Wen Guan,Yunlei Zhang,Yao Chen,Jianchun Wu,Yu Cao,Yanan Wei,Pengwei Huo
Efficient nanoreactors for the catalytic oxidation of the key platform compound HMF to the high value-added chemical FDCA are highly desirable in the field of biomass transformation. Herein, hierarchical porous bowl-like nitrogen-doped carbon supported AuPd bimetallic (AuPd/pBN x C) nanoreactors were synthesized by the following steps: precipitation polymerization, carbonization, SiO 2 sphere removal, and sol curing. By changing the amount of nitrogen doping and removing the template, AuPd/pBN x C nanoreactors with a hierarchical porous structure and adjustable basicity were prepared. The alkaline sites of N x C carriers provided anchoring sites for metals and had a certain adsorption affinity for HMF and its intermediates. Theoretical calculations and adsorption experiments indicated that the doped nitrogen significantly enhanced the combining capacity between the HMF molecule and nanoreactors. The nanoreactor was used for the tandem oxidation of HMF to FDCA in water, and the highest FDCA yield of 97.6% could be obtained under optimum reaction conditions. The reaction process was evaluated by kinetics calculations, and the oxidation of FFCA to FDCA was confirmed as the rate-determining step. The regeneration experiments showed that the AuPd/pBN x C nanoreactors could be recycled and reused at least five times without an obvious loss in catalytic activity.
Linen Wu,Jie Gong,Lei Ge,Changcun Han,Siman Fang,Yongji Xin,Yujing Li,Yan Lu
In this study, novel AuPd bimetallic co-catalyst decorated Cd 0.5 Zn 0.5 S photocatalyst was successfully synthesized via an in-situ chemical deposition method . The physical as well as the photophysical properties of the as-obtained AuPd/Cd 0.5 Zn 0.5 S samples were characterized by X-ray diffractometry (XRD), Transmission electron microscope (TEM), UV–vis diffuse reflection spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS) and surface photovoltage spectroscopy (SPV). The AuPd bimetallic co-catalysts showed dramatic photo-generated charge separation efficiency in Cd 0.5 Zn 0.5 S sample, and thus significantly enhance the H 2 production activity under visible light irradiation. The AuPd/Cd 0.5 Zn 0.5 S sample with 0.5 wt% content had the highest catalytic activity , and the corresponding H 2 evolution rate is 3.65 mmol g −1 h −1 , which was about 12 times as that of pure Cd 0.5 Zn 0.5 S sample under visible light irradiation . The photocatalytic activity of the photocatalyst was stable even after 9 cycling photocatalytic experiments. A possible mechanism on the photocatalytic enhancement of AuPd NPs was systematically investigated, which can provide a novel concept for the synthesis of other desirable photocatalytic materials.
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