ACS Combinatorial Science最新文献

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All Roads Lead to Rome: Isomers with Divergent Cathode Modification Mechanisms toward Ohmic Contact 条条大路通罗马:具有不同阴极改性机制的异构体实现欧姆接触
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-25 DOI: 10.1021/jacs.4c0956710.1021/jacs.4c09567
Huanxiang Jiang*, Qi Liang, Haishuo Guo, Andong Zhang*, Xuewen Wang, Zheng Tang and Zhishan Bo*, 
{"title":"All Roads Lead to Rome: Isomers with Divergent Cathode Modification Mechanisms toward Ohmic Contact","authors":"Huanxiang Jiang*,&nbsp;Qi Liang,&nbsp;Haishuo Guo,&nbsp;Andong Zhang*,&nbsp;Xuewen Wang,&nbsp;Zheng Tang and Zhishan Bo*,&nbsp;","doi":"10.1021/jacs.4c0956710.1021/jacs.4c09567","DOIUrl":"https://doi.org/10.1021/jacs.4c09567https://doi.org/10.1021/jacs.4c09567","url":null,"abstract":"<p >Cathode interfacial layers (CILs) hold utmost importance for achieving ohmic contact at the organic semiconductor–cathode interface of organic photovoltaic devices. Delving deep into diverse design principles and working mechanisms is of great significance for designing novel CILs with high performance. Herein, two novel nonamine-based CILs are designed: one featuring a cyclopentadiene unit, designated as CIL-cp; while the other, lacking cyclopentadiene, is referred to as CIL-ph, which is an isomer of CIL-cp. The subtle changes in chemical structures result in distinct modification mechanisms toward ohmic contact. On one hand, the robust electron-withdrawing characteristic of cyclopentadiene endows CIL-cp with lower energy levels, resulting in an interfacial dipole at the active layer–CIL-cp interface due to electron transfer from D18 to CIL-cp. On the other hand, CIL-ph exhibits a strong interfacial dipole at the CIL–Ag interface, which significantly reduces the work function (W<sub>F</sub>) of the silver electrode. Both CIL-cp and CIL-ph demonstrate excellent interfacial modification capability, whereas CIL-cp possesses a stronger electron extraction ability, thus leading to a high power conversion efficiency of 19.31% in the D18:L8-BO system. Our results reveal the distinctive operational mechanism of cyclopentadiene-based CILs, thus offering innovative design ideas for CIL materials.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30262–30271 30262–30271"},"PeriodicalIF":14.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Role of Oxide-Derived Cu on the Initial Elementary Reaction Intermediate During Catalytic CO2 Reduction 氧化物衍生的铜在催化二氧化碳还原过程中对初始基本反应中间体的作用
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-25 DOI: 10.1021/jacs.4c0860310.1021/jacs.4c08603
Zhiwen Jiang, Carine Clavaguéra, Sergey A. Denisov, Jun Ma* and Mehran Mostafavi*, 
{"title":"Role of Oxide-Derived Cu on the Initial Elementary Reaction Intermediate During Catalytic CO2 Reduction","authors":"Zhiwen Jiang,&nbsp;Carine Clavaguéra,&nbsp;Sergey A. Denisov,&nbsp;Jun Ma* and Mehran Mostafavi*,&nbsp;","doi":"10.1021/jacs.4c0860310.1021/jacs.4c08603","DOIUrl":"https://doi.org/10.1021/jacs.4c08603https://doi.org/10.1021/jacs.4c08603","url":null,"abstract":"<p >The catalytic role of oxide-derived Cu (OD-Cu) in promoting CO<sub>2</sub> reduction (CO<sub>2</sub>R) to C<sub>2+</sub> products has been appreciated for decades. However, the dynamic evolution of the surface oxidation states, together with their real correlation to the binding of reaction intermediates, remains unclear due to technical challenges. Here, we show the time-resolved spectroscopic signatures of key OD-Cu-CO<sub>2</sub><sup>•–</sup> intermediates during catalytic CO<sub>2</sub> reduction through one electron transfer from nanoseconds to seconds time scale. We generated the initial intermediate CO<sub>2</sub><sup>•–</sup> radicals in the bulk solution and monitored the interfacial reaction kinetics with well-defined OD-Cu (Cu(0), Cu(I), and Cu(II)) nanoparticles. Combined with molecular simulations, transient absorption profiles analysis reveals that Cu(I) induced a faster CO<sub>2</sub><sup>•–</sup> radical coupling reaction than Cu(0), whereas Cu(II) is only reduced to Cu(I) by the CO<sub>2</sub><sup>•–</sup> radical. Furthermore, the newly developed multistep cumulative pulse methodology uncovered the transition in chemical states of mixed OD-Cu during radical coupling reactions. This pulse radiolysis study provides compelling evidence for the beneficial role of subsurface oxides in early time catalytic CO<sub>2</sub> transformation.