Abstract

Through a facial immersion method, thiomolybdates [Mo₃S(S₂)₆]²⁻ and [Mo₂(S₂)₆]²⁻ clusters have been successfully anchored on SBA-15, and the loaded catalyst was characterized by various methods. The terminal/bridging sulfur atoms on the sulfide cluster have a strong tendency to combine with H atom and then transferred to the S atom of thiophene for hydrodesulfurization. The catalytic activity and desulfurization selectivity of the supported catalysts Mo₃S₁₃/SBA-15 and Mo₂S₁₂/SBA-15 were investigated at different temperature and different time. Direct hydrogenation of thiophene occurs presumably with the participation of –SH groups, produced from the opening of S–S bridges by hydrogen. And the desulfurization of thiophene occurs presumably with the breaking of C–S bond and formation of C-OH bond for the product is butanol. Mo₃S₁₃/SBA-15 and Mo₂S₁₂/SBA-15 display excellent catalytic performance. The conversion rate of thiophene is about 97% for Mo₃S₁₃/SBA-15 and 94% for Mo₂S₁₂/SBA-15, while the desulfurization selectivity is about 97% (Mo₂S₁₂/SBA-15) and 82% (Mo₃S₁₃/SBA-15).

摘要

通过面浸法，硫代钼酸盐[Mo ₃ S(S ₂ ) ₆ ] ^{2 -}和[Mo ₂ (S ₂ ) ₆ ] ^{2 -}簇已成功锚定在SBA-15上，并通过多种方法表征负载的催化剂. 硫化物簇上的末端/桥连硫原子有很强的与H原子结合的趋势，然后转移到噻吩的S原子上进行加氢脱硫。负载型催化剂Mo ₃ S ₁₃ /SBA-15和Mo ₂ S ₁₂的催化活性和脱硫选择性/SBA-15 在不同温度和不同时间进行了研究。噻吩的直接氢化可能发生在 -SH 基团的参与下，由氢打开 S-S 桥产生。噻吩的脱硫大概是随着 C-S 键的断裂和 C-OH 键的形成而发生的，产物是丁醇。Mo ₃ S ₁₃ /SBA-15 和Mo ₂ S ₁₂ /SBA-15 表现出优异的催化性能。Mo ₃ S ₁₃ /SBA-15的噻吩转化率约为97%，Mo ₂ S ₁₂ /SBA-15的转化率约为94%，脱硫选择性约为97%（Mo ₂ S ₁₂/SBA-15) 和 82% (Mo ₃ S ₁₃ /SBA-15)。