ACS Materials Letters最新文献

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Improved Mechanical Adhesion Enabled by Bilayer Hole Transport Layers in Perovskite Solar Cells 钙钛矿太阳能电池中双层空穴传输层提高机械粘附性能
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-07-20 DOI: 10.1021/acsmaterialslett.6c00479
Muzhi Li, Chenchao Xie, Rohit Prasanna, Joseph M. Luther, Nicholas Rolston
{"title":"Improved Mechanical Adhesion Enabled by Bilayer Hole Transport Layers in Perovskite Solar Cells","authors":"Muzhi Li,&nbsp;Chenchao Xie,&nbsp;Rohit Prasanna,&nbsp;Joseph M. Luther,&nbsp;Nicholas Rolston","doi":"10.1021/acsmaterialslett.6c00479","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00479","url":null,"abstract":"<p>We investigate buried-interface mechanical integrity in metal-halide perovskite half-cells using carbazole-based self-assembled monolayers (SAMs) and bilayer hole transport layers composed of metal oxide underlayers and SAMs. Combining macroscopic and microscopic characterization, we quantify interfacial fracture energy (<em>G</em><sub>c</sub>​) and identify delamination pathways. SAM deposition on NiO<sub><em>x</em></sub> increases <em>G</em><sub>c</sub> by approximately 10-fold compared with ITO, highlighting the importance of oxide underlayer selection. To isolate the effect of removing noncovalently bonded SAM molecules, we use vapor-deposited perovskite as a solvent-free model system, decoupling the rinse step inherent to solution processing. Removing loosely bound SAM molecules increases <em>G</em><sub>c</sub> from 0.94 ± 0.08 J·m<sup>–2</sup> to 4.82 ± 0.79 J·m<sup>–2</sup>. These results show that oxide selection and SAM binding quality are both critical for strengthening buried interfaces and designing mechanically robust perovskite solar cells.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2317–2322"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148688122","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
Stepwise Ligand Tuning of Copper Clusters for CO2 Electroreduction Pathway Control 铜簇配体逐步调谐用于CO2电还原途径控制
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-06-24 DOI: 10.1021/acsmaterialslett.6c00341
Renqian Zhou, Naveen M. Halappa, Mengtian Jin, Yafeng Xu, Ruofan Sun, Yu-Ying Yang, Lijie Wang, Peng Yuan, Bahaaeddin Irziqat, Wentao Wu, Tengyue He, Mohammed Faihan Alotaibi, Mohammad Bodiuzzaman, Yanrong Xue, Liang Yi, Zhaohua Wang, Mutalifu Abulikemu, Shadi Fatayer, Omar F. Mohammed, Xu Lu, Osman M. Bakr
{"title":"Stepwise Ligand Tuning of Copper Clusters for CO2 Electroreduction Pathway Control","authors":"Renqian Zhou,&nbsp;Naveen M. Halappa,&nbsp;Mengtian Jin,&nbsp;Yafeng Xu,&nbsp;Ruofan Sun,&nbsp;Yu-Ying Yang,&nbsp;Lijie Wang,&nbsp;Peng Yuan,&nbsp;Bahaaeddin Irziqat,&nbsp;Wentao Wu,&nbsp;Tengyue He,&nbsp;Mohammed Faihan Alotaibi,&nbsp;Mohammad Bodiuzzaman,&nbsp;Yanrong Xue,&nbsp;Liang Yi,&nbsp;Zhaohua Wang,&nbsp;Mutalifu Abulikemu,&nbsp;Shadi Fatayer,&nbsp;Omar F. Mohammed,&nbsp;Xu Lu,&nbsp;Osman M. Bakr","doi":"10.1021/acsmaterialslett.6c00341","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00341","url":null,"abstract":"<p>Copper-based materials with tailored surface modifications hold great potential for electrocatalytic CO<sub>2</sub> reduction reactions (CO<sub>2</sub>RR), particularly in the selective formation of multicarbon (C<sub>2+</sub>) products. However, progress remains limited by an incomplete understanding of the atomic-level coordination environment and associated physicochemical properties. Here, we investigate ligand effects on CO<sub>2</sub>RR performance by a series of atomically precise Cu clusters–Cu<sub>6</sub>(X)<sub>6</sub>, where X represents the thiourea derivative. Notably, Cu<sub>6</sub>(N,N′-diphenylthiourea)<sub>6</sub> achieves maximum Faradaic efficiency of 80.6% toward C<sub>2</sub> products at 150 mA cm<sup>−2</sup>, demonstrating an optimized balance of multiple proton-coupled electron transfer pathways. In contrast, the incorporation of an electron-donating ligand (−NMe<sub>2</sub>) shifts approximately 30% of C<sub>2</sub> products to CH<sub>4</sub>, while an electron-withdrawing ligand (−CF<sub>3</sub>) increases the proportion of C<sub>1</sub> products driven by modified hydrophilicity and electron-donating capability. These findings provide critical insights into atomic-level surface engineering and offer valuable guidance for the rational design of CO<sub>2</sub>RR catalysts.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2210–2219"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148682609","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
