbsp;, and ,&nbsp;Emma K. Gibson*,&nbsp;","doi":"10.1021/acs.chemmater.5c01417","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01417","url":null,"abstract":"<p >The impact of rare-earth (RE) doping in ceria-zirconia─critical for enhancing thermal stability and optimizing redox properties─on surface palladium (Pd) behavior has been investigated. RE doping was found to weaken metal–support interactions, leading to increased Pd mobility, with notable effects on oxygen storage capacity and light-off performance under model exhaust conditions. The mobility and redox characteristics of Pd were assessed through in situ thermal experiments using X-ray absorption spectroscopy at the Pd K-edge and synchrotron powder diffraction. Complementary Ce K-edge EXAFS and Rietveld refinements confirmed the structure and composition of the doped ceria-zirconia material. Deactivation studies and lifetime prediction are essential for commercial catalysts, particularly for three-way catalysts (TWCs) designed for decade-long operation. To probe long-term stability, in situ thermal treatments were conducted to induce separation of the metastable ceria–zirconia solid solution. These accelerated thermal aging treatments were then compared with a prolonged, seven week aging protocol, and regular in situ synchrotron PXRD measurements provided insights into the phase separation process. The influence of thermal aging on metal–support interactions was further assessed through catalytic performance testing.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 18","pages":"7214–7226"},"PeriodicalIF":7.0,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.chemmater.5c01417","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145117376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Evaluating the Energy Conversion Performance of Rare-Earth-Based Cu3RETe3 Thermoelectric Materials with Strong Electronic Correlations","authors":"Oleksandr Cherniushok,&nbsp;, ,&nbsp;Oleksandr V. Smitiukh,&nbsp;, ,&nbsp;Dariusz Wieczorek,&nbsp;, ,&nbsp;Oleg V. Marchuk,&nbsp;, ,&nbsp;Bartlomiej Wiendlocha,&nbsp;, ,&nbsp;Taras Parashchuk*,&nbsp;, and ,&nbsp;Krzysztof T. Wojciechowski,&nbsp;","doi":"10.1021/acs.chemmater.5c01744","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01744","url":null,"abstract":"<p >A key challenge in thermoelectric materials development is achieving low thermal conductivity without compromising the electrical performance. Rare-earth tellurides, due to their complex crystal chemistry and intrinsic defects, offer a pathway to optimize these conflicting parameters. In this work, we investigated the structural and thermoelectric properties of a series of ternary rare-earth copper tellurides, Cu₃<i>RE</i>Te₃ (<i>RE</i> = Er, Ho, Tb). Our findings reveal that the specific rare-earth element plays a critical role in determining the crystal structure of these compounds. Notably, the Er- and Ho-containing phases predominantly crystallize in the orthorhombic <i>Pmn</i>2₁ structure, whereas the Tb analogue adopts a trigonal <i>R</i>-3 structure. Owing to this structural difference, the Tb-based compound exhibits approximately twice the effective mass─and, correspondingly, a 2-fold increase in the Seebeck coefficient─attributed to band convergence, as confirmed by theoretical calculations. All materials exhibit intrinsically low lattice thermal conductivity, attributed to strong lattice anharmonicity and point defect scattering, particularly pronounced in Cu₃TbTe₃. Hall effect and Seebeck measurements indicate <i>p</i>-type semiconducting behavior with carrier concentrations on the order of 10²⁰ cm^–3. First-principles calculations show the presence of strong electronic correlations, and GGA+U method is necessary to confirm semiconducting electronic structures and support experimental trends in carrier mobility and Seebeck coefficient. Among the compounds, Cu₃HoTe₃ achieves the highest peak thermoelectric figure of merit (<i>ZT</i> ≈ 0.9 at 873 K), while Cu₃TbTe₃ delivers the highest average performance (<i>ZT</i>_ave = 0.4 over the temperature range of 298–873 K). These findings highlight the potential of Cu₃<i>RE</i>Te₃ compounds as efficient rare-earth-based thermoelectric materials for energy conversion applications.