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Disentangling Cooperative Electron Correlation and Primary Coordination Sphere Effects in [4Fe-4S]+ Structural Isomerism and π-Acid Activation [4Fe-4S]+结构异构和π-酸活化中的协同电子相关解缠及初级配位球效应
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acs.jpclett.5c03723
Shelby T. Davis, Daniel Gibney, Jan-Niklas Boyn
Iron–sulfur (Fe–S) clusters are ubiquitous cofactors known to perform critical biological functions like multielectron transfer and redox catalysis within complex enzymatic frameworks, making them promising targets for the rational design of modular, bioinspired catalysts and materials. Advancements have been made toward establishing structure–function-activity relationships through synthesis and structural characterization of biomimetic Fe–S clusters. However, their conformational plasticity and multiconfigurational character pose significant challenges in capturing the underlying electronic structure. The treatment of both strong and dynamic correlation effects is integral in bridging the gap between electronic and physical structure to rationalize metallocluster reactivity. Here, we employ a computationally tractable, multireference methodology that captures both strong and dynamic correlation effects to simulate a series of chemically and electronically diverse, site-differentiated [4Fe-4S]+ clusters, elucidating the effects of cooperative electron correlation and primary coordination sphere modification on electron and spin (de)localization, geometric isomerism, and chemical reactivity.
铁硫(Fe-S)簇是普遍存在的辅助因子,已知在复杂的酶框架中执行关键的生物功能,如多电子转移和氧化还原催化,使它们成为合理设计模块化,仿生催化剂和材料的有希望的目标。仿生Fe-S簇的合成和结构表征在建立结构-功能-活性关系方面取得了进展。然而,它们的构象可塑性和多构型特征对捕获潜在的电子结构提出了重大挑战。强关联效应和动态关联效应的处理对于弥合电子和物理结构之间的差距以使金属团簇反应性合理化是不可或缺的。在这里,我们采用了一种计算易于处理的多参考方法,该方法捕获了强相关性和动态相关性效应,模拟了一系列化学和电子多样性,位点分化的[4Fe-4S]+簇,阐明了协同电子相关性和主配位球修饰对电子和自旋(去)定位,几何异构和化学反应性的影响。
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引用次数: 0
Ambient Tunneling Microscopy of Surface Annealing and Ligand Exchange Reactions on Metal–Organic Chalcogenolates 金属-有机硫代酸盐表面退火和配体交换反应的环境隧道显微镜研究
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acs.jpclett.5c03885
Chamathka Dehiwala Liyanage, Anietie W. Williams, Qiaoling Fan, Mariya Aleksich, Thilini M. Dinamithra, Brian G. Willis, Kerry Gilmore, J. Nathan Hohman
We introduce the use of scanning tunneling microscopy (STM) on microcrystalline metal–organic chalcogenolates (MOChas). We demonstrate the suitability of these compounds as STM substrates directly after drop casting onto graphitic surfaces, followed by chemical treatment. We successfully imaged 1-dimensional (1D) silver(I) methyl 2-mercaptobenzoate (2MMB) and the archetypical 2-dimensional (2D) MOCha, silver(I) benzeneselenolate (mithrene). The resolution afforded by STM was used to make new insights into the surface chemistry and displacement reactions. We observed the annealing and displacement reactions of mithrene and 2MMB and the transformation of the former into 2D silver(I) n-nonaneselenolate. MOCha crystals are amenable to STM imaging directly as-prepared from powders, despite the presence of its insulating organic units. We observed defects, crystal growth dynamics, and the formation of grains and superstructures. Visualizing such topographical heterogeneities could prove vital for understanding bulk functionality in this optoelectronic material class.