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30164–30173 30164–30173"},"PeriodicalIF":14.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585555","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Topological Band Engineering of One-Dimensional π-d Conjugated Metal–Organic Frameworks 一维π-d共轭金属有机框架的拓扑带工程
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-25 DOI: 10.1021/jacs.4c1178210.1021/jacs.4c11782
Tingfeng Zhang, Nuoyu Su, Tianyi Hu, Weihua Wang* and Zhengfei Wang*, 
{"title":"Topological Band Engineering of One-Dimensional π-d Conjugated Metal–Organic Frameworks","authors":"Tingfeng Zhang,&nbsp;Nuoyu Su,&nbsp;Tianyi Hu,&nbsp;Weihua Wang* and Zhengfei Wang*,&nbsp;","doi":"10.1021/jacs.4c1178210.1021/jacs.4c11782","DOIUrl":"https://doi.org/10.1021/jacs.4c11782https://doi.org/10.1021/jacs.4c11782","url":null,"abstract":"<p >One-dimensional (1D) <i>π-d</i> conjugated metal–organic frameworks (c-MOFs) have garnered widespread research interest in chemical energy storage and conversion. In this work, we introduce a universal principle to engineer the topological bands of 1D c-MOFs. Connected by <i>d</i> orbitals of transition metals, two equivalent hidden molecular π orbitals in 1D c-MOFs can generate a staggered hopping within and between the organic ligands, forming Su–Schrieffer–Heeger-shaped 1D topological bands. Guided by this discovery, we investigate the electronic structures of the typical 1D c-MOF assembled from Ni atoms and 2HQDI (QDI = 2,5-diamino-1,4-benzoquinonediimine) precursors (NiQDI) by first-principles calculations, revealing 1D topological bands around the Fermi level. Due to local bonding variations at the QDI terminations, these two hidden molecular π orbitals become atomically bonded but electronically separated at the edge QDI, creating spatially localized in-gap topological edge states at the end of the NiQDI chain. This definitive signature for 1D topological bands is identified through differential conductance spectra in scanning tunneling microscopy measurements. Our results provide conclusive experimental evidence for topological bands in 1D c-MOFs, paving the way for exploring the topological physics in organic materials through frontier molecular orbitals.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30539–30547 30539–30547"},"PeriodicalIF":14.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Phototriggered Hydrogen Persulfide Donors via Hydrosulfide Radical Formation Enhancing the Reactive Sulfur Metabolome in Cells 通过氢硫化物自由基的形成增强细胞中活性硫代谢组的光诱导过硫化氢供体
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-25 DOI: 10.1021/jacs.4c1154010.1021/jacs.4c11540
Biswajit Roy, Meg Shieh, Tsuyoshi Takata, Minkyung Jung, Eshani Das, Shi Xu, Takaaki Akaike and Ming Xian*, 
{"title":"Phototriggered Hydrogen Persulfide Donors via Hydrosulfide Radical Formation Enhancing the Reactive Sulfur Metabolome in Cells","authors":"Biswajit Roy,&nbsp;Meg Shieh,&nbsp;Tsuyoshi Takata,&nbsp;Minkyung Jung,&nbsp;Eshani Das,&nbsp;Shi Xu,&nbsp;Takaaki Akaike and Ming Xian*,&nbsp;","doi":"10.1021/jacs.4c1154010.1021/jacs.4c11540","DOIUrl":"https://doi.org/10.1021/jacs.4c11540https://doi.org/10.1021/jacs.4c11540","url":null,"abstract":"<p >Hydrogen persulfide (H<sub>2</sub>S<sub>2</sub>) is an important sulfur-containing signaling molecule that plays a crucial role in the homeostasis of various organ systems, such as the renal, cardiovascular, liver, and gastrointestinal systems. However, research on H<sub>2</sub>S<sub>2</sub> in biological settings is still challenging due to its instability and high reactivity. Compounds that can controllably release H<sub>2</sub>S<sub>2</sub> (also known as donors) are thus crucial