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Hierarchically structured NiCo-layered double hydroxides derived from cellulosic filter paper for enhanced photoelectrocatalytic water oxidation 源自纤维素滤纸的分层结构nico层状双氢氧化物,用于增强光电催化水氧化
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-27 DOI: 10.1016/j.colsurfa.2026.139732
Shichao Li , Hongtao Lu , Shiyi Wang , Jie Sun , Yifan Zhang , Weichen Tian , Jiaxing Yang , Jiao Li
Developing low-cost and highly efficient photoelectrocatalysts for water oxidation process occurring on photoanode is crucial in the improvement of photoelectrochemical (PEC) cell efficiency. Herein, NiCo-layered double hydroxides (NiCo-LDHs) were synthesized by using a facile hydrothermal method with filter paper as natural cellulosic template. The NiCo-LDH fabricated with a Ni/Co molar ratio of 1:4 in the mixed precursor solution (T-NiCo (1:4)) retains a well hierarchical microfibrous structure composed of wrinkled LDH nanosheets. The light absorption capability in visible region, electrochemically active surface area, photocurrent response, charge transfer kinetics of T-NiCo (1:4) are obviously improved compared to those properties of NiCo-LDHs with other ratios and the P-NiCo microflower synthesized without cellulosic template, delivering an average O2 evolution rate of 0.37 μmol h–1. This significantly enhanced PEC performance of T-NiCo (1:4) photoanode for catalytic water oxidation is mainly attributed to the hierarchical microstructure that provides abundant hollow spaces for internal light absorption, and the staggered nanosheets like petals that offer more active sites. Moreover, the multivalent states of nickel and cobalt facilitate the transfer and separation of photogenerated carriers. This work provides a feasible strategy for designing LDHs-related catalytic materials for the application in PEC cell.
开发低成本、高效的光阳极水氧化催化剂是提高光电电池效率的关键。本文以滤纸为天然纤维素模板,采用水热法合成了NiCo-LDHs。在混合前驱体溶液(T-NiCo(1:4))中制备的Ni/Co摩尔比为1:4的NiCo-LDH保留了由皱褶状LDH纳米片组成的良好分层微纤维结构。与其他比例的NiCo-LDHs和无纤维素模板合成的P-NiCo微花相比,T-NiCo(1:4)的可见光吸收能力、电化学活性表面积、光电流响应、电荷转移动力学等性能均有明显改善,平均O2析出速率为0.37 μmol h-1。T-NiCo(1:4)光阳极催化水氧化的PEC性能显著提高,主要归功于其层次化的微观结构,为内部光吸收提供了丰富的中空空间,而像花瓣一样交错的纳米片提供了更多的活性位点。此外,镍和钴的多价态有利于光生载流子的转移和分离。本研究为设计用于PEC电池的ldhs相关催化材料提供了可行的策略。
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引用次数: 0
Molecular engineering of low-viscosity deep eutectic solvents for high-capacity and selective SO₂ capture 用于高容量和选择性捕集二氧化硫的低粘度深共晶溶剂的分子工程
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-27 DOI: 10.1016/j.colsurfa.2026.139735
Li-Ming Cheng, Kang-Shou Yin, Jin-Bo Xu, Yong-Hui Liu, Shao-He Wang, Jun Du
Sulfur dioxide (SO₂) is a toxic industrial pollutant and valuable chemical feedstock, making its efficient capture critical for environmental protection and resource recycling. This work rationally designed a novel DES system using 1,3-dimethylimidazolium chloride ([Dim]Cl) as the hydrogen-bond acceptor (HBA) and imidazole as the hydrogen-bond donor (HBD), leveraging a previously underexplored design principle: structural simplification of the HBA cation to mitigate viscosity without sacrificing absorption performance. The optimized [Dim]Cl+imidazole (1:0.5) DES achieves an exceptional SO₂ absorption capacity of 20.69 ± 0.73 mol/kg at 298.2 K and 102.2 kPa (exceeds the majority) while maintaining a low viscosity of 47.1 ± 3.3 cP—over 4-fold lower than analogous [Emim]Cl-based DESs (198.3 cP) with comparable capacity and far below the viscosity of most high-capacity ILs (>200 cP). This low viscosity promotes rapid mass transfer, as confirmed by pseudo-first-order kinetics (k₁=0.089 ± 0.016 mol/(kg·min), R²> 0.98). The DES also exhibits outstanding selectivity (SO₂/CO₂=547, SO₂/N₂=1169) and perfect regenerability over ten cycles. At low concentrations(<10kpa), the DES exhibits enhanced selectivity(SO₂/CO₂=5013, SO₂/N₂=15563). A synergistic absorption mechanism was elucidated via spectroscopic analysis and quantum chemical calculations: SO₂ is simultaneously captured by multiple sites—Cl⁻ (strong nucleophilic coordination) and the imidazole ring (weak basicity and hydrogen-bonding facilitation). This multi-site interaction is the origin of the DES’s superior performance.