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 18","pages":"7377–7389"},"PeriodicalIF":7.0,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.chemmater.5c01744","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145117375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Upcycling of Polyethylene Terephthalate Waste into Closed-Loop Recyclable Carbon Fiber-Reinforced Polymer Composites with High Performance","authors":"Saipeng Feng,&nbsp;Jiawei Xie,&nbsp;Yang Ding,&nbsp;Chang-Cun Yan* and Feng Yan*,&nbsp;","doi":"10.1021/acs.chemmater.5c01214","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01214","url":null,"abstract":"<p >The proper management of polyethylene terephthalate (PET) waste and the development of recyclable carbon fiber-reinforced polymer composites (CFRPCs) are two of the most concerning topics in the field of sustainable polymer chemistry. In this study, we propose an effective strategy that simultaneously addresses these challenges through the upcycling of PET waste into closed-loop recyclable CFRPCs with a high mechanical performance. Specifically, aminolysis products of wasted PET were used as the main building blocks to construct the closed-loop recyclable polymer matrix with judiciously designed dialdehyde moieties and phosphate-based cross-linkers. The matrix exhibited a high tensile stress of about 120 MPa, which is far superior to PET and most close-loop recyclable thermosets reported in the literature. When composited with carbon fibers (CFs), the resulting CFRPCs demonstrated both high tensile strength over 500 MPa and flexural stress over 630 MPa, reaching the practical standard. The matrix can be degraded into its monomers, and CFs can be recycled nondestructively in a solvent-assisted method, which can be reused to fabricate new CFRPCs without significant performance degradation. This research offers a promising paradigm for simultaneously resolving the issues of PET degradation and CFRPC recycling.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 17","pages":"6667–6677"},"PeriodicalIF":7.0,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009801","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":"Injectable Bioactive Polyurethane Adhesive for Critical-Size Cranial Defect Restoration","authors":"Lin Yang,&nbsp;Xiaolei Guo,&nbsp;Yuan Feng,&nbsp;Jingjing Lin,&nbsp;Mingtao Luo,&nbsp;Zhen Li,&nbsp;Jiehua Li,&nbsp;Dan Lu*,&nbsp;Feng Luo* and Hong Tan,&nbsp;","doi":"10.1021/acs.chemmater.5c01618","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01618","url":null,"abstract":"<p >Critical-size bone defects are difficult to autonomously regenerate. Bioactive tissue adhesives are promising materials for bone defect restoration, but the imbalance between the adhesion and cohesion of traditional adhesives leads to structural instability, ultimately resulting in suboptimal long-term repair outcomes. This work developed a dual-component injectable biodegradable polyurethane adhesive (PUA-H) with osteoinductive repair capability. Regardless of concentration, the structural design balances the adhesion and cohesion of PUA-H, with the bone adhesion strength achieved at 668.9 ± 80.6 kPa. Notably, this design mitigates the impact of wet environments and significantly enhances the adhesive durability. Nanohydroxyapatite (nHAP) was incorporated into the adhesive to further enhance the osteogenic activity. Inspired by mussels, catechol groups were grafted onto the chain extender and cross-linker to establish strong metal–ligand coordination, enabling sustained Ca^2 + release over 60 days. In <i>in vitro</i> experiments and in critical-size cranial defect models, the PUA-H group exhibited exceptional osteoinductive activity and repair efficacy. This work provides a strategy for adhesion regulation in tissue adhesives, particularly suitable for the precision repair of large irregular bone defects.