Journal of Colloid and Interface Science最新文献_第3页

Unraveling the spontaneous advancement of precursor films from a liquid reservoir to an isolated wall 揭示前驱体膜从液体储层到隔离壁的自发推进

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-01-29 DOI: 10.1016/j.jcis.2026.140007

Yung-Ching Wang , Yi-Min Chen , Heng-Kwong Tsao , Yu-Jane Sheng

Hypothesis

Although the spreading of precursor films associated with total wetting liquids can be observed in droplet wetting or capillary flow, concurrent variations in evolving meniscus shape and transient Laplace pressure complicate the direct observation of the precursor film dynamics. To overcome this challenge, the present study employs a configuration that allows the liquid source to stabilize at the entrance, enabling the advancement of the precursor film to be exclusively monitored and analyzed under a constant driving force.

Methods

The spontaneous advancement of precursor films, leaking from a reservoir to an isolated wall, is investigated using many-body dissipative particle dynamics simulations. The influences of surface wettability and the entrance width on the precursor film dynamics are systematically quantified.

Findings

The advancing precursor film exhibits diffusion-like behavior, where the propagation length scales with t^1/2. The spreading rate is governed by the interplay between the driving forces, characterized by the spreading coefficient (S) and entrance width (N), and the resistive wall friction. Specifically, the spreading rate increases with S at low wettability but eventually saturates. This saturation suggests that the increase in driving forces is effectively offset by the rising wall friction. Furthermore, widening the entrance facilitates faster spreading by reducing the Laplace pressure.

假设：虽然在液滴润湿或毛细管流动中可以观察到与总润湿液体相关的前驱膜的扩散，但在演变的半月板形状和瞬态拉普拉斯压力的同时变化使前驱膜动力学的直接观察复杂化。为了克服这一挑战，本研究采用了一种允许液源在入口稳定的配置，使前驱体膜的推进能够在恒定的驱动力下进行专门的监测和分析。方法采用多体耗散粒子动力学模拟方法，研究了前驱体膜从储层泄漏到隔离壁的自发推进过程。系统地量化了表面润湿性和入口宽度对前驱体膜动力学的影响。发现前驱体膜呈扩散状，其传播长度与t1/2成正比。扩散速率由扩散系数S和入口宽度N与阻力壁面摩擦力的相互作用决定。具体来说，在低润湿性下，扩散速率随S的增加而增加，但最终趋于饱和。这种饱和表明，驱动力的增加被壁面摩擦力的增加有效地抵消了。此外，扩大入口通过降低拉氏压力来促进更快的扩散。

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引用次数: 0

A photothermal antibacterial hydrogel based on a “nano-bridge” strategy with high toughness and self-healing capacity 基于“纳米桥”策略的具有高韧性和自愈能力的光热抗菌水凝胶。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-01-29 DOI: 10.1016/j.jcis.2026.139995

Junyan Wang , Jianhui Wang , Laixiang Zhu , Na Zhang , Nannan Xu , Fuhao Liu , Yanqing Wang , Chuanhui Gao

Constructing integrated multifunctional hydrogels with both high toughness and diverse functionalities is beneficial for the development of flexible antibacterial materials and wearable sensors. However, current hydrogels often fail to achieve a synergistic balance among toughness, antibacterial activity, and sensing responsiveness, limiting their practical applications. Herein, a “nano-bridge” strategy is proposed to fabricate a double-network hydrogel system (PHS-CT) composed of a covalent polyacrylamide network and a dynamic borate-crosslinked hydroxypropyl guar gum/sodium alginate network. The incorporated Cu-TA nanosheets serve not only as “structural bridges” to enhance the crosslinking density and mechanical performance (strain up to 1997.7%, toughness up to 1.53 MJ/m³), but also as “functional bridges” to enable photothermal conversion and improved antibacterial activity (bacterial killing rate of 99.0% against E. coli under NIR irradiation). In addition, benefiting from the dynamic reversibility of borate ester bonds as well as the re-forming capability of hydrogen bonds at the fracture interface, the hydrogel exhibits favorable self-healing ability (self-healing efficiency up to 91.0%), and can function as a flexible strain sensor capable of accurately detecting both large-scale and subtle deformations. This strategy provides a feasible strategy for constructing multifunctional dual-network hydrogels, and may be useful for photothermal antibacterial and flexible sensing applications.

