Aqueous phase reforming of methanol for hydrogen production over highly-dispersed PtLa/CeO2 catalyst prepared by photochemical reduction method

制氢 甲醇 催化作用 离解(化学) 水溶液 吸附 水煤气变换反应 化学 无机化学 光化学 双水相体系 产量(工程) 氧气 材料科学 有机化学 冶金
作者
Yongheng Lu,Chao Wang,Xianglong Luo,Riyang Shu,Libin Lei,Jianping Liu,Zhipeng Tian,Yuhe Liao,Ying Chen
出处
期刊:International Journal of Hydrogen Energy [Elsevier BV]
卷期号:62: 1054-1066 被引量:23
标识
DOI:10.1016/j.ijhydene.2024.03.164
摘要

Hydrogen production by catalytic aqueous phase reforming (APR) of biomass oxygenated derivatives in relatively mild conditions is a promising way to produce hydrogen . In this work, Pt/CeO 2 -HT, Pt/La–CeO 2 -HT and PtLa/CeO 2 catalysts were synthesized by a novel photochemical reduction method and applied to the methanol APR. Extensive characterizations have proved that the mild catalyst preparation method gave it a high dispersion of Pt species and the addition of La modified the metal-support interaction. The results showed that La-modified Pt/La–CeO 2 -HT and PtLa/CeO 2 catalysts exhibited better catalytic performance than the Pt/CeO 2 -HT catalyst, among which the hydrogen yield was the highest for the surface La-modified PtLa/CeO 2 catalyst (177.7 mmol/g cat ). This was mainly attributed to the surface modification of La resulted in a significant increase in the number of moderately strong basic sites and surface oxygen vacancies in the PtLa/CeO 2 catalyst. The enhancement of catalyst basicity effectively promoted the dissociation of H 2 O to produce hydroxyl groups , while a large number of surface oxygen vacancies provided more active sites for the adsorption and dissociation of H 2 O. And their synergistic behavior efficiently facilitated the water gas shift (WGS) reaction, resulting in a significant increase in hydrogen yield of methanol APR. Associated with the in situ DRIFTS analyzes and the results indicated by WGS reaction, possible promotion mechanism was proposed. • Highly-dispersed APR catalysts were prepared by a novel photochemical reduction method. • The PtLa/CeO 2 catalyst exhibited the highest catalytic activity and H 2 yield (177.7 mmol/g cat ). • Possible reaction mechanism of the synergistic effect on oxygen vacancies and basic sites is verified.
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