本文介绍了扫描隧道显微镜(STM)在微晶金属-有机硫代酸盐(MOChas)上的应用。我们证明了这些化合物在滴铸到石墨表面后直接作为STM衬底的适用性,然后进行化学处理。我们成功地成像了一维(1D)银(I)甲基2-巯基苯甲酸酯(2MMB)和典型的二维(2D) MOCha,银(I)苯烯酸酯(甲基)。STM提供的分辨率用于对表面化学和位移反应有新的认识。我们观察了米二烯和2MMB的退火和位移反应,以及前者转化为二维银(I) n-壬壬烯酸盐。尽管存在绝缘有机单元,但MOCha晶体可以直接从粉末中制备STM成像。我们观察了缺陷、晶体生长动力学以及晶粒和超结构的形成。可视化这种地形异质性对于理解这种光电材料类的体功能至关重要。
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引用次数: 0
Giant Room-Temperature Magnetocaloric Effect in Two-Dimensional Ternary Transition Metal Chalcogenides 二维三元过渡金属硫属化合物的巨室温磁热效应
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acs.jpclett.5c03908
Yangjun Hou, Xiong Xu, Guangwei Zhai, Chang Niu, Jiaxin Gan, Min Li, Hui Wang
We investigate the magnetic exchange interaction, magnetic anisotropy (MAE), and magnetocaloric effect (MCE) of ternary transition metal chalcogenides A2MX4 (A = Ti or V; M = W or Mo; X = S or Se). We find that Ti2WS4 and Ti2WSe4 exhibit large entropy changes of 5.97 and 5.51 μJ m–2 K–1, respectively, under a magnetic field near room temperature. Analysis based on perturbation theory indicates that strong second-nearest-neighbor exchange coupling plays an important role in MCE, along with a large MAE of ∼10 meV that is attributed to the coupling contributions of dx2y2 and dz2 orbitals of the W atom. Moreover, strain and carrier doping effectively modulate the MAE and Curie temperature, leading to remarkable enhancement of the MCE. This work provides important insights into the design of two-dimensional materials with enhanced MCE and is expected to facilitate further advancements in room-temperature magnetic refrigeration for practical applications.
研究了三元过渡金属硫族化合物A2MX4 (A = Ti或V; M = W或Mo; X = S或Se)的磁交换相互作用、磁各向异性(MAE)和磁热效应(MCE)。在接近室温的磁场作用下,Ti2WS4和Ti2WSe4的熵变较大,分别为5.97和5.51 μJ m-2 K-1。基于微扰理论的分析表明,强次近邻交换耦合在MCE中起着重要作用,并且W原子的dx2-y2和dz2轨道的耦合贡献使MAE达到了~ 10 meV。此外,应变掺杂和载流子掺杂有效地调节了MCE和居里温度,从而显著提高了MCE。这项工作为增强MCE的二维材料的设计提供了重要的见解,并有望促进室温磁制冷在实际应用中的进一步发展。
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引用次数: 0
A Multifunctional LiF as Passivated Material for an Efficient and Stable Perovskite Photodetector 作为高效稳定钙钛矿光电探测器钝化材料的多功能LiF
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acs.jpclett.5c03764
Lixiang Huang, Jia Yang, Yukun Wang, Guoxin Li, WeiFeng Wu, YeJun Xu
Metal cation and halide anion defects in perovskite films play a pivotal role in determining the performance and stability of perovskite photodetectors. In this study, LiF was utilized as a passivation material, both doped into the perovskite bulk phase and applied as a passivation layer on the top surface of the perovskite film. LiF forms hydrogen bonds and strong ionic interactions with perovskites, effectively passivating lattice and surface defects. Furthermore, as an insulator, LiF suppresses bimolecular and defect-assisted recombination, thereby enhancing carrier mobility and device stability. The optimized LiF-passivated MAPbI3–xBrx perovskite photodetector achieved an external quantum efficiency (EQE) of up to 87.5%, a maximum detectivity of 4.48 × 1013 Jones, and a theoretical linear dynamic range of 157.52 dB. Remarkably, the device retained 82% of its EQE after 2400 h of maximum power point tracking.
