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The effect of particle size on the dynamics of self-electrophoretic Janus micromotors, sputtering distribution, and rectifying voltage 粒径对自电泳Janus微电机动力学、溅射分布和整流电压的影响
Q3 Materials Science Pub Date : 2022-04-01 DOI: 10.1016/j.jciso.2022.100046
Shuaishuai Meng , Yueyue Zhang , Yaming Liu , Zhenchao Zhang , Kunpeng Ma , Xiaowen Chen , Qiang Gao , Xing Ma , Wei Wang , Huanhuan Feng

Micromotors have gained increasing attention in last two decades, due to their controllable self-propulsion maneuverability at micro scales. However, the effect of particle size on micromotors is still vague and interwoven due to the micromotors’ size, polydisperse distribution, and structural variations. Microfluidic technology is used to clarify the phenomenon, due to its precise micro scale fabrication. Herein, we fabricated a H2O2-driven self-electrophoretic Janus micromotor and systematically explored the effects of particle size on their dynamics, the sputtering distribution, and the rectifying voltages. Their speeds were found to be inversely proportional to their sizes. When the particle size was fixed, their speeds increased as coating thickness increased until its hemisphere was fully coated, and this critical coating thickness was also proportional to the sizes of the micromotors. As further investigation goes on, we noticed that electrical voltage to rectify micromotor was proportional to its size too. To summarize, our results showed that larger micromotors moved more slowly, required a thicker metal coating to reach full speeds, and needed higher voltages to be rectified. Through all of these investigations, we believed that microfluidic technology is a valuable tool, which can systematically probe micromotors dynamics and clarify our understanding of micromotors behaviors.

由于微电机在微尺度上具有可控的自推进机动性能,近二十年来受到越来越多的关注。然而,由于微电机的尺寸、多分散分布和结构的变化,颗粒尺寸对微电机的影响仍然是模糊和相互交织的。微流控技术由于其精确的微尺度制造而被用于澄清这一现象。在此,我们制作了一个h2o2驱动的自电泳Janus微电机,并系统地研究了粒径对其动力学、溅射分布和整流电压的影响。他们发现它们的速度与它们的大小成反比。当颗粒尺寸固定时,随着涂层厚度的增加,其速度增加,直到其半球完全被涂层,并且这个临界涂层厚度也与微电机的尺寸成正比。随着进一步的研究,我们注意到整流微电机的电压也与其尺寸成正比。总而言之,我们的结果表明,较大的微电机移动更慢,需要更厚的金属涂层才能达到全速,并且需要更高的电压来整流。通过这些研究,我们认为微流控技术是一种有价值的工具,可以系统地探索微电机动力学,阐明我们对微电机行为的理解。
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引用次数: 4
Responsive emulsions with Janus topology constructed by magneto-surfactants and remote control of emulsion stability 磁表面活性剂构建具有Janus拓扑的响应性乳剂,并对乳剂稳定性进行远程控制
Q3 Materials Science Pub Date : 2022-04-01 DOI: 10.1016/j.jciso.2022.100043
Haixia Zhang , Lingling Ge , Rong Guo

The fluids with well-defined inner structure and intrinsic responsibility are demanding to the maintenance and regulation of normal functions in living systems. Inspired by this, responsive Janus droplets are constructed by small molecules of magneto-surfactants, and the traditional vortex mixing is applied to guarantee large-scale fabrication. Silicone oil (SO) and Vegetable oil (VO) as two immiscible oils are introduced as inner phases of the Janus emulsions. The topology and subsequently the magnetic responsive performance of Janus emulsion is controlled by adjusting the oil composition with various viscosity, the surfactant concentration and the mass ratio of two oils. Moreover, the remote control of the emulsion stability is realized by the external magnetic field, of which the demulsification mechanism is investigated. The anisotropic and responsive droplets with advantages of deformability, encapsulation capability, and biocompatibility would expand the application of emulsions in targeted therapy, drug delivery and magnetic materials science.

