Aqueous phase reforming of biomass-derived acids over a highly dispersed platinum catalyst.

Abstract

Aqueous-phase reforming (APR) of biomass-derived effluent is an attractive route to renewable hydrogen, yet real, acid-rich streams reform poorly and rapidly deactivate the commercial catalysts. Herein, we propose a rational catalyst design strategy involving Pt atoms anchored on nitrogen-doped carbon and interfaced with ZnO domains. The developed catalyst (HD-PtN/ZnO/C) features highly dispersed Pt as C-C activation sites; Lewis-acidic ZnO to enhance the inner water-gas shift (WGS) reaction; N-induced locally alkaline microenvironment that facilitates the adsorption and activation of acidic substrates, successfully establishing a synergistic system. The design enables nearly a complete conversion of the mixed aliphatic acids effluent, corresponding to TOFH2 as 5288 h-1, 3.4 times higher than that from the commercial Pt/C catalyst. N-doping not only facilitates an excellent hydrogen yield (61.3 mmolH2 gTOC-1) but also contributes significantly to the stability of Pt and ZnO species. This catalyst represents a breakthrough by simultaneously maintaining high APR activity and catalyst structural stability in a real acidic effluent system. Sustainability tests showed activity can be fully recovered by a mild 300 °C calcination, enabling at least five cycles. This work paves the way for an efficient and durable hydrogen production from acidic industrial wastewater and expands the applications of single-atom catalysts.