钙钛矿薄膜中的金属阳离子和卤化物阴离子缺陷是决定钙钛矿光电探测器性能和稳定性的关键因素。在本研究中,LiF作为钝化材料,既掺杂到钙钛矿体相中,又作为钝化层应用于钙钛矿膜的上表面。LiF与钙钛矿形成氢键和强离子相互作用,有效钝化晶格和表面缺陷。此外,作为绝缘体,liff抑制双分子和缺陷辅助重组,从而提高载流子迁移率和器件稳定性。优化后的lif钝化MAPbI3-xBrx钙钛矿光电探测器的外量子效率(EQE)高达87.5%,最大探测率为4.48 × 1013 Jones,理论线性动态范围为157.52 dB。值得注意的是,该设备在2400小时的最大功率点跟踪后保持了82%的EQE。
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引用次数: 0
Mn-Promoted CuZnAl Oxide for Enhanced Low-Temperature Reverse Water–Gas Shift Reaction 锰促进CuZnAl氧化物增强低温逆水气转换反应
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acs.jpclett.5c03875
Zengxi Feng, Wei Wang, Jiming Wang, Xiaoyu Liang, Yi Shi, Min Wang
The reverse water–gas shift (RWGS) reaction is crucial for CO2 utilization toward carbon neutrality. However, its efficiency under mild conditions is limited by low-temperature activity and rapid deactivation from metal sintering in conventional catalysts, including the cost-effective but thermally unstable Cu-based systems. In this work, the introduction of Mn into CuZnAl catalysts was demonstrated to significantly enhance their performance in the low-temperature RWGS reaction by promoting more oxygen vacancy formation. MnCuZnAl-Red catalysts achieve superior 26% CO2 conversion and 98% CO selectivity at 400 °C, with a CO formation rate of 422 mmol gcat–1 h–1. Characterization confirms that Mn enhances CO2 adsorption and activation by generating abundant oxygen vacancies. In-situ Fourier infrared (FT-IR) spectroscopy reveals a surface associative pathway. This work highlights Mn’s role in enhancing RWGS activity through tailored oxygen chemistry.
逆水气转换(RWGS)反应对二氧化碳利用实现碳中和至关重要。然而,它在温和条件下的效率受到低温活性和传统催化剂中金属烧结的快速失活的限制,包括成本效益高但热不稳定的cu基催化剂。本研究证明,在CuZnAl催化剂中加入Mn可以促进低温RWGS反应中形成更多的氧空位,从而显著提高CuZnAl催化剂的性能。在400℃条件下,MnCuZnAl-Red催化剂的CO转化率为26%,CO选择性为98%,CO生成速率为422 mmol gcat-1 h-1。表征证实Mn通过产生丰富的氧空位来增强CO2的吸附和活化。原位傅里叶红外光谱(FT-IR)揭示了表面结合途径。这项工作强调了Mn在通过定制氧化学增强RWGS活性中的作用。
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引用次数: 0
Enhancing Perovskite Solar Cell Performance via Engineering the Hole Transport Interface with Star-Shaped Nitrogen-Rich Material 星形富氮材料的空穴传输界面工程提高钙钛矿太阳能电池性能
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1021/acs.jpclett.5c03830
Wenbin Zhang, Ziyang Xia, Cheng Chen, Yaru Gao, Gang Fang, Bin Cai, Ming Cheng
Precise perovskite interface modification is regarded as a highly promising strategy to enhance the performance of efficient perovskite solar cells (PSCs). Herein, star-shaped small-molecule interface passivation material (IPM) TB-CZ (N,N′,N″-((benzene-1,3,5-triyltris(1H-benzo[d]imidazole-2,1-diyl))tris(benzene-4,1-diyl))tris(9-ethyl-N-(9-ethyl-9H-carbazol-3-yl)-9H-carbazol-3-amine)) was designed and synthesized to regulate the perovskite/spiro-OMeTAD interface. The core of TB-CZ is a nitrogen-rich benzimidazole compound in which the C–N and C═N groups can effectively passivate the Pb2+ defects in perovskites through multidentate coordination interactions. The side chain is equipped with a methoxy-free carbazole group, a design that significantly improves the material solubility and thus enhances the quality of perovskite films. The perovskite modified by TB-CZ can effectively optimize its energy levels, promoting hole extraction and transport. Consequently, the TB-CZ-modified PSCs achieve a power conversion efficiency (PCE) of 24.9% at an active area of 0.055 cm2 and maintain a commendable PCE of 22.0% even at an upscaled active area of 1 cm2, thereby showcasing its outstanding performance. Moreover, the modified device demonstrates remarkable long-term stability by retaining 81% of its initial PCE after storage for 1000 h under ambient conditions without any encapsulation. This work provides a strategy for the rational design of star-shaped passivation materials to enhance the PCE and stability of the PSCs.
