Regulating the complex environment accounting for the stability, selectivity, and activity of catalytic metal nanoparticle interfaces represents a challenge to heterogeneous catalyst design. Here, we introduce narrow, bottom-up synthesized graphene nanoribbons (GNRs) as a new class of graphitic support material, and demonstrate dramatic enhancement of electrocatalytic performance for nanoparticle composite materials featuring GNRs. We find that the catalytic environment created by GNR composites boosts activity and selectivity across several electrocatalytic applications, notably including CO<sub>2</sub> and CO reduction. Additionally, the interaction between GNRs and metal nanoparticles leads to high nanoparticle dispersion and improved stability, yielding stable current and selectivity over periods as long as 24h. Narrow GNRs, because they are synthesized in a bottom-up fashion from small molecule precursors, offer structural and electronic tunability unrivaled by other graphitic materials. We demonstrate this tunability using tailor-made functionalized GNRs that can adjust the catalytic onset potential, alter the mechanism of electrocatalysis at the nanoparticle surface, or even shift reactivity to yield new electrocatalytic products. We further employ advanced imaging, spectroscopic, and electrochemical techniques to characterize GNR-nanoparticle composites structurally and electronically, to understand the nature of the materials’ interaction and its role in electrocatalytic performance. Our findings have implications across the wide range of fields and applications that make use of catalytic inorganic nanoparticles, for which GNRs could prove a powerful complement.

Synergistic performance enhancement in graphene nanoribbon – metal nanoparticle composites for electrocatalysis

253rd National Meeting (2017)

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