Abstract
The most active and efficient catalysts for the electrochemical hydrogen evolution reaction (HER) rely on platinum, a fact that increases the cost of producing hydrogen and thereby limits the widespread adoption of this fuel. Here, a metal-free organic electrocatalyst that mimics the platinum surface by implementing a high work function and incorporating hydrogen-affine hydrogen bonds is introduced. These motifs, inspired from enzymology, are deployed here as selective reaction centres. It is shown that the keto-amine hydrogen-bond motif enhances the rate-determining step in proton reduction to molecular hydrogen. The keto-amine-functionalized polymers reported herein evolve hydrogen at an overpotential of 190 mV. They share certain key properties with platinum: a similar work function and excellent electrochemical stability and chemical robustness. These properties allow the demonstration of one week of continuous HER operation without notable degradation nor delamination from the carrier electrode. Scaled continuous-flow electrolysis is reported and 1 L net molecular hydrogen is produced within less than 9 h using 2.3 mg of polymer electrocatalyst.
Highlights
The most active and efficient catalysts for the electrochemical hydrogen evolution reaction (HER) rely on platinum, a fact that increases the cost of thermodynamic exchange current i0.[1,2,3] Only when these requirements are met will hydrogen evolution occur at minproducing hydrogen and thereby limits the widespread adoption of this fuel
Efficient hydrogen evolution reaction (HER) electrocatalysts explore conducting polydopamine (PDA) as electrocatalysts require minimum binding energies for adsorbed whose organic surfaces offer a remarkable degree of catalytic hydrogen ∆GH* along with a surface configuration that will activity by tuning structural designs and conductivity.[35,36] reduce protons in an acidic environment as quantified via the We first sought to engineer a high work function, as this has
We explored experimentally the reaction parameters of the previously reported oxidative chemical vapor deposition.[37,39]
Summary
The most active and efficient catalysts for the electrochemical hydrogen evolution reaction (HER) rely on platinum, a fact that increases the cost of thermodynamic exchange current i0.[1,2,3] Only when these requirements are met will hydrogen evolution occur at minproducing hydrogen and thereby limits the widespread adoption of this fuel. The photoemission (UV and X-ray) results as well as the Raman spectra confirm that higher reaction temperature in the oCVD synthesis forms DHI-PDA with
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