钙钛矿界面的精确修饰被认为是提高高效钙钛矿太阳能电池(PSCs)性能的一种很有前途的策略。本文设计合成了星形小分子界面钝化材料(IPM) tbcz (N,N ',N″-(苯-1,3,5-三基三is(1h -苯并[d]咪唑-2,1-二基))三is(苯-4,1-二基))三is(9-乙基-N-(9-乙基- 9h -咔唑-3-基)- 9h -咔唑-3-胺)),用于调节钙钛矿/ spio - ometad界面。TB-CZ的核心是一种富氮苯并咪唑化合物,其中的C - N和C = N基团可以通过多齿配位相互作用有效地钝化钙钛矿中的Pb2+缺陷。侧链上配有无甲氧基咔唑基团,这一设计显著提高了材料的溶解度,从而提高了钙钛矿薄膜的质量。经TB-CZ改性的钙钛矿能有效优化其能级,促进空穴的提取和输运。因此,tb - cz -修饰的PSCs在0.055 cm2的有效面积下实现了24.9%的功率转换效率(PCE),即使在1 cm2的放大有效面积下也保持了22.0%的PCE,从而展示了其出色的性能。此外,改进后的器件在环境条件下储存1000小时后,在没有任何封装的情况下保持了81%的初始PCE,表现出了显著的长期稳定性。本研究为合理设计星形钝化材料以提高PCE和PSCs的稳定性提供了策略。
{"title":"Enhancing Perovskite Solar Cell Performance via Engineering the Hole Transport Interface with Star-Shaped Nitrogen-Rich Material","authors":"Wenbin Zhang, Ziyang Xia, Cheng Chen, Yaru Gao, Gang Fang, Bin Cai, Ming Cheng","doi":"10.1021/acs.jpclett.5c03830","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c03830","url":null,"abstract":"Precise perovskite interface modification is regarded as a highly promising strategy to enhance the performance of efficient perovskite solar cells (PSCs). Herein, star-shaped small-molecule interface passivation material (IPM) TB-CZ (<i>N</i>,<i>N</i>′,<i>N</i>″-((benzene-1,3,5-triyltris(1<i>H</i>-benzo[<i>d</i>]imidazole-2,1-diyl))tris(benzene-4,1-diyl))tris(9-ethyl-<i>N</i>-(9-ethyl-9<i>H</i>-carbazol-3-yl)-9<i>H</i>-carbazol-3-amine)) was designed and synthesized to regulate the perovskite/spiro-OMeTAD interface. The core of TB-CZ is a nitrogen-rich benzimidazole compound in which the C–N and C═N groups can effectively passivate the Pb<sup>2+</sup> defects in perovskites through multidentate coordination interactions. The side chain is equipped with a methoxy-free carbazole group, a design that significantly improves the material solubility and thus enhances the quality of perovskite films. The perovskite modified by TB-CZ can effectively optimize its energy levels, promoting hole extraction and transport. Consequently, the TB-CZ-modified PSCs achieve a power conversion efficiency (PCE) of 24.9% at an active area of 0.055 cm<sup>2</sup> and maintain a commendable PCE of 22.0% even at an upscaled active area of 1 cm<sup>2</sup>, thereby showcasing its outstanding performance. Moreover, the modified device demonstrates remarkable long-term stability by retaining 81% of its initial PCE after storage for 1000 h under ambient conditions without any encapsulation. This work provides a strategy for the rational design of star-shaped passivation materials to enhance the PCE and stability of the PSCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"58 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Photochromic, Thermosalient, Photophysical, and Electrochemical Properties of Pyridyl–Quinolinyl–Ethylene-Derived Multifunctional Organic Materials 吡啶-喹啉乙烯衍生多功能有机材料的光致变色、热显性、光物理和电化学性质
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.jpclett.5c03952
Tamil Selvan Kannan, Uma Kurakula, Raghavender Medishetty, Goutam Kumar Kole
This study offers a comprehensive structure–property correlation of a novel olefin E-1-(4′-pyridyl)-2-(4″-quinolinyl) ethylene (PQE) and its N-methylated derivative (MPQE) and demonstrates how crystal packing, hydration, and conjugation collectively dictate their solid-state photoreactivity and photochromic, thermosalient, photophysical, and electrochemical properties. PQE exhibited a quantitative [2 + 2] photocycloaddition reaction forming its head-to-tail dimer, which further exhibited a reversible cleavage of the cyclobutane ring. Crystals of PQE exhibited a color change under UV light, indicating photochromic behavior. Two different crystal forms, namely, MPQE and hydrated MPQE·2.25H2O, were obtained by tuning the crystallization medium. Despite having suitable stacking of MPQE cations, MPQE·2.25H2O remained photoinert; however, it exhibited a thermosalient behavior due to dehydration-induced lattice strain. MPQE displayed bathochromic spectral shifts in comparison to neutral PQE, indicating the effect of N-quaternization. The dimer, BPBQCB, displayed hypsochromic and hypochromic spectral shifts compared to PQE, for loss of conjugation. Their redox characteristics have been explored. Such observation of multifunctional behavior is rare and offers potentials for various applications.
