Self-Supported Ceramic Electrode of 1T-2H MoS₂ Grown on the TiC Membrane for Hydrogen Production

Binder-free, cost-effective, and stable hydrogen evolution reaction electrocatalytic electrodes with a customized size are urgently needed for large-scale industrial hydrogen production. Toward this challenge, self-supported TiC@MoS2 (TCMS) ceramic membrane electrodes were fabricated by a self-template strategy. Porous TiC ceramic membranes with straight finger-like pores were first fabricated by phase inversion tape-casting and sintering. Then, a 1T-2H MoS2 nanosheet layer grew on the porous conductive TiC skeleton. The high conductivity of the TCMS skeleton promotes charge transfer, while the porous structure, which consists of abundant finger-like and cavernous pores, favors proton transfer and bubble transfer during the electrolysis process. The optimal TCMS composition displayed an overpotential of −127 mV at −10 mA·cm–2, a Tafel slope of 41 mV·dec–1, and an extremely high electrochemical active area of 1079.4 mF·cm–2 as well as remarkable stability in 0.5 M H2SO4. A high Faradaic efficiency of 99.7% was also achieved. The superior electrocatalytic performance was ascribed to the synergistic effect of the tight bonding and the crystal matching between TiC and MoS2, the unique dual pore structure, the abundant exposed active sites of MoS2 nanoflakes, and the high 1T-MoS2 content. First-principles density functional calculations showed that the 1T-MoS2/TiC hybrid has the lowest free energy for H adsorption (0.116 eV) and the highest density of states near the Fermi level, which leads to a strong catalytic activity.