Abstract
2D-layered materials have attracted increasing attention as low-cost supports for developing active catalysts for the hydrogen evolution reaction (HER). In addition, atomically thin Ti3 C2 Tx (MXene) nanosheets have surface termination groups (Tx : F, O, and OH), which are active sites for effective functionalization. In this work, heteroatom (boron)-doped Ti3 C2 Tx (MXene) nanosheets are developed as an efficient solid support to host ultrasmall ruthenium (Ru) nanoparticles for electrocatalytic HER. The quantum-mechanical first-principles calculations and electrochemical tests reveal that the B-doping onto 2D MXene nanosheets can largely improve the intermediate H* adsorption kinetics and reduce the charge-transfer resistance toward the HER, leading to increased reactivity of active sites and favorable electrode kinetics. Importantly, the newly designed electrocatalyst based on Ru nanoparticles supported on B-doped MXene (Ru@B-Ti3 C2 Tx ) nanosheets shows a remarkable catalytic activity with low overpotentials of 62.9 and 276.9mV to drive 10 and 100mA cm-2 , respectively, for the HER, while exhibiting excellent cycling stabilities. Moreover, according to the theoretical calculations, Ru@B-Ti3 C2 Tx exhibits a near-zero value of Gibbs free energy (ΔGH* = 0.002eV) for the HER. This work introduces a facile strategy to functionalize MXene for use as a solid support for efficient electrocatalysts.
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