Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2017-04-15 , DOI: 10.1016/j.apcatb.2017.04.011 Zichun Wang , Jun Huang , Rose Amal , Yijiao Jiang
Solid-state 13C high-power proton decoupling (HPDEC), cross-polarization (CP), and 2-dimensional (2D) 13C-13C homonuclear correlation NMR techniques were used to study the adsorption of acetaldehyde on the flame-made fluorinated TiO2 (F-TiO2) catalyst, subsequent photocatalytic oxidation, and complete photo-decomposition at the presence of oxygen under UV light irradiation. Crotonaldehyde is formed via the acid-catalyzed aldol condensation through the adsorption of acetaldehyde on the F-TiO2 catalyst at room temperature without light illumination. At the presence of molecular oxygen as an electron acceptor, surface bonded acetaldehyde and crotonaldehyde are completely oxidized by the transient holes in the oxygen framework generated by UV light irradiation. This work provides clear evidence for the formation of crotonaldehyde, acetic acid, and formic acid, along with acetate and formate complexes. The identified surfaces complexes participate actively in the photocatalytic oxidation and do not play a significant role in the poisoning of the active sites, at least in such concentrations. The reaction pathways are therefore established.
中文翻译:
在火焰制F-的TiO乙醛的光催化氧化的固体NMR研究2催化剂
固态13 C大功率质子去耦(HPDEC),交叉极化(CP)和二维(2D)13 C- 13 C同核相关NMR技术用于研究乙醛在火焰制成的材料上的吸附氟化的TiO 2(F-TiO 2)催化剂,随后进行光催化氧化,并在紫外光照射下在氧气存在下完成光分解。巴豆醛是通过酸催化的醛醇缩合反应通过乙醛在F-TiO 2上的吸附而形成的。催化剂在室温下不需光照。在分子氧作为电子受体的存在下,表面键合的乙醛和巴豆醛被紫外线辐射产生的氧骨架中的瞬态孔完全氧化。这项工作为巴豆醛,乙酸和甲酸以及乙酸盐和甲酸络合物的形成提供了明确的证据。至少在这样的浓度下,所鉴定的表面复合物积极地参与光催化氧化并且在活性位点的中毒中不发挥显著作用。因此建立了反应途径。