Modulating Thermal Field and Electric Field for Enhanced Photocatalysis: From Mechanism to Structure Design 调制增强光催化的热场和电场:从机理到结构设计
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-06-24 DOI: 10.1021/acsmaterialslett.6c00432
Yukai Chen, Yaochen Jin, Qinglian Tan, Yiyi Ji, Dan Wang, Rulin Dong, Jiaojiao Fang
{"title":"Modulating Thermal Field and Electric Field for Enhanced Photocatalysis: From Mechanism to Structure Design","authors":"Yukai Chen,&nbsp;Yaochen Jin,&nbsp;Qinglian Tan,&nbsp;Yiyi Ji,&nbsp;Dan Wang,&nbsp;Rulin Dong,&nbsp;Jiaojiao Fang","doi":"10.1021/acsmaterialslett.6c00432","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00432","url":null,"abstract":"<p>Photocatalysis is pivotal for addressing global energy and environmental challenges. However, its efficiency is constrained by narrow light absorption, rapid photogenerated carrier recombination, and sluggish kinetics. Regulation of thermal and electric fields (by photothermal/piezoelectric/pyroelectric effects) serves as a versatile strategy to overcome these bottlenecks, with merits of facile operation, high efficiency, and no secondary pollution. Different from previous studies emphasizing the photothermal conversion or the piezoelectric effect, this work focuses on the synergistic modulation of thermal and electric fields, along with the pyroelectric effect. In detail, this review summarizes advances in thermal modulation, piezoelectric regulation, and thermo-piezoelectric synergy, clarifying their core mechanisms. Structural design strategies of regulatory systems and applications in key photocatalytic reactions are discussed. Furthermore, current challenges and plausible future directions are prospected, providing theoretical support and technical guidance for designing efficient photocatalytic systems and promoting their industrialization.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2114–2130"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148672596","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
Microfluidic Three-Dimensionally Printed Multicomponent Chinese Medicine Hydrogel Patches for Skin Photodamage Treatment 微流控三维打印多组分中药水凝胶贴片治疗皮肤光损伤
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-07-01 DOI: 10.1021/acsmaterialslett.6c00488
Xuan Wang, Xinyue Cao, Lingbao Zeng, Yuanjin Zhao
{"title":"Microfluidic Three-Dimensionally Printed Multicomponent Chinese Medicine Hydrogel Patches for Skin Photodamage Treatment","authors":"Xuan Wang,&nbsp;Xinyue Cao,&nbsp;Lingbao Zeng,&nbsp;Yuanjin Zhao","doi":"10.1021/acsmaterialslett.6c00488","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00488","url":null,"abstract":"<p>Traditional Chinese medicine exhibits considerable therapeutic potential in skin photodamage treatment. Current research focuses on improving its delivery system and therapeutic effect. Here, microfluidic 3D-printed multicomponent Chinese medicine Crocin (CR) and <em>Dendrobium officinale</em> polysaccharide (DOP) hybrid hydrogel patches are proposed for promoting photodamaged skin repair. By using the 3D printing technology, CR and DOP mixed hydrogels have been spun and knitted into microfiber patches. Benefiting from the good biocompatibility, porous structure, and high moisture retention, the hydrogels could provide an ideal microenvironment for cellular survival. Meanwhile, the loaded CR and DOP could be effectively released and synergistically exhibit antioxidant and antibacterial properties, thus scavenging the excessive reactive oxygen species (ROS) and reducing the bacterial infection risks at the photodamaged sites. We believe that the microfluidic 3D-printed multicomponent Chinese medicine hydrogel patches are promising effective dressings for future skin photodamage management and cosmeceutical development.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2330–2338"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148666342","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