流体具有明确的内部结构和内在责任,对维持和调节生命系统的正常功能是有要求的。受此启发,反应灵敏的Janus液滴由磁表面活性剂的小分子构成,并应用传统的涡旋混合来保证大规模制造。介绍了硅油(SO)和植物油(VO)两种不混相油作为Janus乳剂的内相。通过调节不同粘度的油的组成、表面活性剂的浓度和两种油的质量比来控制Janus乳液的拓扑结构和磁响应性能。利用外加磁场实现了乳状液稳定性的远程控制,并对外加磁场的破乳机理进行了研究。具有可变形性、包封性和生物相容性等优点的各向异性和响应性微滴将扩大乳剂在靶向治疗、药物传递和磁性材料科学方面的应用。
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引用次数: 0
pH and ionic strength triggered destabilization of biocompatible stable water-in-oil-in-water (W/O/W) emulsions pH和离子强度触发了生物相容性稳定水包油(W/O/W)乳状液的失稳
Q3 Materials Science Pub Date : 2022-04-01 DOI: 10.1016/j.jciso.2021.100039
Marine Protat , Noémie Bodin-Thomazo , Frédéric Gobeaux , Florent Malloggi , Jean Daillant , Nadège Pantoustier , Patrick Perrin , Patrick Guenoun

The design of biocompatible multiple emulsions is an important challenge in the field of controlled delivery systems for protecting and delivering compounds encapsulated and protected in the innermost phase. In this paper, we use biocompatible water – Miglyol®812 water-in-oil-in-water (W/O/W) emulsions stabilized by a stimuli-responsive diblock copolymer consisting of poly(dimethylsiloxane) (PDMS) and poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) to design an easy-to-process new delivery W/O/W system. Such emulsions are formed in a single emulsification step. They present a high encapsulation yield and are shown to be stable over months. As such, the encapsulation of a hydrophilic dye (Alexa fluor) in the innermost water phase is successfully demonstrated over months. These emulsions are stimulable either by a shift in pH level or in ionic strength. The former destabilizes the multiple emulsion and leads to a simple one while the latter partly maintains the multiple character. Eventually both stimulations are effective in the dye release and molecular mechanisms are proposed for explaining the observed two-stage kinetics of release.

生物相容性多重乳剂的设计是控制递送系统领域的一个重要挑战,用于保护和递送包裹在最内层相的化合物。在本文中,我们使用生物相容性水- Miglyol®812水包油包水(W/O/W)乳液,由刺激响应的二嵌段共聚物组成的聚(二甲硅氧烷)(PDMS)和聚(2-(二甲氨基)甲基丙烯酸乙酯)(PDMAEMA)稳定,设计了一种易于处理的新型W/O/W系统。这种乳剂是在一次乳化步骤中形成的。它们具有很高的包封率,并且在几个月内保持稳定。因此,亲水染料(Alexa氟)在最内层水相的封装已经成功地演示了几个月。这些乳剂可以通过pH值的变化或离子强度的变化来刺激。前者使复合乳液失稳,形成单一乳液,后者部分保持了复合乳液的特性。最后,这两种刺激在染料释放中都是有效的,并提出了分子机制来解释所观察到的两阶段释放动力学。
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引用次数: 1
Self-assembly of colloidal superballs under spherical confinement of a drying droplet 在干燥液滴的球形约束下胶体超球的自组装
Q3 Materials Science Pub Date : 2022-04-01 DOI: 10.1016/j.jciso.2021.100037
Sarah Schyck , Janne-Mieke Meijer , Lucia Baldauf , Peter Schall , Andrei V. Petukhov , Laura Rossi

Understanding the relationship between colloidal building block shape and self-assembled material structure is important for the development of novel materials by self-assembly. In this regard, colloidal superballs are unique building blocks because their shape can smoothly transition between spherical and cubic. Assembly of colloidal superballs under spherical confinement results in macroscopic clusters with ordered internal structure. By utilizing Small Angle X-Ray Scattering (SAXS), we probe the internal structure of colloidal superball dispersion droplets during confinement. We observe and identify four distinct drying regimes that arise during compression via evaporating droplets, and we track the development of the assembled macrostructure. As the superballs assemble, we found that they arrange into the predicted paracrystalline, rhombohedral C1-lattice that varies by the constituent superballs’ shape. This provides insights in the behavior between confinement and particle shape that can be applied in the development of new functional materials.

