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Carbon-based materials that act as supports to design electrocatalysts have been actively pursued for fuel cells and overall water-splitting (OWS) applications. However, carbon-based supports face serious carbon corrosion at high positive potentials, affecting catalyst activity and stability and hindering practical applicability. Herein, carbon-free transition metal-oxide–based 2D titanate nanosheet support has been proposed, demonstrating the applicability of titanate nanosheets as an alternative support for designing electrocatalysts. A new chemical route to produce large 2D nanosheets of titanate via exfoliation has been discovered. Colloidal 2D titanate nanosheet support allows the growth of active nickel molybdenum oxide (NiMoOx) forming Titanate@NiMoOxcore–shell materials. Fine heat treatment at different temperatures facilitates in situformation of MoOxin NiMoOxlayers on 2D titanate boosting catalytic activity. An increase in heat treatment facilitates an increase in the semiconductivity of the titanate phase and a simultaneous decay of the active MoOxcomponent, resulting in poor activity. The optimal catalyst Titanate@NiMoOx_200 required an overpotential of 0.54 and 1.19 VRHEfor the HER and the OER and an overall cell voltage of 1.75 V to deliver a current density of 10 mA cm–2with spectacular stability for up to 24 h in KOH media. Spectroscopic and microscopy analyses prove the efficient electronic interaction between MoOxand NiMoOxin the hybrid components. Density functional theory and experimental work suggest that the MoOx/NiMoOxhybrid shows higher water adsorption energy and excellent water-splitting performance. This work sheds light on the feasibility and practical application of titanate support for the rational design of diverse electrocatalysts from noble to non-noble metal-based electrocatalysts for a range of electrochemical applications.

The CO poisoning effect leads to serious performance degradation of polymer electrolyte membrane fuel cells using reformed H2as fuel. To address this problem, PtRu-based catalysts have been extensively studied over decades. Nevertheless, the catalyst stability issue due to Ru dissolution has always risen to the surface. Here, we propose a solution to simultaneously achieve high CO tolerance and stability of PtRu catalysts viaintroducing a defect-controlled carbon molecular sieve layer. The ultrathin carbon shell with controlled pore structures allows for the selective permeation of H2, providing exceptionally high CO tolerance. The molecular sieve effect is demonstrated even by Ru-free Pt nanoparticles with carbon shells. The carbon shell-encapsulated PtRu nanoparticles also show remarkably improved stability due to the protective carbon layer. This atomic-scale molecular sieve effect is expected to bring about a radical change in the design of CO tolerant catalyst structures that have been entirely dependent on metal composition.