research tools. Currently, available H<sub>2</sub>S<sub>2</sub> donors are still very limited, with most of them relying on modified disulfide templates. These templates possess an unavoidable limitation of being susceptible to cellular disulfide exchange which can compromise their efficacy. In this work, we explored nondisulfide-based and nonoxidation-dependent templates for the design of H<sub>2</sub>S<sub>2</sub> donors. We found that tertiary naphthacyl thiols could undergo phototriggered C–S homolytic cleavage to form H<sub>2</sub>S<sub>2</sub> via hydrosulfide (HS) radicals. In addition, the release of H<sub>2</sub>S<sub>2</sub> was associated with the formation of a product with strong blue fluorescence, which allowed for real-time monitoring of the release process. This reaction was demonstrated to proceed effectively in both buffers and cells, with the ability to enhance intracellular production of persulfides, including GSSH, CysSSH, H<sub>2</sub>S<sub>2</sub>, H<sub>2</sub>S<sub>3</sub>, etc. It provides a unique photocontrolled H<sub>2</sub>S<sub>2</sub> donor system with distinct advantages compared to known H<sub>2</sub>S<sub>2</sub> donors due to its good stability and spatiotemporal control ability.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30502–30509 30502–30509"},"PeriodicalIF":14.4,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Upside-Down Adsorption: The Counterintuitive Influences of Surface Entropy and Surface Hydroxyl Density on Hydrogen Spillover 颠倒吸附:表面熵和表面羟基密度对氢溢出的反直觉影响
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-24 DOI: 10.1021/jacs.4c0753910.1021/jacs.4c07539
Kelle D. Hart, Margaret J. Hollobaugh, Audrey M. Battiste, Tae Yong Yun, Angela Pathickal Abraham, Mohammad Hamidizirasefi, Ian M. Loscher and Bert D. Chandler*, 
{"title":"Upside-Down Adsorption: The Counterintuitive Influences of Surface Entropy and Surface Hydroxyl Density on Hydrogen Spillover","authors":"Kelle D. Hart,&nbsp;Margaret J. Hollobaugh,&nbsp;Audrey M. Battiste,&nbsp;Tae Yong Yun,&nbsp;Angela Pathickal Abraham,&nbsp;Mohammad Hamidizirasefi,&nbsp;Ian M. Loscher and Bert D. Chandler*,&nbsp;","doi":"10.1021/jacs.4c0753910.1021/jacs.4c07539","DOIUrl":"https://doi.org/10.1021/jacs.4c07539https://doi.org/10.1021/jacs.4c07539","url":null,"abstract":"<p >Although hydrogen spillover is often invoked to explain anomalies in catalysis, spillover remains a poorly understood phenomenon. Hydrogen spillover (H*) is best described as highly mobile H atom equivalents that arise when H<sub>2</sub> migrates from a metal nanoparticle to an oxide or carbon support. In the 60 years since its discovery, few methods have become available to quantify or characterize H*-support interactions. We recently showed <i>in situ</i> infrared spectroscopy and volumetric chemisorption can quantify reversible H<sub>2</sub> adsorption on Au/TiO<sub>2</sub> catalysts, where adsorbed hydrogen exists as H* and interacts with titania surface hydroxyl (TiOH) groups. Here, we report parallel thermogravimetric analysis and Fourier transform infrared spectroscopy methods for systematically manipulating the surface TiOH density. We examine the role of surface hydroxylation on spillover thermodynamics using van't Hoff studies to determine apparent adsorption enthalpies and entropies at constant H* coverage, which is necessary to maintain constant H* translational entropy. Although surface TiOH groups are the likely adsorption sites, the data show removing hydroxyl groups increases spillover. This surprising finding─that adsorption increases as the adsorption site density decreases─is associated with improved thermodynamics on dehydroxylated surfaces. A strong adsorption enthalpy–entropy correlation implicates the changing surface entropy of the titania support itself (i.e., an initial state effect) is deeply intertwined with the H* configurational entropy. These effects are surprising and should apply to all low-coverage adsorbates where entropy terms dominate more traditional enthalpic considerations. Moreover, this study points toward a kinetic test for invoking spillover in a reaction mechanism: namely, in situ dehydroxylation should enhance spillover processes.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30091–30103 30091–30103"},"PeriodicalIF":14.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585585","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
