Abstract:
Single-atom catalysts (SACs) show expressively enhanced activity toward diverse reactions due to maximized atomic utilization of metal sites, while their facile, universal, and massive preparation remains a pronounced challenge. Here we report a facile strategy for the preparation of SACs by use of the inherent confined space between the template and silica walls in template-occupied mesoporous silica SBA-15 (TOS). Different transition metal precursors can be introduced into the confined space readily by grinding, and during succeeding calcination single atoms are constructed in the form of M-O-Si (M = Cu, Co, Ni, and Zn). In addition to the generality, the present strategy is easy to scale up and can allow the synthesis of 10 g of SACs in one pot through ball milling. The Cu SAC has been applied for CO2 cycloaddition of epichlorohydrin, and the activity is obviously higher than the counterpart prepared without confined space and various reported Cu-containing catalysts.
摘要:
单原子催化剂(SAC)由于金属位点的原子利用率最大化,对各种反应显示出明显增强的活性,虽然他们很容易,普遍,大规模的准备仍然是一个明显的挑战。在这里,我们报告了通过使用模板占据的介孔二氧化硅SBA-15(TOS)中模板和二氧化硅壁之间固有的有限空间来制备SAC的简便策略。不同的过渡金属前体可以很容易地通过研磨引入到有限的空间,在随后的煅烧过程中,单原子以M-O-Si(M=Cu,Co,Ni,和锌)。除了一般性,本策略易于扩大规模,并且可以通过球磨在一锅中合成10gSAC。CuSAC已用于表氯醇的CO2环加成,并且活性明显高于在没有受限空间的情况下制备的对应物和各种报道的含Cu催化剂。