A Dual-Action Bletilla striata Polysaccharide Copolymer Attenuates Cartilage Degeneration in an In Vivo Osteoarthritis Rat Model 双作用白芨多糖共聚物减轻骨关节炎大鼠体内模型软骨退变
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-07-15 DOI: 10.1021/acsmaterialslett.6c00453
Lien-Chen Wu, Yu-Ying Lin, Yueh-Ying Hsieh, Che-Yung Kuan, Chang-Jung Chiang, Feng-Huei Lin
{"title":"A Dual-Action Bletilla striata Polysaccharide Copolymer Attenuates Cartilage Degeneration in an In Vivo Osteoarthritis Rat Model","authors":"Lien-Chen Wu,&nbsp;Yu-Ying Lin,&nbsp;Yueh-Ying Hsieh,&nbsp;Che-Yung Kuan,&nbsp;Chang-Jung Chiang,&nbsp;Feng-Huei Lin","doi":"10.1021/acsmaterialslett.6c00453","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00453","url":null,"abstract":"<p>Osteoarthritis (OA) treatment via intra-articular (IA) hyaluronic acid is hindered by rapid degradation and poor chondroprotection. To address these limitations, this study engineered a dual-action IA biomaterial by cross-linking <em>Bletilla striata</em> polysaccharide (BSP) with poly(ethylene glycol) diglycidyl ether (PEGDE). The resulting copolymer (BSPP) exhibited a 15% molecular weight increase and enhanced aqueous stability, showing only 5% degradation on day 3 compared to the complete dissolution of pristine BSP. In vitro, BSPP exhibited excellent biocompatibility, enhancing chondrocyte viability to 124.02 ± 2.14%, and protected cells against lipopolysaccharide-induced stress. In vivo, in a monosodium iodoacetate-induced OA rat model, BSPP significantly alleviated pain, maintaining a mechanical pain threshold of 48.24 ± 1.93 g at week 3 compared to 21.03 ± 1.67 g in the untreated group. Histological analysis at week 4 confirmed cartilage preservation, reducing the OARSI histopathology score from 9.714 ± 3.74 to 2.10 ± 1.52.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2339–2344"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148666418","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
Dual Optical Sensing of Temperature and Low Oxygen Partial Pressure Using a Thermally Activated Delayed Fluorescence Organic Material 利用热激活延迟荧光有机材料的温度和低氧分压双光学传感
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-06-24 DOI: 10.1021/acsmaterialslett.6c00438
Christian Hernández-Álvarez, Marcin Runowski, Michał Mońka, Sebastian Mahlik, Illia E. Serdiuk
{"title":"Dual Optical Sensing of Temperature and Low Oxygen Partial Pressure Using a Thermally Activated Delayed Fluorescence Organic Material","authors":"Christian Hernández-Álvarez,&nbsp;Marcin Runowski,&nbsp;Michał Mońka,&nbsp;Sebastian Mahlik,&nbsp;Illia E. Serdiuk","doi":"10.1021/acsmaterialslett.6c00438","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00438","url":null,"abstract":"<p>Although luminescent materials enable noninvasive optical sensing for biomedical and industrial applications, their implementation remains limited by narrow operating ranges, complex synthesis and low sensitivity. Here, we present NAPAcI, a luminescent material that functions as a dual optical sensor for pressure and temperature. Under UV excitation, its photoluminescence shows strong dependence on oxygen pressure and temperature. The emission response was calibrated using an extended Stern−Volmer equation for ratiometric sensing. The remarkable sensing performance is attributed to thermally activated delayed fluorescence, enhanced by the heavy-atom effect of the iodine substituents. This design promotes ultrafast intersystem crossing on the subnanosecond scale and reverse intersystem crossing within tens of nanoseconds, while significantly reducing the prompt fluorescence rate, thereby tailoring the material for air-pressure sensing. Consequently, NAPAcI exhibits low measurement uncertainty, high repeatability, and robust performance. These results position NAPAcI as a cost-effective platform for optical pressure and temperature monitoring.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2283–2290"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148666550","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