二氧化硫(so2)是一种有毒的工业污染物和有价值的化工原料,其有效捕获对环境保护和资源回收至关重要。本研究以1,3-二甲基咪唑氯([Dim]Cl)为氢键受体(HBA),咪唑为氢键给体(HBD),合理设计了一种新型的DES系统,利用了以前未被开发的设计原则:在不牺牲吸收性能的情况下,简化HBA阳离子的结构以降低粘度。优化[暗淡]Cl +咪唑(1:0.5)DES达到一个特殊所以₂吸收能力20.69 ±0.73  摩尔/公斤298.2 K和102.2 kPa(超过多数),同时保持低粘度47.1 ±3.3  cP / 4倍低于类似(以)Cl-based密不可分(198.3 cP)和类似的能力远低于大多数高容量ILs的粘度(200年祝辞 cP)。伪一级动力学证实,这种低粘度促进了快速的传质(k₁=0.089 ± 0.016 mol/(kg·min), R²>; 0.98)。DES还表现出优异的选择性(SO₂/CO₂=547,SO₂/N₂=1169)和良好的十次循环再生能力。在低浓度(<10kpa)下,DES表现出增强的选择性(SO₂/CO₂=5013,SO₂/N₂=15563)。通过光谱分析和量子化学计算阐明了一种协同吸收机制:SO₂同时被cl -(强亲核配位)和咪唑环(弱碱性和氢键促进)多个位点捕获。这种多站点交互是DES优越性能的来源。
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引用次数: 0
Highly crystalline carbon dots as dual function interfacial modifiers for defect passivation and phase stabilization in perovskite solar cells 高结晶碳点作为钙钛矿太阳能电池缺陷钝化和相稳定的双功能界面改进剂
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139722
Junjie Wang , Xinxin Li , Haozhi Jiao , Jiansheng Yang , Lingpeng Yan , Changzeng Ding , Yongzhen Yang , Chang-Qi Ma
Perovskite solar cells (PSCs) have achieved remarkable power conversion efficiencies, however, their operational instability originating from buried interfacial defects and phase degradation of perovskites remains a critical challenge. Although carbon dots (CDs) have been widely explored as defect passivators, their capability to regulate perovskite phase stability has rarely been explored. In this study, we report highly crystalline carbon dots enriched with amino, carboxyl, and hydroxyl groups as a dual-function interfacial modifier at the SnO2/perovskite buried interface. Distinct from conventional amorphous CDs, the high crystallinity of these CDs enables enhanced defect-passivation capability and improved ability to suppress harmful phase transitions, thereby simultaneously passivating Pb²⁺-related defects and suppressing the detrimental α-to-δ phase transition during device operation. The multifunctional surface groups coordinate with undercoordinated Pb²⁺ and I⁻, thereby effectively inhibiting the formation of PbI2 and the phase degradation of perovskites. Consequently, the CDs-modified perovskite films exhibit improved crystallinity, enlarged grain sizes, suppressed interfacial non-radiative recombination and enhanced interfacial charge extraction. The optimized PSCs deliver a champion power conversion efficiency of 21.50 % and retain 83 % of their initial efficiency after 1000 h of continuous illumination, significantly outperforming the control devices, which retain only 43 %. This work reveals an overlooked role of crystalline carbon dots in regulating perovskite phase stability and provides a simple, low-cost, and effective strategy for simultaneously improving the efficiency and operational stability of PSCs.