构建具有高韧性和多种功能的一体化多功能水凝胶有利于柔性抗菌材料和可穿戴传感器的发展。然而，目前的水凝胶往往无法在韧性、抗菌活性和传感响应性之间实现协同平衡，限制了它们的实际应用。本文提出了一种“纳米桥”策略来制备由共价聚丙烯酰胺网络和硼酸交联羟丙基瓜尔胶/海藻酸钠动态网络组成的双网络水凝胶体系（PHS-CT）。加入的Cu-TA纳米片不仅作为“结构桥”提高交联密度和力学性能（应变高达1997.7%，韧性高达1.53 MJ/m3），而且作为“功能桥”实现光热转化和提高抗菌活性（近红外照射下对大肠杆菌的细菌杀灭率为99.0%）。此外，得益于硼酸酯键的动态可逆性和破裂界面氢键的再形成能力，水凝胶具有良好的自修复能力（自修复效率高达91.0%），可以作为柔性应变传感器，准确检测大规模和微小变形。该策略为构建多功能双网络水凝胶提供了一种可行的策略，并可用于光热抗菌和柔性传感应用。

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引用次数: 0

Dual kinetics-enhanced crystalline BiOF hollow nanorods toward high-capacity and high-rate aqueous alkaline batteries 用于大容量、高倍率碱性水电池的双动力学增强晶体生物of空心纳米棒。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-02-01 DOI: 10.1016/j.jcis.2026.140028

Yuntian Lan , Qiaoling Bi , Zhen Zhang , Yuzhan Liu , Fengming Zhou , Qi Zhang , Zexing Wu , Jiarun Li , Zhenyu Xiao

Lack of double-high (high energy density and power density) anode materials is the key bottleneck for the application of Aqueous alkaline batteries (AABs). Although the emergence of Bismuth-based materials provides an opportunity to solve this issue, due to their high theoretical capacity via a three-electron redox reaction and suitable operating potential, their restricted ion diffusion kinetics via closed-packed atomic arrangement limit their application performance. Herein, the bismuth oxyfluoride hollow nanorods (BiOF-HNs) with intrinsic layer atom configuration have been constructed by the crystallization optimization and morphology engineering synergistic strategy during MOF etching process. Bi³⁺ hydrolysis is the key points to achieve the co-precipitating and repining reactions of BiOF at the surface of Bi MOF for hollow nanorods morphology. The BiOF-HNs deliver dramatically increased electron conductivity and ion transport ratio with the work function of 6.42 eV and OH⁻ diffusion value of 2.11 × 10⁻¹³ cm² s⁻¹. Therefore, the optimized BiOF-HNs electrode delivers a remarkable specific capacity of 342.2 mAh g⁻¹ (1232 F g⁻¹) at 1 A g⁻¹ and maintains 86% capacity retention at 20 A g⁻¹. Furthermore, the assembled BCNP (basic cobalt/nickel phosphate)//BiOF-HNs AABs achieve a high energy density of 157.81 Wh kg⁻¹ at 1.28 kW kg⁻¹ and outstanding cycling stability (81% after 9000 cycles). The exploration of BiOF materials with morphology and crystalline optimization in AABs application, may offer new insights of design high performance aqueous anode materials.

