Journal of Materials Science & Technology ( IF 11.2 ) Pub Date : 2023-03-05 , DOI: 10.1016/j.jmst.2022.12.057 Raqiqa Tur Rasool , Ghulam Abbas Ashraf , Mohsin Pasha , Muhammad Farooq Saleem , Djamel Ghernaout , Mohammed M. Fadhali , Hai Guo
In this work, we developed a promising photocatalyst in CsPbBr3 quantum dots (QDs) because of their exceptional optoelectronic characteristics. However, QDs applications in the field of photocatalysis were mainly hampered by their poor stability and insufficient charge transfer efficiency. Herein, a novel and efficient MnSnO2@CsPbBr3 (MSO@QDs) nanocomposite was first time effectively designed and synthesized by a wet impregnation method for peroxymonosulfate (PMS) activation under the light. The newly generated interface phase of QDs between MnSnO2 (MSO) showed great potential to improve light absorption, leading to effective separation and transfer of photoelectron-hole pairs. This novel nanocomposite MSO@QDs showed great Flurbiprofen (FL) removal efficiency under the PMS/Light system. It should be noted that this nanocomposite removed 85.74% of FL in just 70 min, which was almost 1.11 and 2.51 times greater than using pure QDs and pure MSO, respectively. Based on thorough measurements of structural analysis, Brunauer-Emmett-Teller (BET), UV-vis spectra, electrochemical impedance spectroscopy (EIS), transient photocurrent response, and a potential mechanism for organic pollutants degradation over MSO@QDs nanocomposite was envisioned. The principal reactive species of photoinduced holes (h+), i.e. O2˙−, SO4˙−, ˙OH, and non-radical (1O2) were characterized via scavengers’ technique and electron paramagnetic resonance (EPR) measurements. The highest photocatalytic performance for the removal of MO, MB, and IBU was demonstrated by MSO@QDs nanocomposite/PMS, revealing their excellent ability to remove organic pollutants through photo-oxidation. Furthermore, the developed nanocomposite exhibited good stability in an aqueous medium. According to computational investigation using the density functional theory (DFT) method, the site's higher Fukui index f 0 value corresponds to a greater propensity to be attacked by reactive species. This work offers a fresh perspective on developing further high-efficiency, low-cost photocatalysts for wastewater treatment.
中文翻译:
纳米级 MnSnO2@CsPbBr3 量子点异质结构光催化剂作为过一硫酸盐高效降解有机污染物;DFT计算
在这项工作中,我们开发了一种很有前途的 CsPbBr 3量子点 (QD) 光催化剂,因为它们具有出色的光电特性。然而,量子点在光催化领域的应用主要受到稳定性差和电荷转移效率不足的制约。在此,首次通过湿浸渍法有效设计和合成了一种新型高效的 MnSnO 2 @CsPbBr 3 (MSO@QDs) 纳米复合材料,用于光下过氧单硫酸盐 (PMS) 活化。MnSnO 2之间新生成的量子点界面相(MSO) 显示出提高光吸收的巨大潜力,从而导致光电子-空穴对的有效分离和转移。这种新型纳米复合材料 MSO@QD 在 PMS/Light 系统下显示出出色的氟比洛芬 (FL) 去除效率。应该注意的是,这种纳米复合材料仅在 70 分钟内就去除了 85.74% 的 FL,分别比使用纯 QD 和纯 MSO 高出近 1.11 倍和 2.51 倍。基于对结构分析的全面测量,设想了 Brunauer-Emmett-Teller (BET)、紫外-可见光谱、电化学阻抗谱 (EIS)、瞬态光电流响应以及 MSO@QDs 纳米复合材料降解有机污染物的潜在机制。光致空穴的主要活性物质(h + ),即O 2 ˙ −, SO 4 ˙ − , ˙ OH 和非自由基 ( 1 O 2 ) 通过清除剂技术和电子顺磁共振 (EPR) 测量来表征。MSO@QDs 纳米复合材料/PMS 展示了去除 MO、MB 和 IBU 的最高光催化性能,揭示了它们通过光氧化去除有机污染物的出色能力。此外,所开发的纳米复合材料在水性介质中表现出良好的稳定性。根据使用密度泛函理论 (DFT) 方法的计算调查,该站点的较高福井指数f 0值对应于被活性物质攻击的更大倾向。这项工作为进一步开发用于废水处理的高效、低成本光催化剂提供了新的视角。