Abstract
Various heteroatom doped metal organic frameworks (MOFs) and MOFs derived materials with high activity are designed as electrochemical water splitting catalysts. However, local geometrical configuration transformation or local structure distortion on account of heteroatom doping are usually neglected. Herein, this work firstly investigated local structure transformation of metallic oxygen clusters to β-Ni(OH)2-like geometrical configuration (edge-shared octahedrons) in heteroatom (Ru, Cr, Sn and Ce) doped nickel based metal hydroxide-organic frameworks (MHOFs). The transformation process, atomic/electronic structure and composition are investigated via spectroscopy methods such as X-ray absorption structure spectroscopy, X-ray photoelectron spectroscopy and Raman spectroscopy. Hereinto, Ru doped Ni-MHOFs with high local geometrical configuration transformation as a representative one was deeply studied to reveal hydrogen evolution reaction properties. Density functional theory calculations provided a deep understanding of the effect of organic linker defect on local structure and descriptor of p-band center of O. This work provides a sight into local structural transformation in heteroatom doped MHOFs and proposes a novel strategy to modulate structural microenvironment of MOFs materials towards electrochemical applications.
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