π-Conjugation-Induced In Situ Nanoscale Ordering of Spiro-OMeTAD Boosts the Efficiency and Stability of Perovskite Solar Cells π-共轭诱导的螺环-OMeTAD 原位纳米级有序化提高了过氧化物太阳能电池的效率和稳定性
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-24 DOI: 10.1021/jacs.4c0909410.1021/jacs.4c09094
Tao Zhao, Xi Jin, Ming-Hua Li*, Jun Li, Sunfa Wang, Zhongyang Zhang, Peng Sun, Shiju Lin, Qi Chen, Jin-Song Hu*, Yao Li* and Yan Jiang*, 
{"title":"π-Conjugation-Induced In Situ Nanoscale Ordering of Spiro-OMeTAD Boosts the Efficiency and Stability of Perovskite Solar Cells","authors":"Tao Zhao,&nbsp;Xi Jin,&nbsp;Ming-Hua Li*,&nbsp;Jun Li,&nbsp;Sunfa Wang,&nbsp;Zhongyang Zhang,&nbsp;Peng Sun,&nbsp;Shiju Lin,&nbsp;Qi Chen,&nbsp;Jin-Song Hu*,&nbsp;Yao Li* and Yan Jiang*,&nbsp;","doi":"10.1021/jacs.4c0909410.1021/jacs.4c09094","DOIUrl":"https://doi.org/10.1021/jacs.4c09094https://doi.org/10.1021/jacs.4c09094","url":null,"abstract":"<p >Spiro-OMeTAD hole transport materials typically exhibit an amorphous state in perovskite solar cells. However, the lack of structural ordering leads to weak intermolecular interaction, inferior carrier transfer, and poor stability in devices. Herein, we developed a π-conjugation-induced short-range ordering strategy to modulate the stacking order of spiro-OMeTAD during film formation. A clear molecular ordering at the nanoscale is observed, which enhances intermolecular π–π stacking in spiro-OMeTAD and enables effective carrier extraction and favorable energy level alignment. The nanoscale-ordered spiro-OMeTAD allows the achievement of perovskite solar cells with a champion efficiency of 25.37%, surpassing devices utilizing amorphous spiro-OMeTAD (23.52%). The unencapsulated device demonstrates enhanced operational stability by retaining 98% of its initial efficiency under continuous 1 sun equivalent illumination at 60 °C for 840 h. This work establishes a significant and valid modulation concept for the stacking order of organic transport materials, paving the way for the development of efficient and stable perovskite solar cells.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 45","pages":"30893–30900 30893–30900"},"PeriodicalIF":14.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608615","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Structural Plasticity as a Driver of the Maturation of Pro-Interleukin-18 结构可塑性是前白细胞介素-18 成熟的驱动力
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-24 DOI: 10.1021/jacs.4c0980510.1021/jacs.4c09805
Jeffrey P. Bonin*, James M. Aramini and Lewis E. Kay*, 
{"title":"Structural Plasticity as a Driver of the Maturation of Pro-Interleukin-18","authors":"Jeffrey P. Bonin*,&nbsp;James M. Aramini and Lewis E. Kay*,&nbsp;","doi":"10.1021/jacs.4c0980510.1021/jacs.4c09805","DOIUrl":"https://doi.org/10.1021/jacs.4c09805https://doi.org/10.1021/jacs.4c09805","url":null,"abstract":"<p >Dynamics are often critical for biomolecular function. Herein we explore the role of motion in driving the maturation process of pro-IL-18, a potent pro-inflammatory cytokine that is cleaved by caspases-1 and -4 to generate the mature form of the protein. An NMR dynamics study of pro-IL-18, probing time scales over 12 orders of magnitude and focusing on <sup>1</sup>H, <sup>13</sup>C, and <sup>15</sup>N spin probes along the protein backbone and amino-acid side chains, reveals a plastic structure, with millisecond time scale dynamics occurring in a pair of β-strands, β1 and β*, that show large structural variations in a comparison of caspase-free and bound pro-IL-18 states. Fits of the relaxation data to a three-site model of exchange showed that the ground state secondary structure is maintained in the excited conformers, with the side chain of I48 that undergoes a buried-to-exposed conformational change in the caspase-free to -bound transition of pro-IL-18, sampling a more extensive range of torsion angles in one of the excited states characterized, suggesting partial unpacking in this region. Hydrogen exchange measurements establish the occurrence of an additional process, whereby strands β1 and β* locally unfold. Our data are consistent with a hierarchy of dynamic events that likely prime pro-IL-18 for facile caspase binding.