Mechanochemical Landscapes of Carbon Electrodes Differentially Modulate Li, Na, and K Interactions 碳电极的机械化学景观差异调节Li, Na和K的相互作用
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-07-09 DOI: 10.1021/acsmaterialslett.6c00394
Abebaw Seyume, Sampad Mandal, Sayan Banerjee
{"title":"Mechanochemical Landscapes of Carbon Electrodes Differentially Modulate Li, Na, and K Interactions","authors":"Abebaw Seyume,&nbsp;Sampad Mandal,&nbsp;Sayan Banerjee","doi":"10.1021/acsmaterialslett.6c00394","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00394","url":null,"abstract":"<p>Carbon-based electrodes are widely used anodes for Li-, Na-, and K-ion batteries. Using first-principles calculations, we show that the mechanochemical landscape of rippled graphene distinctly modulates Na/K and Li binding and diffusion. The vectorial nature of curvature—positive valley-shaped versus negative mountain-shaped regions—strongly affects Na– and K–graphene interactions, whereas Li–graphene interactions remain comparatively insensitive. Na and K binding is governed by the number of weak ion–C interactions: valley regions support a more delocalized interaction network, while mountain regions favor localized binding. In contrast, Li binding remains largely local and is therefore less affected by curvature. Consequently, Na and K are more susceptible than Li to longer-range deformation effects and exhibit anisotropic diffusion on curved electrodes, whereas Li diffusion remains largely isotropic. These results identify deformation-aware nanostructuring as a promising route toward improved Na- and K-ion battery electrodes.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2249–2254"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148675495","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
Photoinduced Charge-Transfer Enables Dynamic Photochromism and Fluorochromism in Polymer Matrix 光致电荷转移使聚合物基质中的动态光致变色和荧光致变色成为可能
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-07-09 DOI: 10.1021/acsmaterialslett.6c00512
Huakai Qiu, Zhixi Su, Wuzhen Luo, Xin Wang, Shunyou Cai, Feiming Li, Jingbin Zeng, Zhixiong Cai
{"title":"Photoinduced Charge-Transfer Enables Dynamic Photochromism and Fluorochromism in Polymer Matrix","authors":"Huakai Qiu,&nbsp;Zhixi Su,&nbsp;Wuzhen Luo,&nbsp;Xin Wang,&nbsp;Shunyou Cai,&nbsp;Feiming Li,&nbsp;Jingbin Zeng,&nbsp;Zhixiong Cai","doi":"10.1021/acsmaterialslett.6c00512","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00512","url":null,"abstract":"<p>Photo-stimuli-responsive luminescent materials are limited in application due to poor stability of their excited states. In donor-acceptor organic systems, photoinduced charge transfer and triplet-state dynamics are strongly governed by molecular interactions and environmental confinement, but their mechanistic regulation remains incompletely understood. Herein, we report a facile strategy to construct dynamic luminescent thin films by incorporating an electron acceptor and tertiary amine donors into a poly(methyl methacrylate) (PMMA) matrix. Photoinduced charge-transfer complexes (PCTCs) are generated in situ. The resulting modulation of charge-transfer and localized triplet states leads to prolonged excited-state lifetimes and distinct emission behaviors, exhibiting color-tunable emission spanning from blue fluorescence to green, yellow, and red, along with a visible orange-yellow afterglow persisting for 2 s. This work elucidates a matrix-assisted mechanism for regulating excited-state dynamics and provides general design principles for stable, high-contrast photoresponsive luminescent materials applicable to anti-counterfeiting and optical patterning.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2345–2353"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148666352","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
Halogenated Organic Laser Emitters for X-ray Imaging 用于x射线成像的卤化有机激光发射器
