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

“随着人们对水质和稀缺性的担忧日益普遍，受污染的水的处理变得越来越紧迫。因此，水中污染物的催化降解是一个备受关注的研究领域。另一个研究驱动力是联合国可持续发展目标，即向所有人提供清洁水。因此，许多不同的材料被研究作为潜在的处理催化剂。有许多污染物可能会引起人们的关注，抗生素就是其中之一。四环素(TC)等抗生素在人类和兽医中被广泛使用，也是农业中的饲料添加剂，因此，在环境水样中经常发现TC含量高，对环境和人类健康构成特定和重大的风险，例如开发新的抗药性细菌菌株。作为水处理策略的一部分，这激发了对从水系统中去除TC的方法的重要研究。二维(2D)过渡金属二卤代化合物已被用作环境相关反应的催化剂，包括氢气生成、污染物降解等，并显示出巨大的前景。如何以一种有效地催化这些反应的形式来合成这些材料是一个困难的问题。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，它自然会在玻璃支撑物上产生薄的、高表面积的涂层。高比表面积是催化应用的关键，而玻璃载体的高温稳定性和透明度使其能够轻松地集成到热/光催化操作中。AACVD已被用于生产2D过渡金属二硫化物，但到目前为止，2D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，二硫化钼的合成已经实现，但要获得坚固的、高质量的材料，还需要进行更多的研究。此外，AACVD需要具有高热稳定性的衬底，如硼硅酸盐玻璃，然而，如果使用导电玻璃(如InSnO)等载体，这些负载型催化剂将实现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载体并在电催化反应中对其进行评估的可能性。目前，这种方法对于传统的以硼硅酸盐为载体的催化剂来说是不可能的。本项目的目标是在合成和应用两个方向上更进一步。在合成过程中使用新的底物将允许测试更多类型的催化剂在降解这些有害污染物方面的有效性。这样，这项工作的影响将最大化。不仅研究AACVD方法[6]和污染降解方法的人会对这项工作感兴趣，而且基材种类的增加将使从事其他应用(例如，传感和电荷存储)的小组可以使用AACVD方法，这些小组目前由于基材的惰性性质而无法使用这种方法，从而确立了我作为该领域的独立研究员的地位。一旦利用AACVD制备了这些材料，就可以对水中污染物进行热、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，如亚甲基蓝，然后工作将转移到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."