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30281–30293 30281–30293"},"PeriodicalIF":14.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Covalent Bonds versus van der Waals Forces: A Picture in Thermal Conduction of Organic Materials 共价键与范德华力:有机材料热传导的图景
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-24 DOI: 10.1021/jacs.4c1184910.1021/jacs.4c11849
Ryosuke Takehara, Tomoya Fukui, Taketo Tano, Meguya Ryu, Suguru Kitani, Hitoshi Kawaji, Junko Morikawa* and Takanori Fukushima*, 
{"title":"Covalent Bonds versus van der Waals Forces: A Picture in Thermal Conduction of Organic Materials","authors":"Ryosuke Takehara,&nbsp;Tomoya Fukui,&nbsp;Taketo Tano,&nbsp;Meguya Ryu,&nbsp;Suguru Kitani,&nbsp;Hitoshi Kawaji,&nbsp;Junko Morikawa* and Takanori Fukushima*,&nbsp;","doi":"10.1021/jacs.4c1184910.1021/jacs.4c11849","DOIUrl":"https://doi.org/10.1021/jacs.4c11849https://doi.org/10.1021/jacs.4c11849","url":null,"abstract":"<p >We present a direct comparison of the heat transport properties between the state in which the constituent molecules are assembled by intermolecular forces and the one in which they are covalently bonded, in a molecular system with identical constituent elements and masses, as well as a nearly identical structure and density. This comparison leading to an essential understanding of thermal conduction in organic materials is made possible by the unique compound found by Wudl et al., which exhibits a single-crystal-to-single-crystal topochemical polymerization with a yield of &gt;99%, in combination with microtemperature wave analysis (<i>μ</i>TWA), which allows accurate measurements of the thermal diffusivity of small single crystals. At room temperature, the thermal conductivity of monomer and polymer single crystals is not significantly different. For both crystals, the thermal conductivity increases monotonically with decreasing temperature. However, below the Debye temperature, the thermal conductivity of the polymer single crystal increases exponentially, giving much larger values than those of the monomer single crystal. Based on physical quantities related to the behavior of phonons, derived from the specific heat analysis, we discuss the differences in heat transport properties in the two states and provide guidelines for achieving high thermal conductivity in organic materials.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30548–30552 30548–30552"},"PeriodicalIF":14.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c11849","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585744","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-Entropy Magnet Enabling Distinctive Thermal Expansions in Intermetallic Compounds 高熵磁体实现金属间化合物的独特热膨胀性
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-24 DOI: 10.1021/jacs.4c1068110.1021/jacs.4c10681
Jinghan Li, Kun Lin*, Hankun Xu, Wanda Yang, Qian Zhang, Chengyi Yu, Qinghua Zhang, Jing Chen, Chin-Wei Wang, Kenichi Kato, Shogo Kawaguchi, Li You, Yili Cao, Qiang Li, Xin Chen, Jun Miao, Jinxia Deng and Xianran Xing, 
