Development of oxygen evolution reaction (OER) electrocatalysts with low cost and high performance is the key procedure in industrial electrolysis of water to produce hydrogen. Unfortunately, current reports heavily rely on empirical investigation and overlook the relationship between types of elements and the degree of amorphous, which hinders the design of amorphous metal−organic frameworks (MOFs) with high catalytic activity. Here, we prepared a series of bimetallic Fe-M-MOFs to explore the types of elements/degree of amorphous/catalytic property relationship. The amorphous FeNi-MOF containing crystalline nanostructures has the best OER performance and splendid stability. Additionally, density functional theory (DFT) demonstrates that benefiting from the strong coupling between Fe and Ni atoms, the d-band center of the active sites in FeNi-MOF (−0.92 eV) moves down compared to Fe-MOF (−1.24 eV), optimizing the *OOH intermediate toward rapid OER kinetics. This work provides a brand new approach to design efficient amorphous MOF electrocatalysts from the perspective of types of elements/degree of amorphous and regulation of the d-band center.
The preparation of low-cost and high-activity oxygen evolution reaction (OER) catalysts is a technical bottleneck in the field of electrolysis of water to produce hydrogen. Amorphous metal-organic frameworks (MOFs) with...
Development of low-cost and high-efficiency electrocatalysts for overall water splitting is of great significance in the sustainable hydrogen economy. Herein, Fe 1.2 (CoNi) 1.8 Se x medium-entropy metal selenides (MESes) nanoparticles are prepared via the selenylation of metal-organic frameworks (MOFs) precursors. The optimal Fe 1.2 (CoNi) 1.8 Se 6 MESe exhibits an outstanding electrocatalytic performance in alkaline media, offering low overpotentials of 66 and 216 mV at 10 mA cm −2 for the hydrogen evolution reaction and oxygen evolution reaction, respectively. A full electrolysis apparatus with Fe 1.2 (CoNi) 1.8 Se 6 MESe as both cathode and anode displays an excellent performance, achieving 10 mA cm −2 at a potential of 1.55 V. Furthermore, density functional theory calculations demonstrate that the formation of MESe enhances the surface charge density and brings the d-band center closer to Fermi level, as compared with that of the MOF precursor. Overall, the proposed strategy of medium-entropy materials presents a low-cost approach to fabricate energy storage and conversion devices.
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