双高（高能量密度和功率密度）负极材料的缺乏是制约水碱性电池应用的关键瓶颈。尽管铋基材料的出现为解决这一问题提供了机会，但由于其通过三电子氧化还原反应的高理论容量和合适的操作电位，其封闭排列的离子扩散动力学限制了其应用性能。在MOF蚀刻过程中，采用结晶优化和形貌工程协同策略，构建了具有本构层原子构型的氟化氧化铋空心纳米棒。Bi3+的水解是实现BiOF在bimof表面共沉淀、共精炼反应的关键。BiOF-HNs的电子电导率和离子输运率显著提高，功函数为6.42 eV， OH-扩散值为2.11 × 10-13 cm2 s-1。因此，优化后的BiOF-HNs电极在1 a g-1下可提供342.2 mAh g-1 （1232 F g-1）的显着比容量，在20 a g-1下可保持86%的容量。此外，组装的BCNP（碱性钴/磷酸镍）//BiOF-HNs AABs在1.28 kW kg-1下可达到157.81 Wh kg-1的高能量密度，并且具有出色的循环稳定性（循环9000次后81%）。探索生物of材料的形态和晶体优化在AABs中的应用，可能为设计高性能水性阳极材料提供新的思路。

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引用次数: 0

Coupling urea production and energy output in Zn-nitrate/carbon dioxide batteries enabled by porous copper‑nickel bimetallic catalysts 多孔铜镍双金属催化剂在硝酸锌/二氧化碳电池中耦合尿素生产和能量输出。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-01-27 DOI: 10.1016/j.jcis.2026.139991

Guoning Chen , Jianbing Chen , Sanshuang Gao , Jun Li , Bohao Chang , Xuguang An , Linfeng Xiao , Hao Cheng , Guangzhi Hu , Yujie Ma

Conventional urea industry faces dual challenges of high energy consumption and carbon emissions. Although electrochemical co-reduction of nitrates and carbon dioxide (CO₂) offers a promising route for green urea synthesis, its electrical-to-chemical energy conversion efficiency remains constrained by sluggish reaction kinetics and high electrical energy demand. Here, we design and report a nitrogen-doped porous carbon (NC) material embedded with dispersed copper‑nickel bimetal nanoparticles (CuNi/NC) for constructing the first example of a Zn-nitrate/CO₂ battery that can output electricity while generating urea with a superior energy efficiency of 1.51 mol_urea kWh⁻¹ and a urea production rate of 110 mg h⁻¹ g_cat⁻¹. The proposed assembled battery exhibits exceptional stability over 300 h, retaining high urea Faradaic efficiency at 36% and yield at 100.9 mg h⁻¹ g_cat⁻¹. In situ X-ray absorption spectroscopy, infrared spectroscopy, and density functional theory simulations confirm that the active metal sites facilitate substrate adsorption and stabilize critical intermediates (*N-C-N, *NH₂, and *NO), thereby effectively accelerating CN coupling. This work breaks the ‘high-energy, single-function’ bottleneck of traditional electrochemical systems, establishing an innovative ‘carbon-negative energy supply’ paradigm for carbon-neutral agriculture and decentralized energy systems.

传统尿素工业面临着高能耗和高碳排放的双重挑战。虽然硝酸盐和二氧化碳（CO 2）的电化学共还原为绿色尿素合成提供了一条有前途的途径，但其电化能转换效率仍然受到反应动力学缓慢和电能需求高的限制。在这里，我们设计并报道了一种嵌入分散铜镍双金属纳米颗粒（CuNi/NC）的氮掺杂多孔碳（NC）材料，用于构建硝酸锌/二氧化碳电池的第一个例子，该电池可以在输出电力的同时产生尿素，其能源效率为1.51摩尔尿素kWh-1，尿素产率为110 mg h-1 gcat-1。所提出的组装电池在300小时内表现出优异的稳定性，保持了36%的尿素法拉第效率和100.9 mg h-1 gcat-1的产率。原位x射线吸收光谱、红外光谱和密度泛函理论模拟证实，活性金属位点有利于底物吸附，稳定关键中间体（*N-C-N、* nh2和*NO），从而有效加速CN耦合。这项工作打破了传统电化学系统“高能量、单一功能”的瓶颈，为碳中和农业和分散能源系统建立了一种创新的“碳负能源供应”范式。