钙钛矿太阳能电池(PSCs)已经取得了显著的功率转换效率,然而,由钙钛矿的埋藏界面缺陷和相降解引起的运行不稳定性仍然是一个关键的挑战。虽然碳点作为缺陷钝化剂已被广泛研究,但其调节钙钛矿相稳定性的能力却很少被研究。在这项研究中,我们报道了富含氨基、羧基和羟基的高结晶碳点作为SnO2/钙钛矿埋藏界面的双功能界面调节剂。与传统的非晶CDs不同,这些CDs的高结晶度增强了缺陷钝化能力,提高了抑制有害相变的能力,从而在钝化Pb 2 +相关缺陷的同时,抑制了器件运行过程中有害的α-to-δ相变。多功能表面基团与欠配位的Pb 2 +和I⁻配合,有效抑制了PbI2的形成和钙钛矿的相降解。结果表明,cd修饰的钙钛矿薄膜结晶度提高,晶粒尺寸增大,界面非辐射复合抑制,界面电荷提取增强。优化后的psc提供了21.50%的冠军功率转换效率,并在1000 h的连续照明后保持了83%的初始效率,显著优于控制设备,后者仅保持了43%。这项工作揭示了晶体碳点在调节钙钛矿相稳定性方面被忽视的作用,并为同时提高PSCs的效率和运行稳定性提供了一种简单、低成本和有效的策略。
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引用次数: 0
In situ self-assembly of Fe-N-C oxygen reduction catalysts and morphology evolution triggered by sulfates Fe-N-C氧还原催化剂的原位自组装及硫酸盐引发的形貌演化
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139708
Linxuan Cao , Qiongyao Guo , Qingmin Hu, Junping Dong
Transition-metal-nitrogen-carbon catalysts have been considered one of the most promising oxygen reduction catalysts. Generally, direct pyrolysis and template approaches are popular in preparation of ORR catalysts. Yet these methods are restricted to a certain extent due to their inherent flaws. Therefore, the elaborate design and controllable synthesis of catalysts still remain challenges. Here, Polydopamine-derived Fe-N-C catalysts are in situ fabricated by self-assembly strategy. Nanorod-like catalysts were obtained by pyrolysis of FeSO4-Phen/PDA/F127@trimethylbenzene composite micelles. The introduction of SO42- ion plays a critical role in the morphology evolution from nanospheres to nanorods with the assistance of phenanthroline. The presence of trimethylbenzene (TMB) facilitates the dispersion of single atom Fe on the surface of composite micelles. Thus the simultaneous modulation of active sites and carbon architectures on Fe-N-C catalysts were achieved by finely regulating the interfaces of composite micelles. The novel catalyst exhibits good ORR activity and durability over Pt/C catalyst with more positive half-wave potential and higher current density. The good electrocatalytic performances are attributed to the larger surface areas, hierarchical porous structures and highly active FeN4 sites. Moreover, Zn-air battery fabricated with Fe-N-C catalysts as the air cathode display higher power density of 116 mW cm−2 and specific capacity of 713 mA h g−1. This work will open up a new avenue for in situ fabrication of M-N-C catalysts (M=Cu, Co, Ni, Mn, Zn) via self-assembly strategy.
