电合成
甘油酸
介孔材料
甘油
材料科学
稀土
金属
核化学
催化作用
化学
有机化学
冶金
电极
电化学
物理化学
作者
Dongping Fan,Lizhi Sun,Rui Yuan,Zhen‐An Qiao,Shunai Che,Ben Liu
摘要
ABSTRACT The electrocatalytic glycerol oxidation reaction (GOR) offers a promising route to synthesize high value-added chemicals, for example glyceric acid (GLA), in an economic and sustainable manner. Despite some great achievements, GLA selectivity and yield rate of GOR electrocatalysis remain unsatisfactory due to uncontrollable C–C bond cleavage of glycerol (for unfavorable C1 and C2 products). In this work, rare-earth-metal (REM)-alloyed PtPb mesoporous nanosheets are demonstrated as novel yet high-performance electrocatalysts for selective GLA electrosynthesis from GOR. The best electrocatalyst—PtPbY MNSs—delivers outstanding performance for GLA electrosynthesis from glycerol, including superior selectivity of 72.5% and recordable yield rate of 656 μmol mgcat−1 h−1, surpassing most electrocatalysts reported in the literature. Meanwhile, PtPbY MNSs hold impressive stability of GOR electrocatalysis, retaining the high GLA selectivity and yield rate for reaching 15 cycles. Superior performance, revealed by in situ characterizations and density functional theory calculations, is ascribed to structural and compositional synergies that kinetically promote the reactivity of glycerol and accelerate the desorption of GLA while minimizing undesirable C–C bond cleavage. This work elaborates a powerful alternative for selective electrosynthesis of high-value-added chemicals from waste alcohols by optimizing chemisorption properties of mesoporous metals by REM alloys.
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