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Energy transfer engineering for programmable fluorescence dynamics in CsPbBr3 perovskite: Toward multimode anti-counterfeiting CsPbBr3钙钛矿可编程荧光动力学的能量转移工程:面向多模防伪
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-06-01 Epub Date: 2026-02-06 DOI: 10.1016/j.jcis.2026.140063
Zhen Wu , Xin Zhang , Yiyuan Tang , Wenzhao Wang , Qiming Zou , Lvming Qiu , Jiani Liu , Bin Hu , Min Gong , Guojie Wang
Smart fluorescent materials with tunable fluorescence in response to external stimuli are of great interest for anti-counterfeiting applications. Herein, we develop a photoresponsive fluorescent material (PRFM) SPD-CsPbBr3@PMMA that integrates perovskite CsPbBr3 with photochromic spiropyran (SPD) in poly(methyl methacrylate) (PMMA), exhibiting multimode fluorescence outputs for advanced anti-counterfeiting applications. The blue-excitable CsPbBr3 nanocrystals enable SPD-CsPbBr3@PMMA a stable green fluorescence at 450 nm excitation wavelength. Ultraviolet light irradiation of SPD-CsPbBr3@PMMA induces the isomerization of SPD from closed-ring to open-ring form and subsequently gives a stable red fluorescence. Fluorescence decay spectra and theoretical calculations indicate that an efficient energy transfer occurs from CsPbBr3 to the open-ring SPD, thereby leading to significant changes in fluorescence. Upon irradiation with visible light (400–750 nm), SPD is reverted to closed-ring form, accompanied by the restoration of green fluorescence. SPD-CsPbBr3@PMMA can exhibit complex and tunable fluorescence changes under room light, blue light, and ultraviolet light modes, making it exceptionally suited for anti-counterfeiting applications. A novel strategy for information anti-counterfeiting by combining SPD-CsPbBr3@PMMA with Morse code and other innovative anti-counterfeiting platforms have been successfully developed. Overall, this study introduces an innovative approach to constructing multimode PRFMs, elucidates the design principles underlying fluorescence-tunable perovskite, and inspires further development in advanced anti-counterfeiting materials.
具有可调谐荧光响应外部刺激的智能荧光材料在防伪应用中具有很大的兴趣。在此,我们开发了一种光响应荧光材料(PRFM) SPD-CsPbBr3@PMMA,该材料将钙钛矿CsPbBr3与聚甲基丙烯酸甲酯(PMMA)中的光致变色螺吡喃(SPD)集成在一起,具有多模式荧光输出,可用于先进的防伪应用。蓝色可激发CsPbBr3纳米晶体使SPD-CsPbBr3@PMMA在450 nm激发波长下具有稳定的绿色荧光。紫外线照射SPD-CsPbBr3@PMMA诱导SPD由闭环异构化为开环,并产生稳定的红色荧光。荧光衰减光谱和理论计算表明,CsPbBr3向开环SPD发生了有效的能量转移,从而导致荧光发生显著变化。在可见光(400-750 nm)照射下,SPD恢复为闭环形式,同时恢复绿色荧光。SPD-CsPbBr3@PMMA可以在室内光,蓝光和紫外线模式下表现出复杂和可调的荧光变化,使其特别适合防伪应用。将SPD-CsPbBr3@PMMA与摩尔斯电码等新型防伪平台相结合,成功开发了一种新型的信息防伪策略。总的来说,本研究介绍了一种构建多模PRFMs的创新方法,阐明了荧光可调钙钛矿的设计原理,并激发了先进防伪材料的进一步发展。
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引用次数: 0
Electron transfer induced ruthenium-oxygen bond compression via d-band Center tailoring for efficient acidic overall water splitting 电子转移诱导钌-氧键压缩通过d波段中心剪裁为有效的酸性整体水分裂。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-02 DOI: 10.1016/j.jcis.2026.140035
Yiwei Jiang , Yu Qiu , Yuwei Zhang , Shuting Liu , Xueli Li , Yantu Zhang , Xiaoting Zhang
Ruthenium-based materials are recognized as theoretically ideal bifunctional catalysts for acidic overall water splitting. However, their practical implementation remains constrained by critical challenges, such as the dissolution and over-oxidation of active sites under operating conditions. In this study, through precise modulation of the electronic structure at the Ru-RuO2 heterojunction interface without incorporating any foreign metal elements, we successfully constructed a unique configuration characterized by compressed RuO bonds. Combined experimental characterization