Tuning selectivity of electrochemical reactions by atomically dispersed platinum catalyst

Abstract

Maximum atom efficiency as well as distinct chemoselectivity is expected for electrocatalysis on atomically dispersed (or single site) metal centres, but its realization remains challenging so far, because carbon, as the most widely used electrocatalyst support, cannot effectively stabilize them. Here we report that a sulfur-doped zeolite-templated carbon, simultaneously exhibiting large sulfur content (17 wt% S), as well as a unique carbon structure (that is, highly curved three-dimensional networks of graphene nanoribbons), can stabilize a relatively high loading of platinum (5 wt%) in the form of highly dispersed species including site isolated atoms. In the oxygen reduction reaction, this catalyst does not follow a conventional four-electron pathway producing H ₂O, but selectively produces H ₂O ₂ even over extended times without significant degradation of the activity. Thus, this approach constitutes a potentially promising route for producing important fine chemical H ₂O ₂, and also offers opportunities for tuning the selectivity of other electrochemical reactions on various metal catalysts.

Abstract

Atomically dispersed metal catalysts display high atom efficiency for electrocatalytic processes. Here, the authors report that sulfur-doped zeolite-templated carbon stabilizes highly dispersed platinum species, predominantly as single-atom centres, and probe its oxygen reduction selectivity.