了解胶体构筑块形状与自组装材料结构之间的关系,对于开发新型自组装材料具有重要意义。在这方面,胶体超级球是独特的积木,因为它们的形状可以在球形和立方之间平滑地转换。胶体超球在球形约束下的组装产生具有有序内部结构的宏观团簇。利用小角x射线散射(SAXS)技术,研究了胶体超球分散液滴在约束过程中的内部结构。我们观察并确定了通过蒸发液滴在压缩过程中产生的四种不同的干燥制度,并跟踪了组装宏观结构的发展。当超级球组装时,我们发现它们排列成预测的准晶、菱形c1晶格,这种晶格随组成超级球的形状而变化。这为约束和粒子形状之间的行为提供了见解,可以应用于新功能材料的开发。
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引用次数: 3
Superwetting antibacterial copper oxide nanoflake foil substrates generated by thermal oxidation 热氧化制备的超湿抗菌氧化铜纳米片箔衬底
Q3 Materials Science Pub Date : 2022-04-01 DOI: 10.1016/j.jciso.2021.100042
Zhixiong Song , Jian Wern Ong , Eric Shen Lin , Hassan Ali Abid , Oi Wah Liew , Tuck Wah Ng

A facile one-step method of roughened copper foils of 0.0076 ​mm thickness heated on the open flame for 15 ​s produced superhydrophilic surfaces that exhibited superwetting at average radial growths of 10.8 ​mm/s following drop dispensation. Superhydrophilicity was found to deteriorate over time and XRD analysis ruled out compositional change as the cause of this behaviour. Instead, SEM imaging revealed wrinkled 20–30 ​nm-thick nanoflakes that were predominantly stretched out initially to engender superwetting properties via Wenzel wetting. These extended microstructures folded up with time due to relaxation of the residual stresses from the thermal oxidation process, resulting in temporal reduction in superhydrophilicity, which can be restored by reapplying thermal oxidation. The impingement of air with 80 psi pressure on the substrate also caused similar deterioration. The superwetting characteristic also endowed these substrates with anti-bacterial properties where a 56% reduction in bacteria count with Staphylococcus epidermidis was found.

一种简单的一步法将厚度为0.0076 mm的粗铜箔在明火上加热15 s,产生了超亲水表面,在滴注后,其平均径向生长速度为10.8 mm/s。发现超亲水性随着时间的推移而恶化,XRD分析排除了成分变化是这种行为的原因。相反,扫描电镜成像显示,褶皱的20-30纳米厚的纳米片最初主要拉伸,通过温泽尔润湿产生超润湿特性。由于热氧化过程中残余应力的松弛,这些扩展的微观结构随着时间的推移而折叠,导致超亲水性的暂时降低,可以通过再次施加热氧化来恢复。压力为80psi的空气对基材的冲击也导致了类似的劣化。超润湿特性也赋予这些底物抗菌性能,其中表皮葡萄球菌细菌数量减少56%。
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引用次数: 1
Surfactant enhanced imbibition in carbonate reservoirs: Effect of IFT reduction and surfactant partitioning 表面活性剂增强碳酸盐岩储层的渗吸:IFT降低和表面活性剂分配的影响
Q3 Materials Science Pub Date : 2022-04-01 DOI: 10.1016/j.jciso.2022.100045
Ziyuan Qi , Ming Han , Shaohua Chen , Jinxun Wang

A majority of carbonate reservoirs are preferably oil-wet or intermediate wet. Spontaneous imbibition represents an important mechanism to enhance oil production. Targeting an oil-wet carbonate reservoir with high temperature and high salinity, several surfactant formulations were investigated to improve oil production by imbibition, focusing on the capacity in interfacial tension (IFT) reduction and surfactant partitioning in water and oil phases in addition to dominant wettability alteration effect. Oil production potentials using different surfactants were evaluated by spontaneous imbibition in Amott cells at 95 ​°C. A base case imbibition test was conducted using a high salinity water with IFT value of 15.2 ​mN/m and an oil-wet carbonate core, and the oil production was 6.4% of oil originally saturated in core. Reducing the oil-water IFT to 10° ​mN/m magnitude achieved 4% incremental oil production beyond base case. When the IFT was further reduced to 10−1 ​mN/m magnitude, the incremental oil production reached 10%. For the case of water-wet core and at the same IFT range, the incremental oil production was 13%. When the IFT was reduced to 10−2 ​mN/m, the incremental oil production was up to 17% for the tests using oil-wet cores, and up to 23% for the water-wet counterpart. When further reducing the IFT to ultra-low magnitude of 10−3 ​mN/m, the oil production was close to that using the imbibition agents with IFT of 10−2 ​mN/m magnitude. For surfactants with no obvious wettability alteration capacity, those surfactants with higher molecular fraction in oil phase and higher adsorption on rock surfaces could remove more oil from the pore wall, and yielded higher imbibition efficiency. This work systematically investigated the major effects of surfactant on oil mobilization during imbibition process, which can help for better understanding of chemical imbibition in carbonates. The findings will shed light on the selection of high performance imbibition agents for carbonate reservoirs.

