Steering the electronic communication between Al/Ru bimetallic clusters in metal–organic framework composites for accelerating hydrogen evolution kinetics†
*a
Siping
Wei
*c
Abstract
Synergistically modulating electron distribution between metal nodes in metal–organic frameworks (MOFs) is an effective strategy to improve the electrocatalytic performance of MOFs. Herein, a special bimetallic MOF composite (Al0.35/Ru0.15-TCPP-CNTs) was constructed by introducing highly dispersed Ru and Al co-existing in the MOF metal clusters and combining them with conductive carboxylic multi-walled carbon nanotubes (CNTs). Notably, the catalyst exhibited excellent hydrogen evolution reaction (HER) performance, with an overpotential of as low as 32 mV at a current density of 10 mA cm−2 in acidic media, comparable to commercial Pt/C. Experimental results and density functional theory (DFT) calculations proved that a reasonable proportion of Al/Ru bimetallic clusters in MOFs and the loaded CNTs induced charge redistribution and cooperative electronic coupling, which not only optimized the adsorption energy of H intermediates (ΔGH*) and produced a possible hydrogen spillover effect, but also increased the specific surface area and facilitated electron/mass transfer. This work may provide an improved method and research idea for the study of MOF electrocatalysts at the atomic level.
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