Support engineering modulated Pt/hierarchical MoSe2@mesoporous hollow carbon spheres for efficient methanol-assisted water splitting

介孔材料 电解 电化学 甲醇 碳纤维 材料科学 分解水 化学工程 电解水 制氢 堆积 电解质 纳米技术 电极 化学 催化作用 复合材料 工程类 物理化学 有机化学 复合数 光催化
作者
Fulin Yang,Wei Qiao,Lice Yu,Shuli Wang,Ligang Feng
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:483: 149055-149055 被引量:15
标识
DOI:10.1016/j.cej.2024.149055
摘要

Hydrogen generation from methanol via methanol-assisted water splitting is a promising electrochemical energy conversion technology but still meets challenges in addressing the low intrinsic activity and easy poisoning problems of the conventional Pt catalysts. Herein, the support engineering modulated Pt by hierarchical MoSe2@mesoporous hollow carbon support was proposed to integrate some structural and catalytic advantages for hydrogen evolution reaction (HER) and methanol oxidation reaction (MOR). Supporting engineering by layered MoSe2 nanosheets confined in mesoporous hollow carbon spheres (MHCSs) is adopted to uniformly anchor Pt nanoparticles (Pt/MoSe2@MHCS), which effectively enhances the conductivity and prevents the layer-by-layer stacking of MoSe2; Strong interaction and coupling ability between Pt and MoSe2 and the resultant electronic structure regulation of the active centers could weaken the binding strength of CO* and H* intermediates during catalysis and strengthen the oxophilicity leading to improved MOR and HER kinetics. Specifically, Pt/MoSe2@MHCS shows a significantly improved MOR current density of 81.1 mA cm−2, about 3.0 times that of the benchmark Pt/C catalyst. Meanwhile, it also exhibits the HER performance of 28 mV to achieve a kinetic current density of 10 mA cm−2 in methanol-contained electrolytes. When employed for overall methanol electrolysis, a lowered input voltage of 1.11 V can be obtained to drive the current density (10 mA cm−2) compared to that for water electrolysis (0.62 V vs. 1.73 V). The electrochemical properties of high activity, rapid catalytic kinetics, and good stability were also demonstrated due to the enhanced oxophilicity and high poisoning tolerance ability resulting from the MoSe2/carbon substrate-induced electron redistribution of Pt sites. This work reports a novel platform to address the catalysis challenges in hydrogen production via the methanol electrolysis technique.
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