Development of effective technologies for clean and sustainable hydrogen energy has been attracting great attention. Toward this end, a promising approach is based on the electrolysis of water for hydrogen production. To date, the most effective electrocatalysts towards hydrogen evolution reaction (HER) are based on Pt-group metals. However, the high costs and natural scarcity have severely limited their broad utilization. Transition metal compounds have been prepared as effective, alternative HER catalysts in a series of recent studies. However, thus far, it has remained a great challenge to develop highly active HER catalysts with a low overpotential based on earth-abundant and cost-effective materials. Recently, carbon-based electrocatalysts have attracted a great deal of interest because of their low overpotentials toward HER. Notably, the active sites of carbon for HER can be modulated by the incorporation of transition metal nanoparticles and (non)metal doping. In this presentation, we will summarize recent progress in the development of carbon-based electrocatalysts toward HER. In particular, we will report recent development in the design and engineering of single-atom catalysts for HER, which is exemplified with graphitic-like carbon nitride (C3N4) nanosheets embedded with ruthenium ions. This takes advantage of the strong affinity of ruthenium ions to pyridinic nitrogen of the tri-s-triazine units of C3N4. Significantly, the hybrid materials exhibit apparent electrocatalytic activity towards HER in acid and the activity increases with the loading of ruthenium metal centers in the C3N4 matrix. Control experiments suggest minimal contributions from the C3N4 nanosheets to the HER activity, and the activity is mostly due to the formation of Ru-N moieties where the synergistic interactions between the carbon nitride and ruthenium metal centers facilitate the adsorption of hydrogen. This is strongly supported by results from density functional theory calculations.

Hydrogen evolution reaction catalyzed by atomically dispersed transition metals in carbon matrices

2019 Spring National Meeting

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