Aerosol assisted chemical vapour deposition (AACVD) of 2D TMDCs for aqueous pollutant degradation

“随着人们对水质和水资源短缺的担忧日益普遍，污水的处理变得越来越紧迫。因此，水媒污染物的催化降解是一个引起人们极大兴趣的研究领域。另一个研究驱动因素是联合国可持续发展目标，即向所有人提供清洁的水。因此，人们研究了许多不同的材料作为潜在的处理催化剂。有许多污染物会引起人们的关注，其中之一就是抗生素。四环素等抗生素广泛用于人类和兽药以及农业中的饲料添加剂，因此，环境水样中经常发现四环素含量很高，对环境和人类健康构成特殊和重大的风险，例如，产生新的耐抗生素细菌菌株。这激发了对从水系统中去除TC作为水处理策略一部分的方法的重要研究。二维（2D）过渡金属二硫化物已被研究作为环境相关反应的催化剂，包括制氢，污染物降解等，并显示出巨大的前景。如何以一种有效催化这些反应的形式最好地合成这些材料是一个难题。一种具有许多显著优点的方法是气溶胶辅助化学气相沉积（AACVD）。AACVD带来的主要好处是，它可以自然地在玻璃支架上产生薄而高表面积的涂层。高表面积对催化应用至关重要，而玻璃支架的高温稳定性和透明度使其易于集成到热/光催化操作中。AACVD已被用于生产二维过渡金属二硫化物，但迄今为止，二维过渡金属二硒化物和二碲化物被证明是难以捉摸的。初步数据表明，二维二硒化钼的合成已经实现，但需要更多的研究，以获得坚固，高质量的材料。此外，AACVD需要具有高热稳定性的衬底，例如硼硅酸盐玻璃，然而，如果使用导电玻璃（例如InSnO）等支撑，则可以实现这些支撑催化剂的大量令人兴奋的新应用。因此，该项目的第二部分将研究开发导电支撑的可能性，并评估它们在电催化反应中的作用。目前，这种方法对于传统的硼硅酸盐载体催化剂来说是不可能的。这个项目的目标是在合成和应用两个方向上走得更远。在合成过程中使用新的底物将允许更多种类型的催化剂被测试其降解这些有害污染物的功效。这样，这项工作的影响将得到最大限度的发挥。这项工作不仅会引起那些研究AACVD方法[6]和污染降解方法的人的兴趣，而且基材种类的增加将使AACVD方法向从事其他应用（例如，传感和电荷存储）的团体开放，这些团体目前由于基材的惰性性质而无法使用该方法，从而使我成为该领域的独立研究员。利用AACVD制备材料后，将进行对水性污染物的热、光催化和电催化降解。虽然最初的工作将使用易于追踪的染料化合物，如亚甲蓝，但工作将转向考虑降解更多的局部污染物，如四环素等抗生素。最后，将对真实世界的水样进行评估。”

"Treatment of polluted water is becoming increasingly urgent as concerns about water quality and scarcity become increasingly prevalent. Consequently, catalytic degradation of water-borne pollutants is a research area attracting significant interest. An additional research driver is the United Nations Sustainable Development Goal to provide clear water to all. Accordingly, many different materials have been investigated as potential treatment catalysts. There are many pollutants that can cause concern, one of which is antibiotics. Antibiotics such as tetracycline (TC) are extensively used in both human and veterinary medicine, as well as a feed additive in agriculture therefore, TC is often found at high levels in environmental water samples presenting a specific and significant environmental and human health risk e.g., the development of new antibiotic-resistant bacterial strains. This is motivating significant research into methodologies for removing TC from aqueous systems as part of water treatment strategies.Two-dimensional (2D) transition metal dichalcogenides have been investigated as catalysts for environmentally relevant reactions including hydrogen generation, pollutant degradation etc. and show significant promise. The issue of how best to synthesise these materials in a form that is effective for catalysing these reactions is a difficult one. One method that offers many significant advantages is aerosol-assisted chemical vapour deposition (AACVD). The principal benefits that AACVD brings is that it naturally yields materials as thin, high surface area coatings on glass supports. High surface area is pivotal for catalytic applications, whilst the high temperature stability and transparency of the glass supports enable facile integration into thermal/photocatalytic operations. AACVD has been utilised to produce 2D transition metal disulphides but to date 2D transition metal diselenides and ditellurides have proved elusive. Preliminary data indicates that the synthesis of 2D molybdenum diselenide has been achieved but more investigation is needed to obtain robust, high-quality materials. Additionally, AACVD requires substrates with high thermal stability, such as borosilicate glass, however a plethora of exciting new applications for these supported catalysts could be realised if supports such as conductive glasses (e.g., InSnO) were utilised. Accordingly, a second strand of this project will investigate the possibility of developing conducting supports and assessing them in electro-catalytic reactions. Currently such an approach is just not possible with conventional borosilicate-supported catalysts.This project aims to go further in both the synthetic and applications focussed directions. Utilising novel substrates for the synthesis process will allow for a wider variety of types of catalysis to be tested for their efficacy in degrading these damaging pollutants. In this way the impacts of this work will be maximised. Not only will the work be of interest to those researching the AACVD method [6] and pollution degradation methods but the increased variety of substrates will open up the AACVD method to groups working on other applications (e.g., sensing and charge storage) who are currently prevented from utilising this method due to the inert nature of the substrates thus establishing me as an independent researcher in this field. Once the materials have been prepared using AACVD, the thermal, photocatalytic and electrocatalytic degradation of waterborne pollutants will be performed. Whilst initial work will be done using easily traceable dye compounds such as methylene blue, work will then move to considering degrading more topical pollutants such as antibiotics like tetracycline. Finally, real-world water samples will be assessed."