and theoretical calculations reveal that interfacial electron transfer induces the compression of RuO bond lengths, which subsequently leads to a downshift of the d-band center compared to pure RuO2. This electronic modulation effectively optimizes the adsorption behavior of both oxygen and hydrogen intermediates, thereby simultaneously lowering the energy barriers for the oxygen evolution reaction and the hydrogen evolution reaction. The synthesized Ru-RuO2@NC catalyst shows impressive bifunctional performance in an acidic electrolyte environment, reaching overpotentials as low as 161 mV for the oxygen evolution reaction and 53 mV for the hydrogen evolution reaction at a current density of 10 mA cm−2. Additionally, it demonstrates outstanding durability, sustaining stable performance for more than 420 h at 10 mA cm−2 during oxygen evolution reaction (OER) and 160 h even at a high current density of 500 mA cm−2 for the hydrogen evolution reaction (HER). This research offers fresh theoretical perspectives and a methodological framework aimed at realizing efficient and stable acidic overall water splitting by means of interface bond manipulation.
钌基材料被认为是理论上理想的酸性全水分解双功能催化剂。然而,它们的实际实施仍然受到关键挑战的限制,例如在操作条件下活性位点的溶解和过度氧化。在这项研究中,通过在不加入任何外来金属元素的情况下精确调制Ru-RuO2异质结界面上的电子结构,我们成功地构建了一个以压缩的RuO键为特征的独特构型。结合实验表征和理论计算表明,界面电子转移导致了RuO键长度的压缩,这随后导致了与纯RuO2相比d波段中心的下降。这种电子调制有效地优化了氧和氢中间体的吸附行为,从而同时降低了析氧反应和析氢反应的能垒。合成的Ru-RuO2@NC催化剂在酸性电解质环境下表现出令人满意的双功能性能,在电流密度为10 mA cm-2时,析氧反应的过电位低至161 mV,析氢反应的过电位低至53 mV。此外,它还表现出出色的耐久性,在10 mA cm-2的析氧反应(OER)中保持420小时以上的稳定性能,即使在500 mA cm-2的高电流密度下也能保持160小时以上的稳定性能。本研究提供了新的理论视角和方法框架,旨在通过界面键操纵实现高效稳定的酸性整体水裂解。
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引用次数: 0
A multifunctional biomass-derived three-dimensional solar evaporator constructed from wasted herbal medical slag for efficient steam generation and water purification 一种多功能生物质衍生的三维太阳能蒸发器,用于高效蒸汽产生和水净化
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-27 DOI: 10.1016/j.jcis.2026.139994
Siqi Wang , Jingjing Fu , Hongjun Chen , Haiyan Wang , Yuxin Yang , Xiaoran Huang , Xiu He , Jun Liu , Huang Zhou
Solar-driven desalination and wastewater purification represent sustainable approaches for clean freshwater production. However, process scalability is limited by insufficient sterilization, complicated fabrication procedures, and poor mechanical stability. In this study, a multi-functional hydrogel-supported solar (MHS) evaporator is proposed that incorporates carbonized Chinese herbal medicine residues in a sodium alginate (SA) gel matrix fabricated using a scalable and cost-effective procedure. The MHS evaporator achieved a water evaporation rate of 2.69 kg m−2 h−1 with an efficiency of 97.7% under one-sun irradiation, demonstrating superior sterilization performance and mechanical durability. Furthermore, the MHS delivers effective seawater desalination and wastewater purification, reducing ionic contaminants by three orders of magnitude while achieving greater than 99% removal of organic pollutants and heavy metals. The purified water exhibits enhanced purity, with greater than 99% elimination of pathogens (E. coli and S. aureus), ensuring viable control of biological contamination during the desalination process. In addition, the MHS evaporator maintained consistent and stable performance over a 30-day period. By incorporating superior sterilization, salt resistance, efficient photothermal conversion, and a high degree of mechanical strength in a scalable design, the MHS evaporator represents a highly promising solution to address freshwater scarcity in resource-limited environments.
