The precise structural integration of single-atom and high-entropy-alloy features for energy electrocatalysis is highly appealing for energy conversion, yet remains a grand challenge. Herein, we report a class of single-atom Mo-tailored PdPtNiCuZn high-entropy-alloy nanosheets with dilute Pt-Pt ensembles and intrinsic tensile strain (Mo₁-PdPtNiCuZn) as efficient electrocatalysts for enhancing the methanol oxidation reaction catalysis. The as-made Mo₁-PdPtNiCuZn delivers an extraordinary mass activity of 24.55 A mg_Pt⁻¹ and 11.62 A mg_Pd+Pt⁻¹, along with impressive long-term durability. The planted oxophilic Mo single atoms as promoters modify the electronic structure of isolated Pt sites in the high-entropy-alloy host, suppressing the formation of CO adsorbates and steering the reaction towards the formate pathway. Meanwhile, Mo promoters and tensile strain synergistically optimize the adsorption behaviour of intermediates to achieve a more energetically favourable pathway and minimize the methanol oxidation reaction barrier. This work advances the design of atomically precise catalytic sites by creating a new paradigm of single atom-tailored high-entropy alloys, opening an encouraging pathway to the design of CO-tolerance electrocatalysts.

The superior PdAg@g-C₃N₄ Mott–Schottky heterojunction exhibits boosting dehydrogenation photocatalysis of formic acid (TOF = 420 h⁻¹) without any additive under visible light (λ > 400 nm) at room temperature.

The hydrogen evolution reaction (HER) of molybdenum disulfide (MoS₂) is limited in alkaline and acid solution because the active sites are on the finite edge with extended basal plane remaining inert. Herein, we activated the interfacial S sites by coupling with Ru nanoparticles on the inert basal plane of MoS₂ nanosheets. The density functional theory (DFT) calculation and experimental results show that the interfacial S electronic structure was modulated. And the results of ΔG_H* demonstrate that the adsorption of H on the MoS₂ was also optimized. With the advantage of interfacial S sites activation, the Ru-MoS₂ needs only overpotential of 110 and 98 mV to achieve 10 mA·cm⁻² in both 0.5 M H₂SO₄ and 1 M KOH solution, respectively. This strategy paves a new way for activating the basal plane of other transition metal sulfide electrocatalysts for improving the HER performance.