本研究提供了一种新型烯烃E-1-(4 ' -吡啶基)-2-(4″-喹啉基)乙烯(PQE)及其n -甲基化衍生物(MPQE)的综合结构-性能相关性,并展示了晶体填充、水合作用和共轭作用如何共同决定了它们的固态光敏性和光致变色、热显性、光物理和电化学性能。PQE表现出定量的[2 + 2]光环加成反应,形成其头尾二聚体,并进一步表现出环丁烷环的可逆裂解。PQE晶体在紫外光照射下表现出颜色变化,显示出光致变色行为。通过调整结晶介质,得到了MPQE和水合MPQE·2.25H2O两种不同的结晶形态。MPQE·2.25H2O虽然有合适的MPQE阳离子堆叠,但仍保持光惰性;然而,由于脱水引起的晶格应变,它表现出热显性行为。与中性PQE相比,MPQE显示出显色光谱偏移,表明n -季铵化的影响。与PQE相比,二聚体BPBQCB由于偶联的损失,表现出了异色和异色的光谱偏移。探讨了它们的氧化还原特性。这种对多功能行为的观察是罕见的,并为各种应用提供了潜力。
{"title":"Photochromic, Thermosalient, Photophysical, and Electrochemical Properties of Pyridyl–Quinolinyl–Ethylene-Derived Multifunctional Organic Materials","authors":"Tamil Selvan Kannan, Uma Kurakula, Raghavender Medishetty, Goutam Kumar Kole","doi":"10.1021/acs.jpclett.5c03952","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c03952","url":null,"abstract":"This study offers a comprehensive structure–property correlation of a novel olefin <i>E</i>-1-(4′-pyridyl)-2-(4″-quinolinyl) ethylene (<b>PQE</b>) and its <i>N</i>-methylated derivative (<b>MPQE</b>) and demonstrates how crystal packing, hydration, and conjugation collectively dictate their solid-state photoreactivity and photochromic, thermosalient, photophysical, and electrochemical properties. <b>PQE</b> exhibited a quantitative [2 + 2] photocycloaddition reaction forming its <i>head-to-tail</i> dimer, which further exhibited a reversible cleavage of the cyclobutane ring. Crystals of <b>PQE</b> exhibited a color change under UV light, indicating photochromic behavior. Two different crystal forms, namely, <b>MPQE</b> and hydrated <b>MPQE·2.25H</b><sub><b>2</b></sub><b>O</b>, were obtained by tuning the crystallization medium. Despite having suitable stacking of <b>MPQE</b> cations, <b>MPQE·2.25H</b><sub><b>2</b></sub><b>O</b> remained photoinert; however, it exhibited a thermosalient behavior due to dehydration-induced lattice strain. <b>MPQE</b> displayed bathochromic spectral shifts in comparison to neutral <b>PQE</b>, indicating the effect of <i>N</i>-quaternization. The dimer, <b>BPBQCB</b>, displayed hypsochromic and hypochromic spectral shifts compared to <b>PQE</b>, for loss of conjugation. Their redox characteristics have been explored. Such observation of multifunctional behavior is rare and offers potentials for various applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"57 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122387","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Fate of the Triplet State of Tryptophan Isolated in the Gas Phase 色氨酸在气相分离时三重态的命运
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.jpclett.6c00010
Oleg V. Boyarkin, Andrei Zviagin, Ruslan Yamaletdinov
UV-induced phosphorescence from the lowest triplet state T1 of tryptophan (Trp) residues is widely used to monitor the structural dynamics of host proteins on long time scales. Probing the intrinsic properties of this optically “dark” state requires studies of Trp isolated in the gas phase, which are challenging due to low sample concentrations and the need to monitor the triplet over extended time scales. We discovered that excitation of cold, protonated noncovalent TrpH+–(H2O)n complexes (n ≥ 6) by UV light of specific wavelengths induces evaporation of two water molecules and promotes tryptophan to the triplet state. Subsequent photofragmentation dynamic, monitored by mass spectrometry and ion spectroscopy, yields rate constants for intrinsic triplet-state quenching via phosphorescence and reverse intersystem crossing. The T1 lifetime is approximately 1 s at 7 K and is dominated by phosphorescence; it decreases to tens of milliseconds at ∼40 K and is estimated to be ∼10 ms at room temperature.
