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Rational design and construction of low-cost and highly efficient electrocatalysts for hydrogen evolution reaction (HER) is meaningful but challenging. Herein, a robust three dimensional (3D) hollow CoSe2@ultrathin MoSe2 core@shell heterostructure (CoSe2@MoSe2) is proposed as an efficient HER electrocatalyst through interfacial engineering. Benefitting from the abundant heterogeneous interfaces on CoSe2@MoSe2, the exposed edge active sites are maximized and the charge transfer at the hetero-interfaces is accelerated, thus facilitating the HER kinetics. It exhibits remarkable performance in pH-universal conditions. Notably, it only needs an overpotential (η10) of 108 mV to reach a current density of 10 mA·cm−2 in 1.0 M KOH, outperforming most of the reported transition metal selenides electrocatalysts. Density functional theory (DFT) calculations unveil that the heterointerfaces synergistically optimize the Gibbs free energies of H2O and H* during alkaline HER, accelerating the reaction kinetics. The present work may provide new construction guidance for rational design of high-efficient electrocatalysts.

Exploring low-cost and earth-abundant catalyst to efficiently release clean H2 from solid hydrogen storage materials is an appealing solution for exhausted fossil fuel and its associated environmental issue. Halloysite (Hal) nanotubes are regarded as promising alternative catalyst support for expensive synthetic support materials due to their low cost and abundant resource. Herein, we report a simple and controllable one-pot reaction followed by chemical reduction approach to manufacture Ni, Co, P hybrids on Hal as high-efficient and non-noble metal catalysts for hydrolysis of ammonia borane (AB). It is revealed that ultrafine Ni0.13Co0.87P nanoparticles with diameter of 1.4 nm are homogenously anchored on Hal surface with excellent stability. The synergy among Ni, Co and P in Ni0.13Co0.87P effectively enhances their interaction with AB, resulting in reduced activation energy (41.8 kJ mol−1) and consequently significant boost of hydrolytic catalytic activity (TOF 47.5 molH2 molcat−1 min−1). A proposed mechanism demonstrates water molecules involve in the hydrolysis reaction and the rate-determining step is the O H cleavage in H2O. This work affords a prospective idea for the exploiting of Hal as well as new point of view for the reasonable design of low-cost AB hydrolysis catalyst.