太阳能驱动的海水淡化和废水净化是清洁淡水生产的可持续途径。然而,工艺的可扩展性受到灭菌不足、制造过程复杂和机械稳定性差的限制。在本研究中,提出了一种多功能水凝胶支撑的太阳能(MHS)蒸发器,该蒸发器将碳化的中草药残留物纳入海藻酸钠(SA)凝胶基质中,采用可扩展且具有成本效益的方法制备。MHS蒸发器在一次太阳照射下的蒸发率为2.69 kg m−2 h−1,蒸发率为97.7%,具有良好的杀菌性能和机械耐久性。此外,MHS提供有效的海水淡化和废水净化,将离子污染物减少三个数量级,同时实现99%以上的有机污染物和重金属的去除率。纯化后的水具有更高的纯度,病原体(大肠杆菌和金黄色葡萄球菌)的去除率超过99%,确保在脱盐过程中有效控制生物污染。此外,MHS蒸发器在30天的时间内保持一致和稳定的性能。MHS蒸发器具有卓越的杀菌、耐盐性、高效的光热转换和高度的机械强度,是解决资源有限环境中淡水短缺问题的一个非常有前途的解决方案。
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引用次数: 0
Molecular insights into sphingomyelin membrane alterations induced by very long-chain lysophospholipids 超长链溶血磷脂诱导鞘磷脂膜改变的分子研究。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-22 DOI: 10.1016/j.jcis.2026.139886
María Isabel Cabrera , Yolanda De Diego-Otero , Raquel Yahyaoui , Laura R. Arriaga , Juan L. Aragones , Pablo Llombart
Hypothesis Lipid membrane structure and mechanics are shaped by the molecular geometry and interactions of their amphiphiles. Very long-chain lysophosphatidylcholines (VLC-LysoPCs), with extended hydrophobic tails, insert into bilayers and perturb packing across leaflets. The VLC-LysoPCs 1-tetracosanoyl- (C24) and 1-hexacosanoyl- (C26) differ in chain length and insertion depth, and are thus expected to differentially modulate bilayer structure and mechanics. When co-incorporated, their distinct insertion depths and conformational behaviors may act cooperatively to reorganize lipid packing and modulate interleaflet coupling in ways unattainable by either species individually. Such synergy may underlie membrane remodeling during pathological VLC-lipid accumulation and offer design principles for synthetic membranes with tunable mechanics. Simulations Atomistic molecular dynamics simulations were performed on sphingomyelin bilayers containing either C24- or C26-LysoPCs, or both co-incorporated. Free energy calculations revealed the insertion mechanisms and thermodynamic profiles of each species. Structural remodeling, conformational dynamics, lipid diffusion, and interleaflet friction were evaluated through equilibrium and non-equilibrium simulations. Findings The insertion free energy of VLC-LysoPCs decreases when both C24 and C26 species are co-present in the sphingomyelin bilayer, indicating a thermodynamically cooperative effect that lowers the energetic cost of further incorporation. While C26 promotes extension of C24, C24 dampens the extension of C26, resulting in mutually modulated conformations that affect membrane packing and facilitate further incorporation. These changes reduced sphingomyelin mobility and decouple membrane leaflets. This is the first report to show that mixtures of VLC-LysoPCs with different chain lengths can cooperatively reshape membrane architecture and mechanics, offering design principles for tailored lipid-based membranes.