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引用次数: 0

Tailoring anion-enriched and fluoroethylene carbonate coordinated weak solvation structure for interfacial-stable lithium metal batteries 界面稳定锂金属电池的富阴离子和氟碳酸乙烯配位弱溶剂化结构。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-02-04 DOI: 10.1016/j.jcis.2026.140027

Maolin Zhang , Rui Hao , Xiaoping Yang , Fan Yang , Zhaoxia Xu , Shixi Liu , Shouyi Yuan , Yubo Xing , Hao Wu , Yannan Zhang , Yiyong Zhang , Wen Lu , Peng Dong , Yingjie Zhang , Fang Cheng

The development of practical lithium (Li) metal battery (LMB) is severely restricted by the poor stability of electrode-electrolyte interfaces (EEIs) and sluggish interfacial kinetics. Modulating Li-ion solvation structure is critical for addressing this issue, but remains challenging. Herein, we propose a novel strategy of incorporating multiple anions and functional solvent to tailor a unique anion-enriched and fluoroethylene carbonate (FEC) coordinated weak solvation structure for interfacial-stable high-performance LMBs. Theoretical calculations and experimental results indicate that the first Li-ion solvation sheath is dominated by multiple anions and FEC molecules, leading to a largely diminished coordination of Li⁺-solvents and an accelerated interfacial dynamics. Simultaneously, inorganic-rich robust EEIs are further constructed via the preferential redox decomposition of the solvated anions and FEC molecules, achieving a remarkable interfacial stability and dendrite-free Li plating/stripping behavior. Consequently, the symmetric Li||Li cells realize an ultra-long stable cycle of 5400 h at 2 mAh cm⁻², and the Li||LiFePO₄ (LFP) full cells demonstrate an excellent rate and cycling performance even under high LFP-loading, relatively low negative/positive capacity ratio (N/P) and less electrolyte usage. Our findings reveal a facile proposal to precisely tailor weak Li-ion solvation structure by integrating anion chemistry and functional solvent, paving the way for advanced electrolyte design and high-performance LMBs development.

电极-电解质界面稳定性差和界面动力学缓慢严重制约了实用锂金属电池的发展。调节锂离子溶剂化结构是解决这一问题的关键，但仍然具有挑战性。在此，我们提出了一种将多个阴离子和功能溶剂结合的新策略，以定制一种独特的阴离子富集和氟乙烯碳酸酯（FEC）协调的弱溶剂化结构，用于界面稳定的高性能lmb。理论计算和实验结果表明，第一个Li离子溶剂化鞘层由多个阴离子和FEC分子主导，导致Li+溶剂的配位大大降低，界面动力学加速。同时，通过溶剂化阴离子和FEC分子的优先氧化还原分解，进一步构建了富无机坚固的eei，实现了显著的界面稳定性和无枝晶的镀/剥离行为。因此，对称的Li||锂电池在2 mAh cm-2下实现了5400 h的超长稳定循环，并且Li||LiFePO4 （LFP）满电池即使在高LFP负载，相对较低的负/正容量比（N/P）和较少的电解质使用下也表现出优异的倍率和循环性能。我们的研究结果揭示了通过整合阴离子化学和功能溶剂来精确定制弱锂离子溶剂化结构的简单建议，为先进的电解质设计和高性能lmb的开发铺平了道路。

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引用次数: 0

PtRu nanoparticle catalysts with adjustable electronic environments for efficient low-temperature dehydrogenation of cycloalkanes 具有可调电子环境的PtRu纳米颗粒催化剂用于环烷烃的高效低温脱氢

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-01-29 DOI: 10.1016/j.jcis.2026.140011