大多数碳酸盐岩储层优选油湿性或中湿性。自发渗吸是提高原油产量的重要机制。针对高温高矿化度的油湿型碳酸盐岩油藏,研究了几种表面活性剂配方,以通过吸胀提高产油量,重点研究了表面活性剂在水相和油相中的界面张力(IFT)降低能力和表面活性剂在水相和油相中的分配,以及主要的润湿性改变效果。在95℃条件下,利用Amott细胞的自发渗吸来评价不同表面活性剂的采油潜力。采用IFT值为15.2 mN/m的高矿化度水和油湿型碳酸盐岩心进行了基本情况渗吸试验,其产油量为岩心原始饱和油的6.4%。将油水IFT降低到10°mN/m量级,使原油产量比基本情况增加4%。当IFT进一步降低到10 ~ 1 mN/m量级时,增产幅度达到10%。对于水湿岩心,在相同的IFT范围内,产油量增加了13%。当IFT降至10 - 2 mN/m时,采用油湿岩心的增产幅度可达17%,采用水湿岩心的增产幅度可达23%。当进一步降低IFT至10−3 mN/m的超低量级时,其产油量与使用IFT为10−2 mN/m的吸附剂时接近。对于无明显润湿性改变能力的表面活性剂,油相分子分数高、在岩石表面的吸附能力强的表面活性剂能从孔壁上去除更多的油,具有较高的吸油效率。系统研究了表面活性剂在吸胀过程中对原油动员的主要影响,有助于更好地理解碳酸盐岩的化学吸胀。这一发现将为碳酸盐岩储层选择高性能渗吸剂提供指导。
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引用次数: 0
Effects of model tear proteins and topical ophthalmic formulations on evaporation inhibition and biophysical property of model tear lipid nanofilm in vitro 模型泪液蛋白和局部眼用制剂对模型泪液脂质纳米膜体外蒸发抑制和生物物理性质的影响
Q3 Materials Science Pub Date : 2021-12-01 DOI: 10.1016/j.jciso.2021.100028
Meng C. Lin , Tatyana F. Svitova

Hypothesis

Biophysical property and water evaporation retardation through a lipid nanofilm can be altered by model tear protein and topical ophthalmic formulation.

Experiment

Evaporation rate and dynamic surface pressure were measured using a sessile drop technique. Water evaporations from 5 individual protein solutions, their mixture, and 6 ophthalmic formulations were quantified. Biophysical property and evaporation through model lipid nanofilms spread on model electrolyte solutions, tear protein solutions, and ophthalmic formulations were assessed.

Findings

Model lipid nanofilms spread on electrolyte solution reduced evaporative fluxes by 43–60%. Evaporative fluxes from individual protein solutions without lipids were 3–19% lower than from electrolytes solution. Evaporative fluxes through lipid nanofilms were decreased by the presence of albumin or lactoferrin in solutions but increased by lysozyme and mucin.

Evaporative fluxes from ophthalmic formulations were 10–43% lower than from electrolyte solution. Evaporations through lipid nanofilms spread on formulations were higher than through lipids on electrolyte solution. Model lipid nanofilms spread on Diquas appeared more rigid than on electrolyte solution but showed softening when spread on Refresh Mega-3.

Some proteins and ophthalmic formulations altered model lipid nanofilms evaporative barriers. Ophthalmic formulation induced changes in biophysical property of model lipid nanofilms in vitro may suggest possible tear film destabilization in vivo.

