Abstract

A feasible and general strategy based multimetallic metal-organic frameworks template is developed to fabricate hierarchical structured multimetallic selenide. The obtained series of transition metal doped iron selenide exhibit high performance for oxygen evolution reaction (OER). Especially, the Cu-doped FeSe2 electrocatalyst shows the lowest overpotential of 193 mV at a current density of 10 mA cm−2 which outperforms previously reported selenide-based electrocatalysts. The experimental results and theoretical simulations demonstrate that the doping of substitutional Cu in the host lattice of FeSe2 optimizes the electronic structure, being favorable for accelerating the electron transfer and boosting reaction kinetic. Meanwhile, the special structure design enables the electrocatalyst with hierarchical structures, affording rich exposed active sites for efficient OER. Therefore, this work provides a feasible strategy for fabricating hierarchical structured metal selenides for potential electrochemical energy storage and conversion.

Highlights

  • The oxygen evolution reaction (OER) as the half reaction of water splitting suffers multistep proton-coupled electron transfer, which leads to unfavorable sluggish kinetics

  • Transition metal selenides (TMSs) as electrocatalysts exhibit various advantages owing to their high theoretical catalytic performance, low cost, and environmental benignity

  • The electrocatalytic performances of various monometallic selenides were first evaluated to select the optimum candidate for subsequent investigation of transition metal doping issue

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Summary

INTRODUCTION

The growing concerns on serious energy crisis and environmental pollution issues stimulate great efforts for exploring renewable energy. Electrochemical water splitting has been considered as a promising way for producing green and renewable hydrogen. the oxygen evolution reaction (OER) as the half reaction of water splitting suffers multistep proton-coupled electron transfer, which leads to unfavorable sluggish kinetics. In order to tackle this problem, the efficient electrocatalysts are highly desirable. Compared with traditional noble metals based electrocatalysts, earth-rich catalysts such as transition metal oxides, hydroxides, phosphides, and chalcogenides are regarded as ideal candidates. Among these materials, transition metal selenides (TMSs) as electrocatalysts exhibit various advantages owing to their high theoretical catalytic performance, low cost, and environmental benignity.. A multimetallic MOFs template-directed strategy is proposed to fabricate highly arrayed transition metal doped iron selenide (Scheme 1). The unique hierarchical structure and the doping of transition metal afford rich exposed active sites, enhanced conductivity, and fast mass transfer, being favorable for boosting the OER process. It is expected that the multimetallic MOFs template-directed strategy could be potentially used for the construction of other electrocatalysts with hierarchical structures for water splitting

Materials
Fabrication of FeM-MOF-74 arrays
Fabrication of M-doped FeSe2 arrays
Characterization
Electrochemical measurements
DFT calculation
RESULTS AND DISCUSSION
CONCLUSIONS
Full Text
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