Xiaoqi Zhang , Aijun Guo , Shouhui Jiao , Xiaoxue Wang , Jiang Wu , Ankang Jia , Zheng Zhang , He Liu , Yueliang Liu , Zongxian Wang

Modulating the electronic structure of active catalytic species to optimise the adsorption and activation steps of reactants is crucial for achieving efficient and stable dehydrogenation of liquid organic hydrogen carriers. In this study, a uniformly dispersed PtRu nanoalloy catalyst (PtRu/Al₂O₃) was successfully prepared on Al₂O₃ sheets through a process strategy combining wet chemical impregnation, low-temperature pre-reduction, and high-temperature annealing. The degree of Pt electron enrichment induced by Ru modification can be precisely controlled by adjusting Pt/Ru ratio, and this enrichment level is positively correlated with Ru coverage. The PtRu alloy with moderate electronic enrichment significantly lowers both the adsorption energy and the CH bond activation energy at key active sites. This facilitated the rapid desorption and transfer of the products, ultimately determining the overall dehydrogenation efficiency. Catalytic tests show that the Pt₂Ru₁/Al₂O₃ catalyst achieves a single-ring cycloalkane dehydrogenation conversion rate of over 99% at 200 °C. Even for decalin, the conversion rate reaches 69% at 230 °C. Furthermore, its apparent activation energy (68.4 kJ/mol) was lower than that of conventional Pt/Al₂O₃, demonstrating the kinetic advantages attributed to the electronic effects in Pt₂Ru₁/Al₂O_3. Both experimental results and theoretical analyses confirm that intermetallic electronic interactions contribute to the enhanced hydrogen production rates, and further elucidate the charge transfer mechanism within the PtRu alloy.

调节活性催化物质的电子结构以优化反应物的吸附和活化步骤是实现液态有机氢载体高效、稳定脱氢的关键。本研究通过湿化学浸渍、低温预还原和高温退火相结合的工艺策略，成功地在Al2O3薄片上制备了均匀分散的PtRu纳米合金催化剂（PtRu/Al2O3）。通过调整Pt/Ru比，可以精确控制Ru修饰后Pt电子的富集程度，富集程度与Ru覆盖率呈正相关。中等电子富集的PtRu合金显著降低了吸附能和关键活性位点的CH键活化能。这促进了产物的快速脱附和转移，最终决定了总体脱氢效率。催化实验表明，在200℃下，Pt2Ru1/Al2O3催化剂的单环烷烃脱氢转化率达到99%以上。即使对于十氢化萘，在230℃时转化率也达到69%。此外，其表观活化能（68.4 kJ/mol）低于常规Pt/Al2O3，表明Pt2Ru1/Al2O3中的电子效应具有动力学优势。实验结果和理论分析均证实了金属间电子相互作用有助于提高PtRu合金的产氢速率，并进一步阐明了PtRu合金内部的电荷转移机制。

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引用次数: 0

Laser mineralization of per- and polyfluoroalkyl substances on laser-induced graphene 单氟烷基和多氟烷基物质在激光诱导石墨烯上的激光矿化。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-02-03 DOI: 10.1016/j.jcis.2026.140040

