Z-scheme heterojunction

z - 方案异质结
  • 文章类型: Journal Article
    在这项研究中,随后通过微波辅助水热技术制备了氧化铜(CuO),将CuO原位生长到不同稀有金属化合物上,制备Z型异质结,以提高水环境中四环素(TC)的降解效率。各种表征证明了所有复合材料的成功合成,形成紧密的异质结界面,其中,核壳结构ZnIn2S4@CuO表现出优异的光催化降解能力。研究结果表明,ZnIn2S4@CuO在水环境中对TC(50mg/L)的降解效率达到95.8%,降解速率分别是CuO和ZnIn2S4的2.41倍和12.93倍,分别,原因是由于ZnIn2S4的引入,Z-scheme异质结结构和内部电场(IEF)的构建和形成,以扩大光催化剂的可见光响应范围,提高电子-空穴分离效率,增强电荷转移。此外,ZnIn2S4@CuO-2具有良好的稳定性和重现性,五个周期后没有明显的活性损失。最后,通过结合使用高分辨率质谱(HR-MC)和前沿电子密度(FED)研究了自由基对TC的精确攻击位置,并提供了合理的降解途径。这项研究的结果提供了一种新的可行方法,可以克服常规光催化材料在有限的可见光吸收范围和快速的载流子复合速率方面的局限性,在污水净化领域具有广阔的应用前景。
    In this study, copper oxide (CuO) was prepared by the microwave-assisted hydrothermal technique subsequently, CuO was grown in situ onto different rare metal compounds to prepare Z-scheme heterojunctions to improve the degradation efficiency of tetracycline (TC) in water environments. Various characterization proved the successful synthesis of all composite materials, and the formation of tight heterojunction interfaces, among which, the core-shell structure ZnIn2S4@CuO exhibited excellent photocatalytic degradation capability. Research results indicated that the degradation efficiency of ZnIn2S4@CuO for TC (50 mg/L) in the water environment reached 95.8 %, and the degradation rate is 2.41 times and 12.93 times that of CuO and ZnIn2S4 alone, respectively, the reason is because of the introduction of ZnIn2S4, Z-scheme heterojunction structures and internal electric field (IEF) is constructed and formed to extend the visible light response range of photocatalysts to improve electron-hole separation efficiency, and enhance charge transfer. In addition, ZnIn2S4@CuO-2 exhibited good stability and reproducibility, with no significant loss of activity after five cycles. Finally, the precise locations of free radical attack on TC were investigated by the combined use of high-resolution mass spectrometry (HR-MC) and frontier electron densities (FEDs), and a reasonable degradation pathway was provided. The results of this research provide a new and viable approach to overcome the limitations of conventional photocatalytic materials in terms of limited visible light absorption range and fast carrier recombination rates, which offers promising prospects for a wide range of applications in the field of wastewater purification.
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  • 文章类型: Journal Article
    电子-空穴对的有效分离在优化跨不同催化和光电系统的光生载流子功能方面仍然至关重要。这项研究提出了一种新型的中空直接Z-方案光催化剂的制造,ZnO/TiO2。全面的分析包括各种技术,如紫外可见光谱(UV-Vis),X射线衍射(XRD)透射电子显微镜(TEM),傅里叶变换红外光谱(FT-IR),热重分析(TGA),和能量色散X射线光谱(EDX)为ZnO/TiO2异质结催化剂的复杂材料特性提供了详细的见解。研究结果表明,锐钛矿型TiO2和纤锌矿型ZnO相共存,每个都在纳米复合材料(NC)结构中保留不同的属性。研究表明,在紫外光照射下,ZnO/TiO2-NCs分解亚甲基蓝和吖啶橙的光催化效果。与它们的潜在结构相关。这些染料的降解增强是由于在ZnO和TiO2之间建立了直接的Z方案异质结。使用量子ESPRESSO采用密度泛函理论(DFT),本研究分析了相图和能带结构,阐明电子性质和结构相关性。该研究表征了ZnO/TiO2复合材料,通过紫外可见光谱显示3.1-3.3eV的带隙,并通过XRD分析确认其形成没有杂质相。TEM和EDX显示出均匀的元素分散(Zn:27%,Ti:29.62%,C:5.03%,O:38.35%)。使用DFT的计算分析表明稳定相随着温度的升高而减少。观察到增强的染料降解(MB:88.9%,AO:84%),除了显著的抗菌活性。我们预测,未来的研究将集中在通过表面改性扩大生产和光催化活性的发展上,同时揭示了在水处理和抗菌应用中多功能使用的机械见解和环境适用性,导致该领域的进一步发展。
    Efficient separation of electron-hole pairs remains pivotal in optimizing photogenerated carrier functionality across diverse catalytic and optoelectronic systems. This study presents the fabrication of a novel hollow direct Z-scheme photocatalyst, ZnO/TiO2. A thorough analysis encompassing various techniques such as Ultraviolet-Visible Spectroscopy (UV-Vis), X-ray Diffraction (XRD), Transmission electron Microscopy (TEM), Fourier Transform Infrared Spectroscopy (FT-IR), Thermogravimetric Analysis (TGA), and Energy-Dispersive X-ray Spectroscopy (EDX) provided detailed insights into the complex material characteristics of the ZnO/TiO2 heterojunction catalyst. The findings revealed coexisting anatase TiO2 and wurtzite ZnO phases, each retaining distinct attributes within the nanocomposites (NCs) structure. The study showcased the photocatalytic efficacy of ZnO/TiO2-NCs in decomposing Methylene Blue and Acridine Orange under UV irradiation, correlated with their underlying structures. Enhanced degradation of these dyes resulted from the establishment of a direct Z-scheme heterojunction between ZnO and TiO2. Employing Density Functional Theory (DFT) using Quantum ESPRESSO, this research analyzed phase diagrams and band structures, elucidating electronic properties and structural correlations. The study characterized a ZnO/TiO2 composite, revealing a band gap of 3.1-3.3 eV through UV-Visible spectroscopy and confirming its formation without impurity phases via XRD analysis. TEM and EDX showed uniform element dispersion (Zn: 27%, Ti: 29.62%, C: 5.03%, O: 38.35%). Computational analysis using DFT indicated a reduction in stable phases with increasing temperature. Enhanced dye degradation was observed (MB: 88.9%, AO: 84%), alongside significant antibacterial activity. In the future we predict that research will focus on development of scaled up production and photocatalytic activity through surface modification, while unveiling mechanistic insights and environmental applicability for multifunctional use in water treatment and antibacterial applications, leading to further advancement of the field.
