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Glycine photosynthesis via C-N coupling of waste plastic and nitrate over diatomic Pd-B catalyst
Zongyang Ya1,2, Mei Li3, Donglong Fu1
1School of Chemical Engineering & Technology, Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University; Collaborative Innovation Center for Chemical Science & Engineering, Tianjin, China.
Abstract:
Photocatalytic C-N coupling offers a promising approach for the sustainable production of amino acids, but the uncontrolled coupling pathway of reaction intermediates limits yield and selectivity. This paper describes a Pd-B diatomic catalyst that can selectively catalyze the photosynthesis of glycine via C-N coupling reaction between waste poly(ethylene terephthalate)-derived ethylene glycol and nitrate, achieving a glycine yield of 2.9 mmol gcat-1 h-1 with a selectivity of 92%. Mechanistic investigations reveal that ethylene glycol is photo-oxidized to glycolaldehyde at the hole-rich B site, while nitrate is photo-reduced to NH4+/NH3 at the electron-rich Pd site. Subsequently, glycolaldehyde undergoes C-N coupling with NH4+/NH3, and further photo-oxidized to form glycine. The Pd-B diatomic site more effectively stabilizes the glycolaldehyde intermediate, resulting in a more favorable C-N coupling pathway than metal oxide and enhancing glycine selectivity. Thus, we show a catalytic system for selective glycine photosynthesis by precisely regulating the reaction pathways of key intermediates.
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