色氨酸(Trp)残基最低三态T1的紫外诱导磷光被广泛用于长时间尺度上监测宿主蛋白的结构动态。探测这种光学“暗”态的固有特性需要对气相中分离的色氨酸进行研究,这是具有挑战性的,因为样品浓度低,并且需要在较长的时间尺度上监测三重态。我们发现,特定波长的紫外光激发冷、质子化的非共价TrpH+ - (H2O)n配合物(n≥6)可诱导两个水分子蒸发并促进色氨酸进入三重态。随后的光碎裂动力学,通过质谱和离子谱监测,通过磷光和反向系统间交叉得到了本征三态猝灭的速率常数。在7 K时,T1寿命约为1 s,以磷光为主;它在~ 40 K时减少到几十毫秒,在室温下估计为~ 10毫秒。
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引用次数: 0
Toward Chemical-Free Depolymerization of Lignin Surrogate: A Mechanistic Insight into Contact-Electro-Catalysis 木质素替代物的无化学解聚:接触电催化机理研究
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.jpclett.6c00192
Linyang Li, Junjun Wu, Ao Xia, Xun Zhu, Qiang Liao
Lignin, an abundant natural organic polymer and renewable resource, presents grand challenges in efficient depolymerization into value-added products. Herein, we propose an innovative green mechanochemical (contact-electro-catalysis; CEC) strategy to completely degrade the lignin model compounds (99.98% within 330 min) in a chemical-free, environmentally benign, and highly efficient manner. This is enabled by ultrasound-induced contact electrification to generate electrons and reactive oxygen species (ROS). Comprehensive mechanistic investigations reveal that ROS play a predominant role in lignin depolymerization. Furthermore, the possible thermal effect of CEC on the lignin depolymerization was also considered. Extensive characterization demonstrates the exceptional recyclability of the CEC reagent with a recovery rate of up to 92%. This approach not only exhibits outstanding performance in accelerating lignin depolymerization but also underscores the immense potential of mechanochemistry as a sustainable technology for biomass and lignin valorization.
木质素是一种丰富的天然有机高分子和可再生资源,其高效解聚制备高附加值产品面临着巨大的挑战。在此,我们提出了一种创新的绿色机械化学(接触电催化;CEC)策略,以无化学、环保和高效的方式完全降解木质素模型化合物(在330分钟内达到99.98%)。这是通过超声波诱导的接触电气化来产生电子和活性氧(ROS)。综合机理研究表明,活性氧在木质素解聚过程中起主导作用。此外,还考虑了CEC对木质素解聚可能产生的热效应。广泛的表征证明了CEC试剂的卓越可回收性,回收率高达92%。这种方法不仅在加速木质素解聚方面表现出色,而且强调了机械化学作为生物质和木质素增值的可持续技术的巨大潜力。
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引用次数: 0
Programming the Excited-State Landscape Via Carborane Count for Dual TADF/RTP 通过碳硼烷计数为双TADF/RTP编程激发态景观
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.jpclett.6c00063
Yangtao Shao, Xubin Wang, Hexi Wei, Xinli Li, Rongrong Huang, Shiwei Yin, Haonan Peng, Yu Fang
Concurrent thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) within one molecular family remain rare. Here we implement carborane-number engineering in o-carborane-functionalized triphenylamines (TPA-1Cb/2Cb/3Cb) to program the S1-Tn landscape (S1 = lowest singlet excited state; Tn = low-lying triplet states). Increasing the carborane count reshapes S1-Tn alignments and facilitates intersystem crossing and Tn-assisted reverse intersystem crossing, while aggregate confinement suppresses nonradiative decay, enabling dual-channel emission. Spectroscopy and transient absorption establish solution-phase TADF for TPA-2Cb/3Cb and solid-state, air-robust TADF/RTP coexistence under ambient atmosphere with ultralong TADF lifetimes of 67.4 ms (TPA-2Cb) and 105.3 ms (TPA-3Cb). TD-DFT based on crystal structures attributes channel allocation to carborane-count-dependent tuning of ΔE(S1-Tn) and finite spin–orbit coupling (SOC), whereas TPA-1Cb remains RTP-dominant due to large S1-T1/T2 separations. These results define a compact route to time-programmable, dual emission and offer a generalizable design principle for building concurrent TADF/RTP in carborane-based luminophores.