脂质膜的结构和力学是由两亲分子的分子几何形状和相互作用决定的。非常长链溶血磷脂酰胆碱(vllc - lysopcs),具有延伸的疏水尾部,插入双层并扰乱小叶间的包装。vllc - lysopcs - 1-四糖烷基- (C24)和1-六糖烷基- (C26)的链长和插入深度不同,因此有望不同地调节双层结构和力学。当它们结合在一起时,它们不同的插入深度和构象行为可能协同作用,重组脂质包装和调节叶间偶联,这是任何一个物种单独无法实现的。这种协同作用可能是病理性vlc -脂质积累过程中膜重塑的基础,并为具有可调力学的合成膜提供设计原则。对含有C24-或C26-LysoPCs,或两者均含有的鞘磷脂双层进行原子分子动力学模拟。自由能计算揭示了每个物种的插入机制和热力学分布。通过平衡和非平衡模拟对结构重塑、构象动力学、脂质扩散和叶间摩擦进行了评估。发现当C24和C26两种物质同时存在于鞘磷脂双分子层时,VLC-LysoPCs的插入自由能降低,表明存在一种热力学协同效应,降低了进一步结合的能量成本。C26促进C24的延伸,而C24抑制C26的延伸,导致相互调节的构象,影响膜的填充,促进进一步的掺入。这些变化降低了鞘磷脂的流动性并使膜小叶分离。这是第一份报告表明,具有不同链长度的vllc - lysopcs混合物可以协同重塑膜结构和力学,为定制脂基膜提供设计原则。
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引用次数: 0
Entropy-driven design of non-metallic heteroatoms codoped hollow carbon nanocages for superior oxygen electrocatalysis 非金属杂原子共掺杂中空碳纳米笼的熵驱动设计,用于优越的氧电催化。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-29 DOI: 10.1016/j.jcis.2026.139990
Xinshuang Lin , Hangyuan Xing , Jiabei Yu , Depeng Zhang , Xinyu Lu , Yuqing Zhang , Yimeng Sun , Sen Zhang , Chao Deng
The design of functional materials with increasing entropy has become a hot field in recent years. Motivated by the traditional concept of high entropy (HE), the anionic doping with multiple heteroelements towards increasing entropy has been considered to be a new clue to design highly efficient catalysts. In present work, we report the design of a non-metallic anion high-entropy (AHE) codoped hollow carbon nanocage as an oxygen catalyst for Zn-air batteries (ZAB). A series of non-metallic heteroatoms, including nitrogen (N), phosphorus (P), sulfur (S), boron (B), and fluorin (F), are employed as anionic dopants to construct the AHE codoped carbon nanocages. The influences of AHE engineering on the electrocatalytic behaviors of the hollow carbon nanocages in the oxygen reactions are explored. Through synergistic modulations on anionic doping engineering and structure design, the AHE doped hollow carbon nanocages achieve the superior oxygen reduction reaction (ORR) activities and faster kinetics in comparison to the counterparts of anionic medium-entropy (AME, e. g. N, P, S, B), anionic low-entropy (ALE, e. g. N, P, S, or N, P/S, or N) doped and undoped samples. Density functional theory (DFT) calculations reveal that the AHE engineering regulates the electronic structure, adjust the energy barrier, and modulate oxygen intermediates adsorption capability, which synergistically accelerate the ORR behaviors. In addition, the full ZAB battery integrated with the AHE codoped hollow carbon nanocages cathode delivers the high power density (212.1 W kg−1) and long cycle life (500 h cycling). More impressively, the solid-state ZAB with the hydrogel electrolyte and AHE doped carbon nanocage cathode shows the good flexibility and high adaptation in a wide temperature range. Therefore, this work not only introduces a synergistic modulation strategy to optimize the anion high-entropy catalysts for oxygen catalysis, but also promotes the fast development of high-performance ZAB towards different working conditions.