Negasi K. Weldengus , Maurício N. Kleinberg , Christopher J. Arnusch

Per- and polyfluoroalkyl substances (PFAS) are persistent and toxic water pollutants that pose significant environmental and health risks. Various methods exist for PFAS treatment, most of which rely on adsorption. However, these methods often produce byproducts that require additional treatment before disposal. Here we show a facile method for degrading model pollutants perfluorooctanoic acid (PFOA) and trifluoroacetic acid (TFA) using a low energy IR CO₂ laser on a laser-induced graphene (LIG) substrate, with NaOH serving as a mineralizing reagent. Laser treatment achieved up to 68% mineralization and the conversion of strong CF bonds present in PFOA into inorganic fluoride (NaF) was observed depending on the laser power, with optimum performance at 8% power. The fluorine mineralization efficiency increased with a larger Na-to-F molar ratio, up to a ratio of 4.5. Additionally, the LIG substrate was reusable for up to five treatment cycles under the optimal laser power. The method was also applied to a more volatile short chain perfluoroalkyl carboxylate TFA, and up to ∼27% of the organic fluorine was converted to NaF as quantified by ion chromatography. Contact angle measurements for both PFOA- and TFA-treated LIG showed decreased wettability after laser irradiation compared to deionized water (DI)-treated controls, possibly indicating incorporation of fluorine (CF) into the LIG chemical structure surface during degradation. The low cost of the methodology and reuse of the substrate offers a sustainable alternative for PFAS degradation and mineralization that might be incorporated into advanced water purification technologies.

全氟烷基和多氟烷基物质（PFAS）是持久性和有毒的水污染物，构成重大的环境和健康风险。目前已有多种处理PFAS的方法，其中大部分依靠吸附法。然而，这些方法通常会产生副产品，需要在处置前进行额外处理。在这里，我们展示了一种简单的方法来降解模型污染物全氟辛酸（PFOA）和三氟乙酸（TFA），使用低能量红外CO2激光器在激光诱导石墨烯（LIG）衬底上，NaOH作为矿化试剂。激光处理实现了高达68%的矿化，并且观察到PFOA中存在的强CF键转化为无机氟化物（NaF），这取决于激光功率，在8%功率时性能最佳。氟矿化效率随着na / f摩尔比的增大而提高，其摩尔比可达4.5。此外，在最佳激光功率下，LIG衬底可重复使用多达五个处理周期。该方法还应用于挥发性更强的短链全氟烷基羧酸TFA，通过离子色谱法定量，高达27%的有机氟转化为NaF。与去离子水（DI）处理的对照相比，经PFOA和tfa处理的LIG在激光照射后的润湿性都有所下降，这可能表明在降解过程中氟（CF）掺入了LIG的化学结构表面。低成本的方法和基材的再利用为PFAS的降解和矿化提供了一个可持续的替代方案，可以纳入先进的水净化技术。

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引用次数: 0

Synergistic effect of carboxyl-functionalized benzothiadiazole-based metal-organic frameworks for enhanced photocatalytic carbon‑nitrogen bond formation 羧基功能化苯并噻二唑基金属有机骨架对增强光催化碳氮键形成的协同作用。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-01-30 DOI: 10.1016/j.jcis.2026.139986

Yujie He , Hongmei Wang , Jiao Chen , Bing Deng , Zhaohui Wang , Ping Liu , Jianli Li

The development of efficient photocatalysts for carbon‑nitrogen (CN) bond formation from aldehydes is highly desirable for the synthesis of functional organic molecules but remains a significant challenge. Herein, we report a novel imidazobenzothiadiazole-based tricarboxylate compound (H₂Ph-COOH, defined as “T-shaped” ligand), and successfully construct the first single-component metal-organic frameworks (MOFs, UiO-68-Ph-COOH) featuring an exposed carboxyl group. This MOFs was effectively employed in the photocatalytic synthesis of amides from aldehydes and amines. The carboxylated T-shaped ligand-based UiO-68-Ph-COOH exhibits outstanding optoelectronic properties and exceptional photocatalytic activity for amide synthesis at room temperature, achieving high yields (up to 92%) within 12 h, along with long-term durability and excellent stability. In comparison, control MOFs (UiO-68-Bt and UiO-68-Ph) derived from linear ligands showed markedly lower catalytic activity (10% and 16% yields, respectively) under identical reaction conditions. Mechanistic studies reveal that the exposed -COOH groups in UiO-68-Ph-COOH act as Brønsted acid sites, which promote the formation of key amino alcohol intermediate and concurrently facilitate the generation of superoxide radical (O₂^•−). This synergistic effect significantly improves the photocatalytic efficiency for amide synthesis. Additionally, UiO-68-Ph-COOH efficiently catalyzes the formation of benzothiazoles and benzimidazoles (up to 94% yield within 1.5 h). This work provides the first demonstration that a single-component MOFs can independently drive photocatalytic amide synthesis and reveals the exposed -COOH functionalization as a crucial design strategy for MOFs-based photocatalysts, thereby opening new avenues for designing efficient MOFs-based photocatalysis of CN bond formation.