过渡金属-氮-碳催化剂被认为是最有前途的氧还原催化剂之一。一般来说,直接热解法和模板法是制备ORR催化剂的常用方法。然而,这些方法由于其固有的缺陷,在一定程度上受到了限制。因此,催化剂的精细设计和可控合成仍然是一个挑战。本研究通过自组装策略原位制备了聚多巴胺衍生的Fe-N-C催化剂。通过热解FeSO4-Phen/PDA/F127@trimethylbenzene复合胶束制备纳米棒状催化剂。在菲罗啉的辅助下,SO42-离子的引入对纳米球向纳米棒的形态演变起着至关重要的作用。三甲基苯(TMB)的存在有利于单原子铁在复合胶束表面的分散。因此,通过精细调节复合胶束的界面,可以实现Fe-N-C催化剂上活性位点和碳结构的同步调节。与正半波电位高、电流密度大的Pt/C催化剂相比,该催化剂具有良好的ORR活性和耐久性。其良好的电催化性能主要归功于较大的比表面积、层次化的多孔结构和高活性的FeN4位点。以Fe-N-C催化剂为空气阴极制备的锌空气电池具有较高的功率密度(116 mW cm−2)和比容量(713 mA h g−1)。这项工作将为通过自组装策略原位制备M- n - c催化剂(M=Cu, Co, Ni, Mn, Zn)开辟一条新的途径。
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引用次数: 0
Brownian dynamics simulation of structural evolution in drying colloid-polymer mixtures 干燥胶体-聚合物混合物结构演化的布朗动力学模拟
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139719
Hyunjeong An, Young Ki Lee
Drying-induced structural evolution in colloid–polymer mixtures plays a crucial role in determining the mechanical and functional properties of composite films. Despite its practical relevance, theoretical studies that simultaneously resolve interfacial stratification and pore/packing evolution during drying of colloid–polymer mixtures remain limited. Here, Brownian dynamics simulations were conducted to elucidate the effects of polymer concentration, chain length, and colloid–polymer interactions on the microstructure of dried colloid–polymer films. Polymer addition markedly altered interfacial stratification and particle packing. In the colloid-only dispersed system, colloidal particles progressively accumulated and packed near the liquid–gas interface; in contrast, in colloid–polymer mixtures, the interfacial region became increasingly enriched with polymer during drying, hindering the formation of a densely packed colloidal layer. An increasing polymer concentration promoted the development of a polymer-enriched layer near the liquid–gas interface, suppressing colloidal accumulation and increasing interfacial porosity. Voronoi analysis was employed to quantitatively characterize the colloidal structures formed within the dried films. Higher polymer concentrations led to greater heterogeneity in interparticle spacing and broader pore-size distributions, whereas variations in polymer chain length exerted only a minor influence on the structural evolution within the tested range. Finally, introducing colloid–polymer attraction through a Lennard–Jones potential significantly reduced polymer migration toward the interface, thereby yielding denser packing and narrower pore-size distributions. These findings suggest that colloid–polymer affinity can be an important factor influencing final film morphology under convection-dominated drying. The present study provides insights into microstructural control in functional colloid–polymer coatings and drying processes, while highlighting the utility of simulation-based prediction for film formation.
干燥诱导的胶体-聚合物混合物的结构演变对复合膜的力学和功能性能起着至关重要的作用。尽管具有实际意义,但同时解决胶体-聚合物混合物干燥过程中界面分层和孔隙/堆积演变的理论研究仍然有限。本文通过布朗动力学模拟来阐明聚合物浓度、链长和胶体-聚合物相互作用对干燥的胶体-聚合物薄膜微观结构的影响。聚合物的加入显著改变了界面分层和颗粒堆积。在纯胶体分散体系中,胶体颗粒在液气界面附近逐渐积聚和堆积;相反,在胶体-聚合物混合物中,在干燥过程中,界面区域越来越多地富集聚合物,阻碍了致密堆积胶体层的形成。聚合物浓度的增加促进了液气界面附近富集聚合物层的发育,抑制了胶体的聚集,增加了界面孔隙度。Voronoi分析用于定量表征干燥膜内形成的胶体结构。聚合物浓度越高,颗粒间距的非均质性越大,孔径分布越宽,而聚合物链长度的变化对测试范围内结构演化的影响较小。最后,通过Lennard-Jones势引入胶体-聚合物吸引力,显著减少了聚合物向界面的迁移,从而产生更致密的填料和更窄的孔隙尺寸分布。这些发现表明,在对流主导的干燥条件下,胶体-聚合物亲和度可能是影响最终膜形态的重要因素。本研究为功能性胶体聚合物涂层和干燥过程的微观结构控制提供了见解,同时强调了基于模拟的薄膜形成预测的实用性。
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引用次数: 0
Effects of oil-water interfacial evolution driven by oil compositional differences on two-phase flow in shale nanopores: A molecular perspective 油组分差异驱动的油水界面演化对页岩纳米孔两相流动的影响:分子视角
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139720
Ziqing Liu , Long Xu , Mingyuan Xin , Tianning Fei , Guodong Yang , Houjian Gong , Mei-Chun Li , Hai Sun , Mingzhe Dong
Hydraulic fracturing promotes widespread oil-water two-phase flow within shale nanopores. Real shale oil exhibits a high degree of compositional complexity. Simplifying shale oil to alkanes in previous studies may overlook the influence of specific components on oil-water interfacial evolution, which governs two-phase flow. In this work, molecular dynamics (MD) simulations are used to investigate the flow behavior of multi-component oil and water within shale nanopores. Compared with alkanes, active component (n-decylamine) and heavy component (asphaltene) show preferential adsorption to the water layer at the oil-water interface, primarily driven by electrostatic interactions. Interestingly, this phenomenon significantly weakens the liquid-liquid slip at the oil-water interface and reduces the flow velocities. It also demonstrates that increasing the pressure gradient promotes desorption of n-decylamine and asphaltenes from the oil-water interface into the pure oil phase. Differences in interaction energy with the water layer lead to a relatively greater desorption of asphaltenes. For a 9 nm nanopore, an increased pressure gradient was found to induce a flow-regime transition from parabolic to piston-like. This study offers new insights into oil-water two-phase flow and provides theoretical guidance for optimizing shale oil production.
