Abstract
The electrocatalytic ethylene glycol (EG) oxidation to value-added chemicals is highly desirable for profitable resource utilization, yet encounters a low yield rate and poor durability. Herein, a class of highly distorted PtPdTe nanosheets (PtPdTe-a) with modulated electronic states and oxophilicity is prepared by reconstructing layered PtPdTe dichalcogenide and delivers a record mass activity (11.78 A mgPt+Pd~(-1)) toward EG oxidation reaction with high glycolic acid (GA) Faradaic efficiency (96.7%). Mechanistic investigations reveal that PtPdTe-a features a strong p-d coupling effect for facilitating the formation and adsorption of hydroxyl adspecies to accelerate the oxidation of carbonyl intermediates, thereby avoiding over-oxidation and switching the pathway toward desired C2 direction. We further demonstrate the unprecedented stability of PtPdTe-a-based electrolyzer for over 1000 h (>150 mA cm~(-2)). The scale-up electrolyzer can achieve GA electrosynthesis with a record yield rate of 5.04 mmol cm~(-2) h~(-1) and a very high initial current density of over 800 mA cm~(-2) from the upgrading of PET. Our new strategy can produce 422.36 g of terephthalic acid, 904.08 g of Na_2SO_4, and 112.69 g of GA from 500 g of PET with a profit of about$880.23 ton~(-1) PET. Besides, PtPdTe-a is highly efficient for ethanol oxidation into acetic acid with excellent selectivity.
NETL
NSTL
Wiley