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Highly Selective Conversion of Glycerol to Formic Acid over a Synergistic Au/Phosphotungstic Acid Catalyst under Nanoconfinement
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-02-24 , DOI: 10.1021/acssuschemeng.0c09057
Yi-Tzu Lin, Jingling Yang, Chung-Yuan Mou

Converting surplus glycerol into the hydrogen storage material, formic acid, can meet the increasing energy demand, yet its commercial production is hindered by the low efficiency. Herein, a nano-confined catalytic system with multiple active sites that consists of ultrasmall Au nanoparticles (NPs) and highly dispersed phosphotungstic acid (PTA) within the nanochannels of mesoporous silica nanoparticles (Au-PTA/MSN) was demonstrated to directly convert glycerol to formic acid in a one-step operation under the mild condition with a selectivity of up to 79.2%. The time-course experiment revealed that such a one-pot process involves synergistic catalysis from glycerol to a triose, followed by the breakdown of the C–C bond of trioses into glycolic acid and formic acid, as well as further oxidative cleavage of glycolic acid to formic acid, which eventually contributed to the highly selective formic acid production. Characterizations showed that the nano-confined Au-PTA/MSN catalytic system incorporated the catalytic actions of Au NPs and phosphotungstic acid in one operation, thus offering a high activity for converting glycerol to formic acid.

中文翻译:

纳米约束下协同金/磷钨酸催化剂上甘油的高选择性转化为甲酸

将多余的甘油转化为储氢材料甲酸可以满足不断增长的能源需求,但是其低效率却阻碍了其商业化生产。本文中,在介孔二氧化硅纳米颗粒(Au-PTA / MSN)的纳米通道内,由超小金纳米颗粒(NPs)和高度分散的磷钨酸(PTA)组成的具有多个活性位点的纳米受限催化体系被证明可直接将甘油转化为在温和条件下一步一步操作生成甲酸,选择性高达79.2%。时程实验表明,这种一锅法涉及从甘油到三糖的协同催化作用,然后将三糖的C–C键分解为乙醇酸和甲酸,以及乙醇酸的进一步氧化裂解甲酸 最终促进了高选择性甲酸的生产。表征表明,纳米受限的Au-PTA / MSN催化体系在一次操作中结合了Au NPs和磷钨酸的催化作用,因此具有将甘油转化为甲酸的高活性。
更新日期:2021-03-08
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