醛类碳氮（CN）键形成的高效光催化剂的开发对于合成功能有机分子是非常需要的，但仍然是一个重大的挑战。在此，我们报道了一种新的咪唑苯并噻唑基三羧酸盐化合物（H2Ph-COOH，定义为“t形”配体），并成功构建了第一个具有暴露羧基的单组分金属有机框架（mof, UiO-68-Ph-COOH）。该MOFs有效地应用于光催化醛类和胺类合成酰胺。基于羧基t形配体的UiO-68-Ph-COOH在室温下具有优异的光电性能和优异的光催化活性，在12小时内获得高收率（高达92%），同时具有长期耐用性和优异的稳定性。相比之下，在相同的反应条件下，由线性配体得到的对照MOFs （UiO-68-Bt和UiO-68-Ph）的催化活性明显较低（产率分别为10%和16%）。机制研究表明，UiO-68-Ph-COOH中暴露的- cooh基团作为Brønsted酸位点，促进关键氨基醇中间体的形成，同时促进超氧自由基（O2•-）的生成。这种协同效应显著提高了酰胺合成的光催化效率。此外，UiO-68-Ph-COOH还能有效催化苯并噻唑和苯并咪唑的生成（在1.5 h内收率高达94%）。这项工作首次证明了单组分MOFs可以独立驱动光催化酰胺合成，并揭示了暴露的-COOH功能化是基于MOFs光催化剂的关键设计策略，从而为设计高效的基于MOFs的CN键形成光催化开辟了新的途径。

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引用次数: 0

Electronic modulation with high-valence metal doping towards high-rate Na4Fe3(PO4)2P2O7 cathode in sodium-ion batteries 钠离子电池中高速率Na4Fe3(PO4)2P2O7阴极的高价金属掺杂电子调制。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-02-01 DOI: 10.1016/j.jcis.2026.140025

Dandan Chen , Haonan Xu , Qiming Duan , Jiajun Wang , Yong Jiang

Na₄Fe₃(PO₄)₂P₂O₇ (NFPP) emerges as a cost-effective structurally stable and environmentally benign cathode material, exhibiting significant potential in the energy storage of sodium-ion batteries. However, inherent low ionic mobility and electronic conductivity of NFPP have affected its power performance. In this study, high-valence transition metal cations (Mo⁶⁺, Ta⁵⁺, Nb⁵⁺, and W⁶⁺) are doped within the NFPP lattice, which induces internal electronic rearrangement and average valence state decrease of Fe cations through distortion of locally corner-sharing FeO polyhedra. The increased FeO bond lengths within Mo-doped NFPP crystals and altered electronic cloud distribution further validates this ionic charge compensation mechanism. High-valence metal-doping can also decrease the bandgap, enhance average electronic conductivity, as well as lower Na⁺ migration barrier, thus increasing Na⁺ diffusion coefficient by three orders of magnitude. Therefore, the optimized Na₄Fe_2.91Mo_0.09(PO₄)₂P₂O₇ cathode material demonstrates excellent rate performance and outstanding cycling stability (retaining 85.86% capacity after 1300 cycles at 1C). In addition, the universal effectiveness of the high-valence transition metal doping strategy is verified by investigation of Ta⁵⁺, Nb⁵⁺, and W⁶⁺ doping based on experimental characterizations and theoretical calculations. These findings provide a new perspective to modulate electronic structure and ionic transport pathway of NFPP, and shedding light on great application prospects of iron-based mixed polyanion cathode materials.