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-06-26 DOI: 10.1021/acsmaterialslett.6c00446
Zuofang Feng, Haina Feng, Chaoyi Han, Huili Ma, Zhengong Meng, Yilong Lei
{"title":"Halogenated Organic Laser Emitters for X-ray Imaging","authors":"Zuofang Feng,&nbsp;Haina Feng,&nbsp;Chaoyi Han,&nbsp;Huili Ma,&nbsp;Zhengong Meng,&nbsp;Yilong Lei","doi":"10.1021/acsmaterialslett.6c00446","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00446","url":null,"abstract":"<p>Organic laser materials, leveraging their inherent high photoluminescence efficiency and ultrashort radiative lifetime, exhibit efficient singlet exciton radiation, making them promising building blocks for ultrafast scintillators. Herein, we propose a nonmacrocyclic cocrystal engineering strategy to address the long-standing trade-off between heavy-atom-enhanced X-ray absorption and fluorescence quenching. By employing a sterically hindered distyrylbenzene (DSB) derivative as a host to encapsulate halogenated terphenyl guests, we construct cavity-adaptive cocrystals (CACs) with laser emission characteristics, achieving synergistic optimization of high X-ray absorption and ultrafast radioluminescence. The best-performing dibrominated CAC microribbons (MRs) exhibit an ultralow detection limit (71.12 nGy/s), high spatial resolution (17 lp/mm), and rapid X-ray response. This work demonstrates that the CACs, guided by a host/guest functional separation principle, offer a versatile platform for developing high-performance, ultrafast organic scintillators, with transformative potential for real-time medical imaging.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2300–2307"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148666632","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
Gradient Enhancement of Ligand Dipole Moment and Confinement Effect in Metal–Organic Frameworks for Boosting Sulfur Hexafluoride–Nitrogen Separation 金属-有机骨架中配体偶极矩梯度增强及约束效应促进六氟化硫-氮分离
IF 8.6 1区 化学
ACS Materials Letters Pub Date : 2026-08-03 Epub Date: 2026-07-19 DOI: 10.1021/acsmaterialslett.6c00486
Limin Wang, Shengjie Lin, Yibo Wang, Yuxuan Du, Yaning Qiao, Yabing He
{"title":"Gradient Enhancement of Ligand Dipole Moment and Confinement Effect in Metal–Organic Frameworks for Boosting Sulfur Hexafluoride–Nitrogen Separation","authors":"Limin Wang,&nbsp;Shengjie Lin,&nbsp;Yibo Wang,&nbsp;Yuxuan Du,&nbsp;Yaning Qiao,&nbsp;Yabing He","doi":"10.1021/acsmaterialslett.6c00486","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.6c00486","url":null,"abstract":"<p>Replacing pure SF<sub>6</sub> with SF<sub>6</sub>/N<sub>2</sub> mixtures curbs emissions but demands efficient low-concentration SF<sub>6</sub> recovery. We report a gradient enhancement strategy combining cis-trans isomerism and methylation to boost ligand dipole moment and confinement in three isostructural partitioned acs-MOFs (<strong>ZJNU-181-trans</strong>, <strong>-cis</strong>, and <strong>-2Me</strong>). Pre-synthesis DFT predictions of SF<sub>6</sub> affinity (<strong>2Me</strong> &gt; <strong>cis</strong> &gt; <strong>trans</strong>) are validated experimentally. At 298 K and 10 kPa, SF<sub>6</sub> uptake follows <strong>2Me</strong> &gt; <strong>cis</strong> &gt; <strong>trans</strong>, consistent with isosteric heats and IAST selectivity (169.8 for <strong>2Me</strong>). Breakthrough tests confirm this order, with <strong>2Me</strong> showing the largest SF<sub>6</sub>/N<sub>2</sub> breakthrough gap (141.5 min g<sup>–1</sup>) and excellent recyclability. DFT reveals that methyl groups act as additional C–H···F donors while creating uniform 7.3 Å pores, synergistically enhancing SF<sub>6</sub> binding to –33.04 kJ mol<sup>–1</sup>. This work establishes gradient dipole-confinement modulation as a generalizable MOF design paradigm.</p>","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"8 8","pages":"2323–2329"},"PeriodicalIF":8.6,"publicationDate":"2026-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148672472","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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