{"title":"High-Entropy Magnet Enabling Distinctive Thermal Expansions in Intermetallic Compounds","authors":"Jinghan Li,&nbsp;Kun Lin*,&nbsp;Hankun Xu,&nbsp;Wanda Yang,&nbsp;Qian Zhang,&nbsp;Chengyi Yu,&nbsp;Qinghua Zhang,&nbsp;Jing Chen,&nbsp;Chin-Wei Wang,&nbsp;Kenichi Kato,&nbsp;Shogo Kawaguchi,&nbsp;Li You,&nbsp;Yili Cao,&nbsp;Qiang Li,&nbsp;Xin Chen,&nbsp;Jun Miao,&nbsp;Jinxia Deng and Xianran Xing,&nbsp;","doi":"10.1021/jacs.4c1068110.1021/jacs.4c10681","DOIUrl":"https://doi.org/10.1021/jacs.4c10681https://doi.org/10.1021/jacs.4c10681","url":null,"abstract":"<p >The high-entropy strategy has gained increasing popularity in the design of functional materials due to its four core effects. In this study, we introduce the concept of a “high-entropy magnet (HEM)”, which integrates diverse magnetic compounds within a single phase and is anticipated to demonstrate unique magnetism-related properties beyond that of its individual components. This concept is exemplified in AB<sub>2</sub>-type layered Kagome intermetallic compounds (Ti,Zr,Hf,Nb,Fe)Fe<sub>2</sub>. It is revealed that the competition among individual magnetic states and the presence of magnetic Fe in originally nonmagnetic high-entropy sites lead to intricate magnetic transitions with temperature. Consequently, unusual transformations in thermal expansion property (from positive to zero, negative, and back to near zero) are observed. Specifically, a near-zero thermal expansion is achieved over a wide temperature range (10–360 K, α<sub>v</sub> = −0.62 × 10<sup>–6</sup> K<sup>–1</sup>) in the A-site equal-atomic ratio (Ti<sub>1/5</sub>Zr<sub>1/5</sub>Hf<sub>1/5</sub>Nb<sub>1/5</sub>Fe<sub>1/5</sub>)Fe<sub>2</sub> compound, which is associated with successive deflection of average Fe moments. The HEM strategy holds promise for discovering new functionalities in solid materials.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30380–30387 30380–30387"},"PeriodicalIF":14.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585743","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Implementation of Digital Computing by Colloidal Crystal Engineering with DNA 利用 DNA 胶体晶体工程实现数字计算
IF 14.4 3区 化学
ACS Combinatorial Science Pub Date : 2024-10-24 DOI: 10.1021/jacs.4c1207810.1021/jacs.4c12078
Xiaoyu Liu, Dongbao Yao*, Yun Wang, Dian Ni, Wenqiang Hua*, Jie Tian, Liulin Yang, Haixin Lin, Haojun Liang and Zhaoxiang Deng*, 
{"title":"Implementation of Digital Computing by Colloidal Crystal Engineering with DNA","authors":"Xiaoyu Liu,&nbsp;Dongbao Yao*,&nbsp;Yun Wang,&nbsp;Dian Ni,&nbsp;Wenqiang Hua*,&nbsp;Jie Tian,&nbsp;Liulin Yang,&nbsp;Haixin Lin,&nbsp;Haojun Liang and Zhaoxiang Deng*,&nbsp;","doi":"10.1021/jacs.4c1207810.1021/jacs.4c12078","DOIUrl":"https://doi.org/10.1021/jacs.4c12078https://doi.org/10.1021/jacs.4c12078","url":null,"abstract":"<p >Toehold-mediated strand displacement (TMSD) provides a versatile toolbox for developing DNA digital computing systems. Although different logic circuits with diverse functions have achieved good performance in terms of complexity and scalability, most previous DNA logic circuits perform information processing only at the molecular level, and nonspecific signal leakages are often difficult to avoid. Here, we demonstrate the feasibility of constructing leakless digital computing systems in three-dimensionally ordered colloidal supercrystals. These systems possess a unique signal leakage resistance by integrating different TMSD-based logic gates with the catalytic assembly of DNA-functionalized gold colloids. A complete set of basic Boolean logic gates and different cascaded logic circuits is constructed on the basis of the catalytic assembly strategy enabled by a facilely designed catassembler, where the output signals are recognized by determining whether specific colloidal supercrystals are formed or not. In addition, a half adder is built through a combination of XOR and AND logic gates with two distinct crystal types as readouts. Finally, a leakless two-digit DNA keypad lock for information security protection is demonstrated. The combination of TMSD-based logic circuits with the universal nanoparticle catalytic assembly offers the possibility to develop highly complicated and leakage-free digital computing systems and promotes macroscopic colloidal superlattice materials with programmable logic functions.</p>","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30573–30583 30573–30583"},"PeriodicalIF":14.4,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585583","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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