增熵功能材料的设计是近年来研究的热点。在传统的高熵(HE)概念的激励下,多异质元素阴离子掺杂的熵递增被认为是设计高效催化剂的新线索。在本工作中,我们报道了一种非金属阴离子高熵(AHE)共掺杂的空心碳纳米笼作为锌空气电池(ZAB)的氧催化剂的设计。采用氮(N)、磷(P)、硫(S)、硼(B)、氟(F)等一系列非金属杂原子作为阴离子掺杂剂,构建AHE共掺杂碳纳米笼。探讨了AHE工程对中空碳纳米笼在氧反应中电催化行为的影响。通过对阴离子掺杂工程和结构设计的协同调节,与阴离子中熵(AME,如N、P、S、B)、阴离子低熵(ALE,如N、P、S或N、P/S或N)掺杂和未掺杂的样品相比,AHE掺杂的空心碳纳米笼具有更好的氧还原反应(ORR)活性和更快的动力学。密度泛函理论(DFT)计算表明,AHE工程调节了电子结构,调节了能垒,调节了氧中间体的吸附能力,协同加速了ORR行为。此外,与AHE共掺杂空心碳纳米笼阴极集成的全ZAB电池具有高功率密度(212.1 W kg-1)和长循环寿命(500 h循环)。更令人印象深刻的是,水凝胶电解质和AHE掺杂碳纳米笼阴极的固态ZAB在宽温度范围内表现出良好的柔韧性和高度的适应性。因此,本工作不仅引入了一种协同调制策略来优化氧催化阴离子高熵催化剂,而且还促进了高性能ZAB向着不同工况的快速发展。
{"title":"Entropy-driven design of non-metallic heteroatoms codoped hollow carbon nanocages for superior oxygen electrocatalysis","authors":"Xinshuang Lin ,&nbsp;Hangyuan Xing ,&nbsp;Jiabei Yu ,&nbsp;Depeng Zhang ,&nbsp;Xinyu Lu ,&nbsp;Yuqing Zhang ,&nbsp;Yimeng Sun ,&nbsp;Sen Zhang ,&nbsp;Chao Deng","doi":"10.1016/j.jcis.2026.139990","DOIUrl":"10.1016/j.jcis.2026.139990","url":null,"abstract":"<div><div>The design of functional materials with increasing entropy has become a hot field in recent years. Motivated by the traditional concept of high entropy (HE), the anionic doping with multiple heteroelements towards increasing entropy has been considered to be a new clue to design highly efficient catalysts. In present work, we report the design of a non-metallic anion high-entropy (AHE) codoped hollow carbon nanocage as an oxygen catalyst for Zn-air batteries (ZAB). A series of non-metallic heteroatoms, including nitrogen (N), phosphorus (P), sulfur (S), boron (B), and fluorin (F), are employed as anionic dopants to construct the AHE codoped carbon nanocages. The influences of AHE engineering on the electrocatalytic behaviors of the hollow carbon nanocages in the oxygen reactions are explored. Through synergistic modulations on anionic doping engineering and structure design, the AHE doped hollow carbon nanocages achieve the superior oxygen reduction reaction (ORR) activities and faster kinetics in comparison to the counterparts of anionic medium-entropy (AME, e. g. N, P, S, B), anionic low-entropy (ALE, e. g. N, P, S, or N, P/S, or N) doped and undoped samples. Density functional theory (DFT) calculations reveal that the AHE engineering regulates the electronic structure, adjust the energy barrier, and modulate oxygen intermediates adsorption capability, which synergistically accelerate the ORR behaviors. In addition, the full ZAB battery integrated with the AHE codoped hollow carbon nanocages cathode delivers the high power density (212.1 W kg<sup>−1</sup>) and long cycle life (500 h cycling). More impressively, the solid-state ZAB with the hydrogel electrolyte and AHE doped carbon nanocage cathode shows the good flexibility and high adaptation in a wide temperature range. Therefore, this work not only introduces a synergistic modulation strategy to optimize the anion high-entropy catalysts for oxygen catalysis, but also promotes the fast development of high-performance ZAB towards different working conditions.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"710 ","pages":"Article 139990"},"PeriodicalIF":9.7,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111830","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
Encapsulation of FeCoNiCrMn high-entropy alloy in N-doped carbon fiber as a robust catalyst for boosting sulfur redox kinetics FeCoNiCrMn高熵合金在n掺杂碳纤维中的包封作为促进硫氧化还原动力学的稳健催化剂。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-28 DOI: 10.1016/j.jcis.2026.139999
YuFei Zhang, LiRong Zhang, FengFeng Han, Yang Zhao, HongXu Su, Lu Li, LiLi Wu, XiTian Zhang, Qi Jin
Lithium‑sulfur batteries (LSBs) suffer from lithium polysulfide (LiPS) shuttling and slow redox kinetics. To mitigate these issues, we report an efficient electrocatalytic interlayer based on a FeCoNiCrMn high-entropy alloy embedded in N-doped carbon nanofibers (HEA@NCNF). The multi-metallic HEA offers abundant active sites, while the N-doped carbon shell not only prevents HEA particle agglomeration and metal leaching, but also establishes a three-dimensional conductive network. Combined X-ray photoelectron spectroscopy and density functional theory calculations elucidate the underlying mechanism: electron modulation from the N-doped carbon layer raises the d-band center of the HEA, thereby strengthening LiPS adsorption and promoting its electrocatalytic conversion. Consequently, the HEA@NCNF interlayer functions as an efficient “trap-and-convert” reactor for LiPSs, which simultaneously suppresses shuttle effects and accelerates redox kinetics. The cells with HEA@NCNF demonstrate exceptional cycling and rate performance, with a capacity decay of only 0.023% per cycle over 1500 cycles at 1C. Remarkably, this superior performance extends to challenging conditions, including high sulfur loading (≥ 7 mg cm−2), lean electrolyte, and high-rate operation. This work demonstrates a strategy of integrating HEAs with conductive N-doped carbon matrices to create a synergistic trap-convert mediator for LiPSs.