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  • 文章类型: Journal Article
    对于这项工作,我们使用n型Bi2WO6和p型PhC2Cu通过简化的超声搅拌技术配制了直接Z方案Bi2WO6/PhC2Cu(PCBW)光催化剂。最佳的0.6PCBW复合材料在低功率蓝光LED灯下具有快速光降解2,4,6-TCP的能力(在120分钟内达到98.6%),分别比原始PhC2Cu和Bi2WO6快8.53倍和12.53倍。此外,电子自旋共振(ESR),时间分辨PL光谱,定量ROS测试表明,PCBW增强了光电载流子的分离能力。它也更容易与水中的溶解氧结合以产生活性氧(ROS)。其中,PCBW在一小时内产生·O2-的能力是纯PhC2Cu的12.07倍。此外,PCBW的H2O2形成速率和表观量子效率是PhC2Cu的10.73倍,表明PCBW不仅具有优异的光催化性能,而且还具有突出的ROS生产能力。此外,Ag光沉积,利用原位X射线光电子能谱(XPS)和密度泛函理论(DFT)计算来确定PCBW中的光生电子迁移路径,系统地证实了Z方案异质结的成功形成。最后,基于中间产品,提出了三种潜在的2,4,6-TCP降解途径。
    For this work, we employed n-type Bi2WO6 and p-type PhC2Cu to formulate a direct Z-scheme Bi2WO6/PhC2Cu (PCBW) photocatalyst via simplified ultrasonic stirring technique. An optimal 0.6PCBW composite exhibited the capacity to rapidly photodegrade 2,4,6-TCP (98.6% in 120 min) under low-power blue LED light, which was 8.53 times and 12.53 times faster than for pristine PhC2Cu and Bi2WO6, respectively. Moreover, electron spin resonance (ESR), time-resolved PL spectra, and quantitative ROS tests indicated that the PCBW enhanced the separation capacity of photocarriers. It also more readily associated with dissolved oxygen in water to generate reactive oxygen species (ROS). Among them, the ability of PCBW to produce ·O2- in one hour was 12.07 times faster than for pure PhC2Cu. In addition, the H2O2 formation rate and apparent quantum efficiency of PCBW are 10.73 times that of PhC2Cu, which indicates that PCBW not only has excellent photocatalytic performance, but also has outstanding ROS production ability. Furthermore, Ag photodeposition, in situ X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations were utilized to determine the photogenerated electron migration paths in the PCBW, which systematically confirmed that Z-scheme heterojunction were successfully formed. Finally, based on the intermediate products, three potential 2,4,6-TCP degradation pathways were proposed.
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  • 文章类型: Journal Article
    Removal of antibiotics from aqueous solutions by photocatalysis is an advanced technology for environmental remediation. Herein, we have fabricated a series of AgX (X = I, Br)/CuBi2O4 composites through an in-situ precipitation method. The photocatalytic activity of the obtained photocatalysts was measured by the degradation of tetracycline (TC) under visible light irradiation (λ > 420 nm). All the AgX (X = I, Br)/CuBi2O4 composites exhibit much higher photocatalytic activity than that of pure CuBi2O4. The enhanced photocatalytic activity is mainly attributed to the efficient interfacial charge separation and migration in the AgX (X = I, Br)/CuBi2O4 heterojunctions. Meanwhile, AgX (X = I, Br)/CuBi2O4 heterojunctions display excellent photocatalytic stability, and the photocatalytic degradation rates were not obvious decreased even after five successive cycles. Based on the energy band structure, the radicals trapping and electronic spin resonance (ESR) experiments, the Z-scheme mechanism of AgBr/CuBi2O4 and type II mechanism of AgI/CuBi2O4 heterojunction photocatalysts were tentatively discussed, respectively.
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