在一个分子家族中同时存在热激活延迟荧光(TADF)和室温磷光(RTP)仍然很少见。我们在邻碳硼烷功能化的三苯胺(TPA-1Cb/2Cb/3Cb)中实施碳硼烷数工程,对S1-Tn结构进行编程(S1 =最低单线激发态;Tn =低洼三重态)。增加碳硼烷数量重塑S1-Tn排列,促进系统间交叉和tn辅助的反向系统间交叉,而聚集体约束抑制非辐射衰变,实现双通道发射。光谱学和瞬态吸收法建立了TPA-2Cb/3Cb的固相TADF与RTP共存,TPA-2Cb和TPA-3Cb的TADF寿命分别为67.4 ms和105.3 ms。基于晶体结构的TD-DFT将通道分配归因于ΔE(S1-Tn)和有限自旋-轨道耦合(SOC)的碳硼烷计数依赖调谐,而TPA-1Cb由于较大的S1-T1/T2分离而仍然是rtp主导。这些结果定义了一种紧凑的时间可编程双发射路线,并为在碳硼烷基发光团中构建并发TADF/RTP提供了可推广的设计原则。
{"title":"Programming the Excited-State Landscape Via Carborane Count for Dual TADF/RTP","authors":"Yangtao Shao, Xubin Wang, Hexi Wei, Xinli Li, Rongrong Huang, Shiwei Yin, Haonan Peng, Yu Fang","doi":"10.1021/acs.jpclett.6c00063","DOIUrl":"https://doi.org/10.1021/acs.jpclett.6c00063","url":null,"abstract":"Concurrent thermally activated delayed fluorescence (TADF) and room-temperature phosphorescence (RTP) within one molecular family remain rare. Here we implement carborane-number engineering in <i>o</i>-carborane-functionalized triphenylamines (TPA-1Cb/2Cb/3Cb) to program the S<sub>1</sub>-T<sub>n</sub> landscape (S<sub>1</sub> = lowest singlet excited state; T<sub>n</sub> = low-lying triplet states). Increasing the carborane count reshapes S<sub>1</sub>-T<sub>n</sub> alignments and facilitates intersystem crossing and T<sub>n</sub>-assisted reverse intersystem crossing, while aggregate confinement suppresses nonradiative decay, enabling dual-channel emission. Spectroscopy and transient absorption establish solution-phase TADF for TPA-2Cb/3Cb and solid-state, air-robust TADF/RTP coexistence under ambient atmosphere with ultralong TADF lifetimes of 67.4 ms (TPA-2Cb) and 105.3 ms (TPA-3Cb). TD-DFT based on crystal structures attributes channel allocation to carborane-count-dependent tuning of Δ<i>E</i>(S<sub>1</sub>-T<sub>n</sub>) and finite spin–orbit coupling (SOC), whereas TPA-1Cb remains RTP-dominant due to large S<sub>1</sub>-T<sub>1</sub>/T<sub>2</sub> separations. These results define a compact route to time-programmable, dual emission and offer a generalizable design principle for building concurrent TADF/RTP in carborane-based luminophores.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"34 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122388","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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