模型泪液蛋白和外用眼用制剂可以改变泪液纳米膜的生物物理性质和水分蒸发阻滞。实验采用固定式液滴法测量了蒸发速率和动态表面压力。对5种单独的蛋白质溶液及其混合物和6种眼科配方的水分蒸发进行了定量。通过模型脂质纳米膜在模型电解质溶液、泪液蛋白溶液和眼科配方上的扩散,评估了生物物理特性和蒸发。模型脂质纳米膜在电解质溶液上的扩散可使蒸发通量降低43-60%。不含脂的单个蛋白质溶液的蒸发通量比电解质溶液低3-19%。溶液中存在白蛋白或乳铁蛋白会降低脂质纳米膜的蒸发通量,但溶菌酶和粘蛋白会增加蒸发通量。眼科配方的蒸发通量比电解质溶液低10-43%。通过脂质纳米膜散布在配方上的蒸发量高于通过脂质在电解质溶液上的蒸发量。涂在Diquas上的脂质纳米膜比涂在电解质溶液上的脂质纳米膜更坚硬,但涂在Refresh Mega-3上的脂质纳米膜表现出软化。一些蛋白质和眼科配方改变了模型脂质纳米膜的蒸发屏障。眼用制剂在体外诱导模型脂质纳米膜生物物理特性的变化,可能提示体内泪膜不稳定。
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引用次数: 1
Comparison of thermoresponsive Diels-Alder linkers for the release of payloads from magnetic nanoparticles via hysteretic heating 通过滞后加热从磁性纳米颗粒释放有效载荷的热响应Diels-Alder连接体的比较
Q3 Materials Science Pub Date : 2021-12-01 DOI: 10.1016/j.jciso.2021.100034
Julien H. Arrizabalaga , Jonathan S. Casey , Jeffrey C. Becca , Lasse Jensen , Daniel J. Hayes

Investigation into the use of thermally reversible Diels-Alder chemistry coupled with magnetic iron oxide nanoparticles has grown over the last decade. This technology has been used for a variety of applications such as thermoresponsive materials, catalytic chemistry, and drug delivery systems. In this study, we evaluate two distinct thermally labile Diels-Alder linkers for the release of payloads from the surface of magnetic iron oxide nanoparticles. Density functional theory (DFT) computational predictions of the Gibbs free energy and enthalpy reaction barriers were performed and revealed a dramatic difference in reverse energy barriers between the two linkers. These thiophene-based cycloadducts were then synthesized, conjugated to the surface of iron oxide nanoparticles, and characterized by NMR and ESI-MS. The results of the modeling were confirmed when the functionalized nanoparticles were subjected to immersion heating and the payload release rates observed were in agreement with the DFT calculations. Similarly, AMF-RF hysteretic heating of the functionalized nanoparticles revealed payload release rates that correlated with the DFT calculations and the data from the heat immersion studies. Together, these results indicate that these distinct thermally labile Diels-Alder linkers can be used to fine-tune the kinetics of payload release from nanoparticles.

在过去的十年里,对热可逆Diels-Alder化学与磁性氧化铁纳米颗粒耦合使用的研究越来越多。该技术已被用于各种应用,如热敏材料、催化化学和药物输送系统。在这项研究中,我们评估了两种不同的热不稳定Diels-Alder连接剂从磁性氧化铁纳米颗粒表面释放有效载荷。密度泛函理论(DFT)计算预测了吉布斯自由能和焓反应势垒,并揭示了两种连接剂之间逆能势垒的显著差异。然后合成了这些噻吩基环加合物,并将其共轭到氧化铁纳米颗粒的表面,并用NMR和ESI-MS对其进行了表征。将功能化纳米粒子置于浸没加热条件下,模型结果得到了验证,所观察到的有效载荷释放率与DFT计算结果一致。同样,功能化纳米颗粒的AMF-RF滞后加热揭示了有效载荷释放率与DFT计算和热浸研究数据相关。总之,这些结果表明,这些不同的热不稳定Diels-Alder连接物可以用来微调纳米颗粒有效载荷释放的动力学。
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引用次数: 5
Pickering nanoemulsions: An overview of manufacturing processes, formulations, and applications 皮克林纳米乳液:制造工艺,配方和应用的概述
Q3 Materials Science Pub Date : 2021-12-01 DOI: 10.1016/j.jciso.2021.100036
Gaëlle Gauthier, Isabelle Capron