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 17","pages":"6823–6836"},"PeriodicalIF":7.0,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009780","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":"Out-of-Plane Rashba Spin-Splitting and Structure-Property Relationships in Layered Cu2AMVSe4 Chalcogenides (A = K, Rb, Cs; MV = V, Nb, Ta)","authors":"Timothy M. McWhorter,&nbsp;Wentao Zhang,&nbsp;Yang Shen,&nbsp;Volker Blum* and David B. Mitzi*,&nbsp;","doi":"10.1021/acs.chemmater.5c01116","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01116","url":null,"abstract":"<p >Recent research targeting functional multinary chalcogenide semiconductors (MCSs) has successfully demonstrated the tailoring of structure-property-application relationships within the I₂-II-IV-X₄ material family (Roman numerals I, II, and IV refer to the oxidation states of the constituent elements; X refers to a chalcogen). To apply and expand upon the experience gained from these systems, we utilize a combined computational and experimental approach to investigate nine members of a compositionally analogous I₂-I′-V-X₄ family, incorporating a coupled substitution of an alkali (I′ = K, Rb, Cs) and a pentavalent transition metal (V = V, Nb, Ta) for the II and IV sites, respectively, while I = Cu and X = Se. Four previously unreported compounds in this set adopt a layered noncentrosymmetric (<i>Ama</i>2 space group) structure, analogous to that of existing family members. One compound, Cu₂CsVSe₄, instead forms a related <i>Pna</i>2₁ lattice. All nine compounds show strong absorption with direct bandgaps ranging from 1.2–2.5 eV, appropriate for potential applications involving optoelectronics and (due to inversion asymmetry) spin-optoelectronics. The density functional theory (DFT) study concludes that the heavy-element (e.g., Ta) containing members exhibit significant out-of-plane Rashba spin splitting of up to 96 meV at the conduction band minimum, suggesting promise for further examination of spin behavior and control. Spin splitting parameters progressively increase across the series V→Nb→Ta, consistent with increased spin–orbit coupling. Optoelectronic properties (e.g., the bandgap) in this series depend primarily upon the identity of the 5+ transition metal ion, while the size of the alkali spacer ions primarily impacts spin-splitting behavior. Finally, thermal analysis studies highlight stability for the considered compounds up to ∼650 °C.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 17","pages":"6603–6618"},"PeriodicalIF":7.0,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009630","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":"Thermally Evaporated Naphthalene Diimides as Electron Transport Layers for Perovskite Solar Cells","authors":"Jack Lawton,&nbsp;Justine S. Wagner,&nbsp;Xiangyu Xiao,&nbsp;Sanggyun Kim,&nbsp;Anna M. Österholm,&nbsp;D. Eric Shen,&nbsp;Sina Sabury,&nbsp;Carlo A. R. Perini,&nbsp;Kunal Datta,&nbsp;Diana K. LaFollette,&nbsp;Ruipeng Li,&nbsp;John R. Reynolds and Juan-Pablo Correa-Baena*,&nbsp;","doi":"10.1021/acs.chemmater.5c01186","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01186","url":null,"abstract":"<p >Thermally evaporated organic electron transport layers (ETLs) have the potential to enable high-performance and scalable perovskite solar cells (PSCs). Among these, naphthalene diimide (NDI)-based ETLs are a promising family of materials that exhibit the optoelectronic properties, ambient stability and versatility required of high-performance ETLs. Here, we synthesized five NDI derivatives with varying functional groups and identified the two most promising candidates for evaluating the impact of molecular structure on processability via thermal evaporation. While phosphonic acid functionalization was shown to introduce thermal instability, leading to chemical changes during evaporation, NDI-bis <i>N</i>-phenyl-bromide (NDI-(PhBr)₂) emerged as a promising ETL candidate. NDI-(PhBr)₂ demonstrated excellent compatibility with the thermal evaporation process and enabled PSCs with power conversion efficiencies (PCEs) of 15.6%, surpassing all previously reported PSCs containing thermally evaporated NDI ETLs. Furthermore, NDI-(PhBr)₂ exhibited excellent operational stability, retaining 75% of the initial PCE after 150 h of operation under continuous illumination at 65 °C. These results highlight the potential of NDI-based ETLs for advancing the scalability and performance of PSCs.