Wu Shilin, Zhao Haijun, Dong Fang, Ling Weitong, Tang Zhicheng, Zhang Jiyi
State Key Laboratory for Oxo Synthesis and Selective Oxidation, and National Engineering Research Center for Fine Petrochemical Intermediates, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, P. R. China.
School of Petroleum and Chemical, Lanzhou University of Technology, Lanzhou 730050, P. R. China.
ACS Appl Mater Interfaces. 2021 Jan 20;13(2):2610-2621. doi: 10.1021/acsami.0c18636. Epub 2021 Jan 7.
In this paper, a simple method to enhance the HO resistance of Ru/TiCeO catalysts for -DCB catalytic combustion by constructing superhydrophobic coating of phenyltriethoxysilane (PhTES) was proposed. The effect of PhTES content on the pore structure, specific surface area, HO resistance, contact angle (CA) value, and catalytic activity of the catalyst was studied. When water was added, the pristine Ru/TiCeO catalytic activity decreased by about 26%, while the Ru/TiCeO-16Ph activity hardly decreased. According to the analysis results of XRD, FT-IR, SEM, and CA, PhTES was closely coated on the surface of Ru/TiCeO to produce a more hydrophobic surface. The Ru/TiCeO-16Ph catalyst had strong hydrophobicity, and the contact angle was 159.8°, which not only significantly enhanced the water resistance and self-cleaning activity but also showed a good elimination temperature ( = 341 °C) for the -DCB. The enhanced water resistance of Ru/TiCeO-XPh catalysts resulted from the reduction of the active centers consumed (water occupying oxygen vacancy sites). The reaction mechanism of the Ru/TiCeO-16Ph catalyst based on surface oxygen species and the Deacon reaction was proposed. This method provided new idea for the design of a new water-resistant composite catalyst and promoted the practical application of the composite catalyst in the catalytic oxidation of -DCB.
本文提出了一种通过构建苯基三乙氧基硅烷（PhTES）超疏水涂层来提高Ru/TiCeO催化剂对二氯苯（-DCB）催化燃烧的抗水性的简单方法。研究了PhTES含量对催化剂的孔结构、比表面积、抗水性、接触角（CA）值和催化活性的影响。加入水后，原始Ru/TiCeO的催化活性下降了约26%，而Ru/TiCeO-16Ph的活性几乎没有下降。根据XRD、FT-IR、SEM和CA的分析结果，PhTES紧密包覆在Ru/TiCeO表面，形成了更疏水的表面。Ru/TiCeO-16Ph催化剂具有很强的疏水性，接触角为159.8°，不仅显著提高了耐水性和自清洁活性，而且对二氯苯显示出良好的消除温度（=341°C）。Ru/TiCeO-XPh催化剂耐水性增强的原因是消耗的活性中心减少（水占据氧空位）。提出了基于表面氧物种和迪肯反应的Ru/TiCeO-16Ph催化剂的反应机理。该方法为新型耐水复合催化剂的设计提供了新思路，促进了复合催化剂在二氯苯催化氧化中的实际应用。