There is an increasing demand for emulsions with low viscosity, a large fraction of dispersed phase, high transparency, or long shelf life. Emulsions consisting of nanosized dispersed droplets meet these criteria, but conventional nanoemulsions require large quantities of surfactants, some of which are unwanted due to health and environmental concerns. Surfactants can then be replaced by solid particles, forming the so-called Pickering emulsions. Combining nanosized droplets and particle-stabilized emulsions leads to Pickering nanoemulsions. Since their first appearance in 2012, they have received increasing attention, but several points remain challenging; the choice of particles according to their origin, shape, sizes, and wetting properties and the process to produce drop sizes in the nano range. This review describes the recent advances in terms of manufacturing processes and destabilization mechanisms of Pickering nanoemulsions. It reports the particles used to stabilize the oil-water interface and strategies to improve their wetting properties, as well as examples of applications for the design of formulations in the pharmaceutics, food packaging, and enhanced oil recovery sectors.

人们对低粘度、分散相含量高、透明度高或保质期长的乳剂的需求越来越大。由纳米级分散液滴组成的乳液符合这些标准,但传统的纳米乳液需要大量的表面活性剂,由于健康和环境问题,其中一些是不需要的。然后,表面活性剂可以被固体颗粒取代,形成所谓的皮克林乳剂。将纳米液滴与颗粒稳定的乳剂相结合,形成了皮克林纳米乳剂。自2012年首次亮相以来,它们受到了越来越多的关注,但有几个问题仍然具有挑战性;根据颗粒的来源、形状、大小和润湿性能选择颗粒,并在纳米范围内生产液滴尺寸。本文综述了近年来在皮克林纳米乳的制备工艺和不稳定机理方面的研究进展。它报告了用于稳定油水界面的颗粒和改善其润湿性能的策略,以及在制药,食品包装和提高石油采收率部门的配方设计中的应用实例。
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引用次数: 17
Molten-salt defect engineering of TiO2(B) nanobelts for enhanced photocatalytic hydrogen evolution 增强光催化析氢的TiO2(B)纳米带熔盐缺陷工程
Q3 Materials Science Pub Date : 2021-12-01 DOI: 10.1016/j.jciso.2021.100031
Daijun Xie, Yingjie Wang, Han Yu, Xinran Yang, Shining Geng, Xiangfu Meng

Defect engineering has been proved to be an effective strategy to adjust the electronic structures and photocatalytic activities of semiconductor oxides. However, due to lack of convenient approach to construct defect, the effect of oxygen vacancy defect on photocatalytic hydrogen evolution has always been controversial. Herein, we proposed a facile molten-salt defect engineering (MSDE) strategy to introduce oxygen vacancies (Vos) defects in TiO2(B) nanobelt (TNB). By tuning the addition amount of NaBH4 during molten-salt calcination process, the concentration of surface oxygen vacancies can be effectively adjusted. As a result, the appropriate oxygen vacancies on TNB not only suppressed the recombination of photogenerated electrons and holes, but also raised the conduction band position of TNB, thereby increasing the reduction potential of photogenerated electrons. The as-prepared photocatalyst TNB-NaBH4-2 with optimal Vos concentration exhibited highly efficient photocatalytic hydrogen evolution performance at a rate of 3.2 ​mmol ​g−1h−1 under simulate solar light, nearly 1.85 times than that of pristine TNB. This work proposes a simple method for constructing moderate oxygen vacancies on metal oxides for enhancing photocatalytic hydrogen evolution.

缺陷工程已被证明是调整半导体氧化物的电子结构和光催化活性的有效策略。然而,由于缺乏简便的缺陷构建方法,氧空位缺陷对光催化析氢的影响一直存在争议。在此,我们提出了一种易熔盐缺陷工程(MSDE)策略,在TiO2(B)纳米带(TNB)中引入氧空位(Vos)缺陷。通过调整熔盐煅烧过程中NaBH4的加入量,可以有效地调节表面氧空位的浓度。因此,在TNB上适当的氧空位不仅抑制了光生电子与空穴的复合,而且提高了TNB的导带位置,从而增加了光生电子的还原电位。制备的最佳Vos浓度的光催化剂TNB- nabh4 -2在模拟太阳光下表现出高效的光催化析氢性能,速率为3.2 mmol g−1h−1,是原始TNB的1.85倍。本文提出了一种在金属氧化物上构建适度氧空位以增强光催化析氢的简单方法。
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