Metal–organic
frameworks (MOFs) are considered
potential
electrocatalysts for efficient water splitting. However, the structure–activity
relationship of most MOFs is not systematically analyzed for electrocatalysis
for anodes and cathodes. In this paper, we provide a strategy to modulate
the electronic microstructure of iron-based bimetallic MOFs (MFe-BDC
(M: Mg, Zn, Cd)) grown on the nickel foam (NF) as bifunctional electrocatalysts
for oxygen evolution reaction (OER) and hydrogen evolution reaction
(HER). The optimal bimetallic CdFe-BDC via modulating appropriate
metal cations of IIA and IIB possesses excellent OER and HER performance
with the lowest overpotentials of 290 mV at 100 mA cm–2 and 148 mV at 10 mA cm–2, respectively. The overall
water splitting performance of the as-prepared CdFe-BDC requires 1.68
V to achieve a current density of 10 mA cm–2 in
the real seawater media, and it exhibits the competitive H2 and O2 production rates of 6.4 and 3.1 μL s–1, respectively, in ambient alkaline conditions, suggesting
its potential practical applications. Density functional theory (DFT)
calculations demonstrate the relationship between microstructure and
electrocatalytic performance of bimetallic MFe-BDC. This work emphasizes
the significance of tailoring the electronic microstructure of bimetallic
MOFs for efficient overall water splitting in alkaline and seawater
environment.
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