锂硫电池(LSBs)受到锂多硫化物(LiPS)穿梭和缓慢氧化还原动力学的影响。为了缓解这些问题,我们报道了一种基于FeCoNiCrMn高熵合金嵌入n掺杂碳纳米纤维的高效电催化中间层(HEA@NCNF)。多金属HEA提供了丰富的活性位点,而n掺杂碳壳不仅可以防止HEA颗粒团聚和金属浸出,还可以建立三维导电网络。结合x射线光电子能谱和密度泛函理论计算阐明了其潜在的机制:来自n掺杂碳层的电子调制提高了HEA的d带中心,从而加强了LiPS的吸附并促进了其电催化转化。因此,HEA@NCNF中间层的功能是作为一个有效的“捕获和转化”反应器的LiPSs,它同时抑制穿梭效应和加速氧化还原动力学。含有HEA@NCNF的电池表现出优异的循环和速率性能,在1C下1500次循环中,每循环容量衰减仅为0.023%。值得注意的是,这种优越的性能可以扩展到具有挑战性的条件下,包括高硫负荷(≥7 mg cm-2)、低电解质和高速率运行。这项工作展示了将HEAs与导电n掺杂碳矩阵集成的策略,以创建LiPSs的协同陷阱转换介质。
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引用次数: 0
Photoluminescence of silicon nanorods via plasmonic gold nanopore arrays 等离子体金纳米孔阵列中硅纳米棒的光致发光。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-29 DOI: 10.1016/j.jcis.2026.140000
Yizhi Wu , Yankai Rong , Mingchao Ren , Xiaoliang Xu
Silicon luminescence remains a significant challenge, and its origin is intense debate ever since. Here we show, for the first time, a luminescent strategy involving silicon nanorods coupled with plasmonic gold nanopore arrays. It is demonstrated that the luminescence intensity of silicon nanorods induced by plasmonic gold nanopore arrays is nine times higher than that of pure silicon nanorod samples. Despite the absence of an insulating spacer between the gold nanopore arrays and silicon nanorods, no luminescence quenching is observed. Furthermore, we employ finite difference time domain simulations to map the electric field distribution and estimate a Purcell factor of 5, which is lower than the experimentally measured luminescence enhancement. This indicates that the observed luminescence enhancement is only partially attributable to the Purcell effect. Importantly, the Purcell effect would not cause a shift in the luminescence peak, whereas a significant peak shift is observed in our experiments. Based on these facts, a novel luminescence mechanism is proposed to complementally account for the remarkable luminescence enhancement observed in our experiments. Plasmonic gold nanopore arrays-induced energy level splitting may appear in silicon nanorods, which generates a localized direct bandgap, thereby yielding enhanced visible light emission.