水力压裂促进了页岩纳米孔内广泛的油水两相流动。真正的页岩油具有高度的成分复杂性。以往的研究将页岩油简化为烷烃,忽略了特定组分对油水界面演化的影响,而油水界面演化控制着两相流动。在这项工作中,采用分子动力学(MD)模拟来研究页岩纳米孔中多组分油水的流动行为。与烷烃相比,活性组分(正癸胺)和重质组分(沥青质)在油水界面处优先吸附于水层,主要受静电相互作用驱动。有趣的是,这种现象显著减弱了油水界面的液-液滑移,降低了流动速度。增大压力梯度可促进正癸胺和沥青质从油水界面解吸进入纯油相。与水层相互作用能的差异导致沥青质的解吸相对较大。对于9 nm的纳米孔,增加的压力梯度可以诱导流型从抛物线型转变为活塞型。该研究为油水两相流动提供了新的认识,为页岩油优化生产提供了理论指导。
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引用次数: 0
Bioinspired antibacterial microspheres: Integrating Co3O4/Mn3O4 nanozyme catalysis and CuO nanoparticles in a single platform 仿生抗菌微球:将Co3O4/Mn3O4纳米酶催化和CuO纳米颗粒整合在一个单一平台上
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139709
Chao Chen, Lei Xia, Wenjun Pan, Sheng Pu, Dongpeng Wang, Yuxin Wang
Oxidase-like enzymes have been considered as the promising antibacterial agent for toxicity of H2O2 can be absolutely avoid. Development of mixed metal oxides-based nanozymes has been considered as an essential method for enhancing the antibacterial activity. Bioinspired by the efficient catalytic action of natural oxidases, novel ternary mixed metal oxides (MMOs) microspheres were designed through modulating the ratio of Co, Mn, Cu as oxidase-like catalytic platform for achieving a biomimetic antibacterial activity. In this work, a composite system leveraging oxidase-like enzymes of Co3O4 and Mn3O4 were designed to achieve efficient catalytic function through substrate capture and generating reactive oxygen radicals (ROS) by tailoring the composition and structure. Additionally, antibacterial components such as CuO nanoparticles and Co3O4 were incorporated to enhance antimicrobial efficacy. Interestingly, by controlling of CoMnCu components ratio at 2:1:1, the achieved ternary Co2MnCu MMOs microsphere exhibits an inhibition rate more than 99.15 % against Escherichia coli. The excellent sterilization ability is primarily attributed to the strong substrate affinity (Km=0.0715 mM) of the oxidase-mimicking and the optimal content (2.7 %) of CuO for the Co2MnCu microsphere composed of nanoneedles. This research shed light on a novel designing strategy for environmentally friendly antibacterial materials and contributes to the advancement of sustainable materials.