Na4Fe3(PO4)2P2O7 （NFPP）作为一种性价比高、结构稳定、环境友好的正极材料，在钠离子电池的储能方面具有重要的潜力。然而，NFPP固有的低离子迁移率和电子导电性影响了其功率性能。本研究在NFPP晶格内掺杂了高价过渡金属阳离子（Mo6+、Ta5+、Nb5+和W6+），通过局部共享角的FeO多面体的畸变引起Fe阳离子内部电子重排和平均价态降低。掺钼NFPP晶体中FeO键长的增加和电子云分布的改变进一步验证了这种离子电荷补偿机制。高价金属掺杂还可以减小带隙，提高平均电子电导率，降低Na+迁移势垒，从而使Na+扩散系数提高3个数量级。因此，优化后的Na4Fe2.91Mo0.09(PO4)2P2O7正极材料具有优异的倍率性能和良好的循环稳定性（在1C下循环1300次后仍保持85.86%的容量）。此外，基于实验表征和理论计算，通过对Ta5+、Nb5+和W6+掺杂的研究，验证了高价过渡金属掺杂策略的普遍有效性。这些发现为调控NFPP的电子结构和离子传输途径提供了新的视角，并揭示了铁基混合聚阴离子正极材料的巨大应用前景。

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引用次数: 0

π-Conjugation engineering in coordination metallopolymers for advanced electrochromic energy storage windows 先进电致变色储能窗配位金属聚合物的π共轭工程。

IF 9.7 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2026-05-15 Epub Date: 2026-02-02 DOI: 10.1016/j.jcis.2026.140033

Yuqi Wu , Bing Cong , Jingjing Yuan , Tianyu Song , Pengwei Zhao , Xiaogang Zhao , Danming Chao , Hongwei Zhou , Chunhai Chen

Coordination metallopolymers (CMPs) have emerged as promising candidates for integrated electrochromic energy storage applications, leveraging their tunable structures that allow for precise control over their optical, electronic, and mechanical properties. However, achieving synergistic enhancement in both electrochromic and energy storage performance remains a significant challenge. To address this, we designed and synthesized two novel D-π-D structured CMPs featuring multiple redox-active centers by virtue of a π-conjugation engineering strategy via facile liquid-liquid interfacial polymerization. The resultant device achieved a high optical contrast of 54.1% at 750 nm, an improved area specific capacitance of 30.46 mF·cm⁻², and a rapid switching speed (2.3 s/1.2 s), attributed to efficient intramolecular charge delocalization and rapid charge transfer kinetics, stemming from the D-π-D molecular architecture. The fabricated smart window demonstrates an effective thermal insulation performance of 14.4 °C temperature reduction versus a general glass window. Furthermore, the electric energy involved in electrochromism could be recycled to power an LED for 30 s. This work provides a viable design strategy for developing high-performance CMPs with integrated electrochromic and energy storage functions.

配合金属聚合物（cmp）已成为集成电致变色储能应用的有前途的候选者，利用其可调结构，可以精确控制其光学，电子和机械性能。然而，实现电致变色和储能性能的协同增强仍然是一个重大挑战。为了解决这一问题，我们利用易于液相界面聚合的π共轭工程策略，设计并合成了两种具有多个氧化还原活性中心的新型D-π-D结构cmp。该器件在750 nm处获得了54.1%的光学对比度，提高了30.46 mF·cm-2的面积比电容，以及快速的开关速度（2.3 s/1.2 s），这归功于高效的分子内电荷离域和源于D-π-D分子结构的快速电荷转移动力学。与普通玻璃窗相比，制造的智能窗户显示出有效的隔热性能，温度降低14.4°C。此外，电致变色过程中产生的电能可以循环利用，为LED供电30秒。这项工作为开发具有集成电致变色和储能功能的高性能cmp提供了可行的设计策略。

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引用次数: 0