硅发光仍然是一个重大的挑战,它的起源一直是激烈的争论。在这里,我们首次展示了一种涉及硅纳米棒与等离子体金纳米孔阵列耦合的发光策略。结果表明,等离子体金纳米孔阵列诱导的硅纳米棒的发光强度是纯硅纳米棒的9倍。尽管在金纳米孔阵列和硅纳米棒之间没有绝缘间隔,但没有观察到发光猝灭。此外,我们使用时域有限差分模拟来绘制电场分布,并估计Purcell因子为5,低于实验测量的发光增强。这表明所观察到的发光增强仅部分归因于珀塞尔效应。重要的是,Purcell效应不会引起发光峰的移位,而在我们的实验中观察到明显的峰值移位。基于这些事实,我们提出了一种新的发光机制来补充解释我们在实验中观察到的显着的发光增强。等离子体金纳米孔阵列诱导的能级分裂可能出现在硅纳米棒中,产生局域直接带隙,从而增强可见光发射。
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引用次数: 0
Combination of electronic structure regulation and controllable phase transition engineering for urea-assisted energy-saving hydrogen production 电子结构调控与可控相变工程相结合的尿素辅助节能制氢。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-01-30 DOI: 10.1016/j.jcis.2026.140018
Tongxue Zhang , Mengmeng Jin , Jingming Bao , Mingwei Yang , Shuai Liu , Wenting Cai , Ke Fan , Kaiwei Wang , Bingxin Zhu , Xubin Zhang , Fumin Wang
Utilizing the thermodynamically favorable urea oxidation reaction (UOR) as a substitute for the oxygen evolution reaction (OER) in conventional water electrolysis offers a viable method for wastewater treatment and energy-efficient hydrogen generation. A series of samples with abundant cation vacancies were synthesized via a hydrothermal method followed by alkaline etching. The electronic and crystal structures of the catalysts were simultaneously modulated by precisely tuning the concentration of the vacancy-inducing medium. The β-type NiCov 1:1–2% with abundant cation vacancies demonstrates superior UOR activity, with just 1.31 and 1.35 V vs. RHE needed to reach current densities of 10 and 100 mA cm−2, respectively. Characterization experiments indicate that the optimization of electronic structure through cation vacancies and distinctive multilayered flake morphology can enhance the number of active sites and improve mass transfer efficiency. A series of in situ measurements further corroborate the rapid yet moderate phase transitions of NiCov 1:1–2%. Theoretical calculations demonstrate that the introduction of cation vacancies optimizes the balance between reactant adsorption and product desorption, leading to a reduced Gibbs free energy barrier for the rate-determining step of UOR. This study offers valuable guidance for the rational design of efficient and versatile catalysts for small-molecule oxidation reactions.
利用热力学有利的尿素氧化反应(UOR)代替传统的电解析氧反应(OER)为废水处理和节能制氢提供了一种可行的方法。采用水热法和碱性蚀刻法制备了一系列具有丰富阳离子空位的样品。通过精确调节空诱导介质的浓度,可以同时调节催化剂的电子结构和晶体结构。β型NiCov为1:1-2%,具有丰富的阳离子空位,具有优越的UOR活性,相对于RHE只需1.31和1.35 V,电流密度分别达到10和100 mA cm-2。表征实验表明,通过阳离子空位和独特的多层片状形貌来优化电子结构可以增加活性位点的数量,提高传质效率。一系列的原位测量进一步证实了NiCov 1:1-2%的快速而温和的相变。理论计算表明,阳离子空位的引入优化了反应物吸附和产物解吸之间的平衡,导致UOR速率决定步骤的吉布斯自由能垒降低。该研究为合理设计高效、通用的小分子氧化反应催化剂提供了有价值的指导。
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引用次数: 0
Hard carbon with tailored microstructure via thermal regulation for high-efficiency sodium-ion batteries 通过热调节为高效钠离子电池量身定制微观结构的硬碳。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-01 DOI: 10.1016/j.jcis.2026.140026
Pengcheng Mao , Jie Di , Yuqi Liu , Jingjing Chen , Xiang Li , Jie Liu , Wenbin Hu , Cheng Zhong
Hard carbon (HC) is the most promising commercially available anode material for sodium-ion batteries (SIBs) due to the high specific capacity, low operation voltage and low cost. However, HC faces the problems of poor initial Coulombic efficiency (ICE) and ambiguous sodium storage mechanism. Furthermore, the relationship between solid electrolyte interphase (SEI) characteristics, particularly its chemical composition and microstructural features, and electrochemical performance remains poorly understood. To this end, HC with abundant closed pores and adjustable defect concentration was prepared in this study using cheap pine bark as raw material through precise thermal regulation. At high pyrolysis temperature, the carbon layer in HC fully grows and promotes the growth of closed pore. The optimized PHC-1300 exhibits a high ICE of 89.6% and an outstanding specific capacity of 347.62 mAh g−1 at 0.1C. Moreover, the PHC-1300//Na3V2 (PO4)3 full-cells also exhibit excellent cycling performance. Based on the electrochemical performance and microstructure of the pine bark-based HC, it is proposed that the sodium storage mechanism is “adsorption-intercalation-filling”. Notably, it is found that the HC surface with suitable defect concentration can induce the formation of fluorine-rich organic SEI phase, which is beneficial to maintain the interfacial stable to improve the cycling stability.