氧化酶类酶被认为是很有前途的抗菌剂,因为H2O2的毒性是完全可以避免的。开发基于混合金属氧化物的纳米酶已被认为是提高抗菌活性的重要方法。以天然氧化酶的高效催化作用为灵感,通过调节Co、Mn、Cu的比例,设计了新型三元混合金属氧化物微球作为类似氧化酶的催化平台,实现了仿生抗菌活性。在这项工作中,利用氧化酶样酶Co3O4和Mn3O4设计了一个复合体系,通过调整组成和结构,通过捕获底物和产生活性氧自由基(ROS)来实现高效的催化功能。此外,加入CuO纳米颗粒和Co3O4等抗菌成分以提高抗菌效果。有趣的是,将CoMnCu组分比控制在2:1:1时,获得的三元Co2MnCu MMOs微球对大肠杆菌的抑制率超过99.15 %。其优异的杀菌能力主要归功于氧化酶模拟物的强底物亲和力(Km=0.0715 mM)和纳米针组成的Co2MnCu微球的最佳CuO含量(2.7 %)。本研究为环境友好型抗菌材料的设计提供了新的思路,为可持续材料的发展做出了贡献。
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引用次数: 0
Passive radiative cooling utilizing a fluorinated liquid crystal-doped polymer dispersed liquid crystal smart window 利用含氟液晶掺杂聚合物分散液晶智能窗口的被动辐射冷却
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139717
Yi-Feng Qiu , Boyu Chen , Jingjing Chen , Dongqian Xue , Xuanyi Yan , Wenhuan Yao , Ping Yu , Zemin He
Energy crises and environmental and climate challenges are becoming increasingly severe, with substantial energy consumption often being squandered on space cooling. Passive Radiative Cooling (PRC) technology can reduce energy consumption while implementing temperature management. This study prepared a series of polymer-dispersed liquid crystal (PDLC) films by introducing fluorinated liquid crystal molecules into PDLC systems. By integrating PDLC materials with PRC technology and leveraging PDLC's excellent dimming capabilities, it resolved the issues of high drive voltage and low contrast inherent in conventional PDLC. Concurrently, the incorporation of fluorinated liquid crystals endowed the PDLC with radiative cooling properties, addressing the inherent conflict in smart window PRC materials between optical performance and cooling capacity. Research findings indicate that compared to conventional PDLC, the resulting films exhibit not only low saturation voltage (<18 V) and high contrast (>70) in optoelectronic performance, but also demonstrate exceptional light modulation capabilities across the solar spectrum. Furthermore, the film exhibits high emissivity (approximately 95 %) in the atmospheric window band (8–14 μm), with a theoretical radiative cooling capacity of 109.09 W/m²/K. This capability reduces simulated indoor ambient temperature by 5.9 °C. This work confirms the application potential of fluorinated PDLC in the field of PRC smart windows.
能源危机以及环境和气候挑战日益严峻,大量能源消耗往往被浪费在空间冷却上。被动辐射冷却(PRC)技术可以在实现温度管理的同时降低能源消耗。本研究将氟化液晶分子引入聚合物分散液晶(PDLC)体系,制备了一系列聚合物分散液晶薄膜。通过将PDLC材料与PRC技术相结合,并利用PDLC出色的调光能力,解决了传统PDLC固有的高驱动电压和低对比度问题。同时,氟化液晶的加入使PDLC具有辐射冷却性能,解决了智能窗口PRC材料在光学性能和冷却能力之间的固有冲突。研究结果表明,与传统的PDLC相比,所得到的薄膜不仅具有低饱和电压(<18 V)和高对比度(>70)的光电性能,而且还具有跨太阳光谱的卓越光调制能力。此外,薄膜在大气窗口波段(8-14 μm)内具有较高的发射率(约95 %),理论辐射制冷量为109.09 W/m²/K。该功能可将模拟室内环境温度降低5.9°C。这一工作证实了氟化PDLC在PRC智能窗领域的应用潜力。
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引用次数: 0
Selective ·OH generation of WO₃ via Facet-directed engineering for photoelectrochemical antibiotic degradation 面向面工程在抗生素光电降解中的选择性·OH生成WO₃
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139715
Tong Tong , Tao Wei , Wenfang Zheng , Jinyou Shen , Wei Yang , Chaoran Dong , Kan Zhang
Tetracycline’s extensive use and persistence have led to significant environmental contamination. Photoelectrochemical (PEC) advanced oxidation processes (AOPs) offer a sustainable solution by harnessing solar-driven water oxidation to generate reactive oxygen species (ROS), enabling energy-efficient degradation of recalcitrant pollutants. However, PEC efficiency is often hindered by sluggish charge transfer and limited selectivity toward hydroxyl-radical formation. Here, we introduce a controlled synthesis strategy for WO3 photoanodes in which exposure of the (002) facet is precisely tuned by simply adjusting the precursor composition. Enriching the (002) facet not only enhances PEC activity but also promotes selective hydroxyl-radical generation. Under 150 min of irradiation, the optimized WO3 photoanode achieves 75 % tetracycline degradation and maintains stable operation for over 10 h. This work highlights the advantages of facet-engineered WO3 and underscores the promise of PEC-based AOPs for efficient antibiotic wastewater treatment.
