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Abstract Water‐splitting reactions such as the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) typically require expensive noble metal‐based electrocatalysts. This has motivated researchers to develop novel, cost‐effective electrocatalytic systems. In this study, a new multicomponent nanocomposite was assembled by combining functionalized multiwalled carbon nanotubes, a Cu‐based metal–organic framework (MOF) (HKUST‐1 or HK), and a sulfidized NiMn‐layered double hydroxide (NiMn‐S). The resulting nanocomposite, abbreviated as MW/HK/NiMn‐S, features a unique architecture, high porosity, numerous electroactive Cu/Ni/Mn sites, fast charge transfer, excellent structural stability, and conductivity. At a current density of 10 mA cm−2, this dual‐function electrocatalyst shows remarkable performance, with ultralow overpotential values of 163 mV (OER) or 73 mV (HER), as well as low Tafel slopes (57 and 75 mV dec−1, respectively). Additionally, its high turnover frequency values (4.43 s−1 for OER; 3.96 s−1 for HER) are significantly superior to those of standard noble metal‐based Pt/C and IrO2 systems. The synergistic effect of the nanocomposite's different components is responsible for its enhanced electrocatalytic performance. A density functional theory study revealed that the multi‐interface and multicomponent heterostructure contribute to increased electrical conductivity and decreased energy barrier, resulting in superior electrocatalytic HER/OER activity. This study presents a novel vision for designing advanced electrocatalysts with superior performance in water splitting. Various composites have been utilized in water‐splitting applications. This study investigates the use of the MW/HK/NiMn‐S electrocatalyst for water splitting for the first time to indicate the synergistic effect between carbon‐based materials along with layered double hydroxide compounds and porous compounds of MOF. The unique features of each component in this composite can be an interesting topic in the field of water splitting. |
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