Unlocking Enhanced Electrochemical Performance of MBene‐MoB Through Controlled Aluminum Dissipation from MoAlB

Abstract 2D transition metal borides, known as MBenes, have attracted considerable attention due to their exceptional properties. This study explores the feasibility of aluminum (Al) etching from MoAlB using environmentally friendly and sustainable fluoride‐free dilute acidic/alkaline solutions at room temperature, revealing its thermodynamic and kinetic viability. Furthermore, it is found that complete removal of Al can be achieved in dilute alkaline reagent under hydrothermal conditions, yielding pristine single/few‐layered MBene‐MoB for the first time, while acidic solutions result in ≈33% etching rates. XRD refinement, which tracks aluminum removal from 0% to 100%, reveals transient metastable phases of MoAl 1‐x B (x < 0.5) in the initial etching stages, evolving into relatively stable pure Mo 2 AlB 2 structures with 50% Al deficiency, serving as a precursor to MBenes. The subsequent loss of Al results in a 2D MBene‐MoB structure. DFT calculations confirm excellent conductivity for MoAlB, MoAl 1−x B (x = 0–1), and MBene‐MoB. Remarkably, MBene‐MoB exhibits superior supercapacitor performance with a 4025.60 mF cm −2 /201.28 F g −1 capacitance. Simulations validate rapid electrolyte diffusion in layered MBene‐MoB, contributing significantly to enhanced capacitance. Additionally, in the hydrogen evolution reaction (HER), MBene‐MoB demonstrates superior catalytic activity compared to the precursor MoAlB and commercial MoB. Calculations suggest the potential for enhancing HER through surface modulation, considering its suboptimal hydrogen adsorption energy.