四环素的广泛使用和持续使用导致了严重的环境污染。光电化学(PEC)高级氧化工艺(AOPs)提供了一种可持续的解决方案,利用太阳能驱动的水氧化来产生活性氧(ROS),从而实现对难降解污染物的高效降解。然而,PEC效率经常受到缓慢的电荷转移和对羟基自由基形成的有限选择性的阻碍。在这里,我们介绍了一种WO3光阳极的受控合成策略,其中(002)面的曝光可以通过简单地调整前驱体组成来精确调节。丰富(002)面不仅可以增强PEC活性,还可以促进选择性羟基自由基的产生。在150 min的辐照下,优化后的WO3光阳极对四环素的降解率达到75% %,并能稳定运行10 h以上。这项工作强调了面工程WO3的优势,并强调了基于pec的AOPs用于高效抗生素废水处理的前景。
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引用次数: 0
Synergistic effect of electronic redistribution in p–n heterojunction for boosted oxygen evolution p-n异质结电子重分布对促进析氧的协同效应
IF 5.4 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-26 DOI: 10.1016/j.colsurfa.2026.139716
Ziyang Yan , Bo Feng , Keyi Lv , Nianwen Song , Ziyong Zhang , Yuchao Zhang , Yanfei Wei , Xiaofei Yu , Lanlan Li , Xinghua Zhang , Xiaojing Yang , Zunming Lu , Juntao Huo
Layered double hydroxides (LDHs) are now used as non-precious metal catalysts, and their main active centers are highly oxidized metal hydroxide oxides. However, poor conductivity, limited active sites, and low stability hinder the further improvement of OER performance. This work creates a p-n heterojunction by coupling deposited n-type semiconductor NiCoFeLDH with p-type semiconductor Co3O4 nanoneedles to create an effective OER catalyst based on a nickel foam (NF) substrate. The Co3O4 nanoneedle shape enhances the contact area and exposure of active sites in NiCoFeLDH. Interfacial electron transfer creates a depletion layer in NiCoFeLDH, decreasing the coordination number of Co atoms and raising their oxidation state. This promotes OH⁻ adsorption and the phase change from Co(OH)2 to CoOOH. XPS, M-S tests, DFT calculations, and UPS analysis all proved that the p-n junction caused electrons to transfer from NiCoFeLDH to Co3O4, resulting in an optimized d band center. Under alkaline circumstances, the Co3O4/NiCoFeLDH@NF electrode requires only 227 mV overpotential to achieve a current density of 100 mA cm−2 and remains stable for more than 200 h, demonstrating excellent catalytic activity and durability.
层状双氢氧化物(LDHs)目前被用作非贵金属催化剂,其主要活性中心是高度氧化的金属氢氧化物。然而,电导率差、活性位点有限和稳定性低阻碍了OER性能的进一步提高。本研究通过将沉积的n型半导体NiCoFeLDH与p型半导体Co3O4纳米针耦合,创建了p-n异质结,从而创建了基于泡沫镍(NF)衬底的有效OER催化剂。Co3O4纳米针的形状增加了NiCoFeLDH中活性位点的接触面积和暴露。界面电子转移在NiCoFeLDH中形成耗尽层,降低Co原子的配位数,提高其氧化态。这促进了OH -吸附和从Co(OH)2到CoOOH的相变。XPS, M-S测试,DFT计算和UPS分析都证明了p-n结导致电子从NiCoFeLDH转移到Co3O4,导致d带中心优化。在碱性环境下,Co3O4/NiCoFeLDH@NF电极只需要227 mV过电位就能达到100 mA cm−2的电流密度,并在200 h以上保持稳定,表现出优异的催化活性和耐久性。
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Colloids and Surfaces A: Physicochemical and Engineering Aspects
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