Boosting the catalytic activity of Pd-nanocatalysts by anchoring transition metal atoms on carbon supports for formic acid dehydrogenation

Abstract

Liquid formic acid (FA) dehydrogenation, which needs high-performance catalysts to generate green hydrogen at room temperature, is a promising chemical hydrogen storage technology that can replace fossil fuels in energy-related devices. In this work, a novel nanocatalyst with ultrafine palladium nanoparticles (Pd NPs) immobilized on a transition metal atom-decorated carbon support was synthesized for the dehydrogenation of liquid FA. Via a hydrothermal of glucose and carbonitride with a following Co doping through a heat treatment process, porous carbons with evenly dispersed Co-sites on it were strategically achieved, which could be used as a support for immobilizing Pd NPs. The obtained Pd/NC-Co1% catalyst exhibited much superior catalytic activities to those samples without Co doping on the support (Pd/NC and PdCo1%/NC), showing an impressive turnover frequency of 3045 h−1 at 50 °C for FA dehydrogenation. Other transition metal species such as Fe- and Ni-decorated carbon nanocatalysts also showed an improved catalytic activity for FA dehydrogenation. This work not only provides an efficient method to synthesize nanocatalysts with ultrafine metal NPs but also demonstrates that highly dispersed metal atoms on the support can effectively affect the immobilized NPs, resulting in an enhancement of catalytic performance.