Akopyan Argam V, Mnatsakanyan Raman A, Eseva Ekaterina A, Davtyan David A, Polikarpova Polina D, Lukashov Maxim O, Levin Ivan S, Cherednichenko Kirill A, Anisimov Alexander V, Terzyan Anna M, Agoyan Artur M, Karakhanov Eduard A
Chemistry Department, Lomonosov Moscow State University, Leninskie gory, 1/3, Moscow 119234, Russia.
A. B. Nalbandyan Institute of Chemical Physics National Academy of Sciences of Armenia, Yerevan 0014, Armenia.
ACS Omega. 2022 Apr 1;7(14):11788-11798. doi: 10.1021/acsomega.1c06969. eCollection 2022 Apr 12.
Herein, we present a new type of high-performance catalyst for aerobic oxidation of organosulfur compounds based on tungsten carbide. The synthesis of tungsten carbide was performed via microwave irradiation of the precursors, which makes it possible to obtain a catalyst in just 15 min. The synthesized catalyst was investigated by a variety of physicochemical methods: X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, electron microscopy, and N adsorption/desorption. It was shown that active centers containing tungsten in the transition oxidation state (+4) play a key role in the activation of oxygen. The main factors influencing the conversion of dibenzothiophene (DBT) were investigated. It should be noted that 100% conversion of DBT can be achieved under relatively mild conditions: 120 °C, 3 h, 6 bar, and 0.5% wt catalyst. The catalyst retained its activity for at least six oxidation/regeneration cycles. The simplicity and speed of synthesis of the proposed catalyst in combination with its high activity and stability open broad prospects for its further use both for oxidative desulfurization and for other reactions of aerobic oxidation of organic substrates.
在此，我们展示了一种新型的基于碳化钨的用于有机硫化合物有氧氧化的高性能催化剂。碳化钨的合成通过对前驱体进行微波辐射来进行，这使得在仅15分钟内就能获得一种催化剂成为可能。通过多种物理化学方法对合成的催化剂进行了研究：X射线衍射、X射线光电子能谱、拉曼光谱、电子显微镜以及N吸附/脱附。结果表明，含有处于过渡氧化态（+4）的钨的活性中心在氧的活化中起关键作用。研究了影响二苯并噻吩（DBT）转化的主要因素。应当指出的是，在相对温和的条件下（120℃、3小时、6巴和0.5%重量的催化剂）可以实现DBT的100%转化。该催化剂在至少六个氧化/再生循环中保持其活性。所提出的催化剂合成的简便性和速度，连同其高活性和稳定性，为其在氧化脱硫以及有机底物的其他有氧氧化反应中的进一步应用开辟了广阔前景。