硬碳(HC)具有高比容量、低工作电压和低成本等优点,是钠离子电池(sib)阳极材料中最有前途的一种。然而,HC面临着初始库仑效率(ICE)较差和钠储存机制不明确的问题。此外,固体电解质间相(SEI)特性,特别是其化学成分和微观结构特征,与电化学性能之间的关系仍然知之甚少。为此,本研究以廉价的松皮为原料,通过精确的热调节,制备出了闭孔丰富、缺陷浓度可调的HC。在高热解温度下,HC中的碳层充分生长,促进了闭孔的生长。优化后的PHC-1300在0.1C时具有高达89.6%的ICE和347.62 mAh g-1的优异比容量。此外,PHC-1300//Na3V2 (PO4)3全电池也表现出优异的循环性能。基于松皮基HC的电化学性能和微观结构,提出其钠的储存机制为“吸附-插层-填充”。值得注意的是,发现缺陷浓度合适的HC表面可以诱导富氟有机SEI相的形成,有利于保持界面稳定,提高循环稳定性。
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引用次数: 0
Tailorable MoS2 quantum dots nanofluids via coordination-confined growth for high-performance lubrication 通过配位限制生长的MoS2量子点纳米流体用于高性能润滑。
IF 9.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-05-15 Epub Date: 2026-02-03 DOI: 10.1016/j.jcis.2026.140049
Ru Yan, Hongyang Wang, Rui Dong, Ping Wen, Mingjin Fan
Conventional solvent-free nanofluids hold promise as lubricants but often face challenges in intricate preparation and unadjustable performance. Herein, we developed a facile one-pot strategy for synthesizing MoS2 quantum dots (QDs) nanofluids (MoNFs) via a coordination-confined growth approach, which features cyan-fluorescent with an average size of 3.8 nm, homogeneously dispersed in a tailored ionic liquid matrix. The resulting MoNFs exhibit tunable viscosity and desirable shear-thinning behavior. When evaluated as lubricants, the optimal formulation (3MoNFs) decreases wear volume by 73.8% compared to the base fluid. Comprehensive characterization of worn track reveals a triplex synergistic lubrication integrating an electric-double-layer film, tribochemical reaction film and solid-like nanofluid layer, concurrently assisted with repairing pre-existing wear scars. Impressively, blending merely 0.7 wt% 3MoNFs into commercial SN 0 W-30 engine oil enhances its anti-wear performance by 47.5%, demonstrating outstanding potential for high-performance lubricants.
传统的无溶剂纳米流体有望成为润滑剂,但在复杂的制备和不可调节的性能方面往往面临挑战。在此,我们开发了一种简单的一锅策略,通过配位限制生长方法合成MoS2量子点(QDs)纳米流体(MoNFs),其特征是蓝绿色荧光,平均尺寸为3.8 nm,均匀分散在定制的离子液体基质中。所得到的MoNFs具有可调的粘度和理想的剪切减薄性能。当作为润滑剂进行评估时,与基础液相比,最佳配方(3MoNFs)减少了73.8%的磨损量。磨损轨迹的综合表征揭示了一种三重协同润滑,包括电双层膜、摩擦化学反应膜和固体状纳米流体层,同时有助于修复已有的磨损疤痕。令人印象深刻的是,仅将0.7 wt%的3MoNFs掺入商用SN 0 W-30发动机油中,其抗磨性能就提高了47.5%,显示出高性能润滑油的巨大潜力。
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引用次数: 0
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Journal of Colloid and Interface Science
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