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 17","pages":"6655–6666"},"PeriodicalIF":7.0,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.chemmater.5c01186","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009843","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Copper-Rich PdxCu1–x Alloy Nanoparticles as Catalyst for Electrochemical Reduction of CO2","authors":"Andreas Dueholm Bertelsen,&nbsp;Rebekka Klemmt,&nbsp;Kirstine Nygaard Kolding,&nbsp;Espen Drath Bøjesen and Bo Brummerstedt Iversen*,&nbsp;","doi":"10.1021/acs.chemmater.5c01148","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01148","url":null,"abstract":"<p >Copper is uniquely able to catalyze the formation of hydrocarbon-derived molecules through the electrochemical carbon dioxide reduction reaction (CO₂RR) in aqueous media. Here, we investigate the change of selectivity and/or activity in CO₂RR by alloying Cu with palladium by using Pd_<i>x</i>Cu_1–<i>x</i> nanoparticles as electrocatalysts. <i>In situ</i> powder X-ray diffraction reveals a much lowered reduction temperature of the Cu-precursor upon alloying and establishes the importance of high heating rates during synthesis to ensure homogeneous Pd alloying into copper-rich Pd_<i>x</i>Cu_1–<i>x</i> nanoparticles. Two different synthetic approaches were used to obtain Pd_<i>x</i>Cu_1–<i>x</i> nanoparticles with a composition range of <i>x</i> = 0.025–0.20, and the complex nanostructures of the particles were highlighted using four-dimensional Scanning Transmission Electron Microscopy (4D-STEM). The activity and selectivity toward electrochemical CO₂RR in 0.1 M KHCO₃ were assessed for increasing Pd contents, and a systematic decrease in faradaic efficiency toward hydrocarbon products was found coupled with an increase in faradaic efficiency toward primarily H₂. The results do not support Pd_<i>x</i>Cu_1–<i>x</i> alloying as a viable method for increasing selectivity toward specific hydrocarbon products in electrochemical CO₂RR.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 17","pages":"6619–6628"},"PeriodicalIF":7.0,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009842","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":"Understanding the Prospects of the Thermoelectric Performance of the YbMg2(Bi,Sb)2 Zintl Phase","authors":"Kushal Mehrotra,&nbsp;Andrei Novitskii* and Takao Mori*,&nbsp;","doi":"10.1021/acs.chemmater.5c01433","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c01433","url":null,"abstract":"<p ><i>AM</i>₂<i>X</i>₂ Zintl compounds, crystallizing in layered structures, have recently garnered attention due to their promising thermoelectric properties. In this study, we explore the chemical bonding and elastic and thermoelectric properties evolution across the full YbMg₂Bi_2–<i>x</i>Sb_<i>x</i> solid solution. The transition from YbMg₂Bi₂ to YbMg₂Sb₂ leads to a continuous linear chemical-bond shortening and thus a significant enhancement in elastic moduli and sound velocity, resulting in overall significant lattice stiffening. Simultaneously, the shift toward more ionic chemical bonding leads to significant changes in the band structure, particularly an increase in effective mass and a decrease in both carrier concentration and mobility, which in turn reduces the power factor for Sb-rich samples. However, a rapid increase in point-defect scattering causes the lattice thermal conductivity to drop from ≈3 to almost 1 Wm^–1–K^–1 at 300 K for the intermediate compositions, thus opening new room for further optimization of the Sb-rich representatives of the YbMg₂Bi_2–<i>x</i>Sb_<i>x</i>. Therefore, in this work, we have demonstrated that despite the seemingly intrinsically higher thermoelectric performance in the Bi-rich region of the YbMg₂Bi_2–<i>x</i>Sb_<i>x</i> solid solution, the Sb-rich representatives may in fact be even more promising due to better mechanical and thermal stability and greater room for further charge carrier concentration optimization.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 17","pages":"6782–6790"},"PeriodicalIF":7.0,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.chemmater.5c01433","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009688","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}