Efficient heterogeneous catalysis of hydrogen oxidation reaction (HOR) by platinum group metal (PGM)-free catalysts in proton-exchange membrane (PEM) fuel cells represents a significant challenge toward the development of a sustainable hydrogen economy. Here, we show that graphene acid (GA) can be used as an electrode scaffold for the noncovalent immobilization of a bioinspired nickel bis-diphosphine HOR catalyst. The highly functionalized structure of this material and optimization of the electrode-catalyst assembly sets new benchmark electrocatalytic performances for heterogeneous molecular HOR, with current densities above 30 mA cm-2 at 0.4 V versus reversible hydrogen electrode in acidic aqueous conditions and at room temperature. This study also shows the great potential of GA for catalyst loading improvement and porosity management within nanostructured electrodes toward achieving high current densities with a noble-metal free molecular catalyst.

Department of Chemical Sciences University of Padova Via Marzolo 1 35131 Padova Italy

Regional Centre of Advanced Technologies and Materials Department of Physical Chemistry Palacký University Olomouc 17 listopadu 1192 12 771 46 Olomouc Czech Republic

Univ Grenoble Alpes CEA CNRS IRIG Laboratoire de Chimie et Biologie des Métaux F 38000 Grenoble France

Univ Grenoble Alpes CEA CNRS IRIG SYMMES F 38000 Grenoble France

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