Abstract
Oxygen reduction reaction towards hydrogen peroxide (H2O2) provides a green alternative route for H2O2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report a boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared to the state-of-the-art oxidized carbon catalyst, B-C catalyst presents enhanced activity (saving more than 210 mV overpotential) under industrial-relevant currents (up to 300 mA cm−2) while maintaining high H2O2 selectivity (85–90%). Density-functional theory calculations reveal that the boron dopant site is responsible for high H2O2 activity and selectivity due to low thermodynamic and kinetic barriers. Employed in our porous solid electrolyte reactor, the B-C catalyst demonstrates a direct and continuous generation of pure H2O2 solutions with high selectivity (up to 95%) and high H2O2 partial currents (up to ~400 mA cm−2), illustrating the catalyst’s great potential for practical applications in the future.
Highlights
Oxygen reduction reaction towards hydrogen peroxide (H2O2) provides a green alternative route for H2O2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates
As O2 molecules can be fully reduced to H2O via a 4e− transfer process[12,13,14], which is the preferred pathway in fuel cell applications, developing highly selective and active 2e−-oxygen reduction reaction (ORR) catalysts is the prerequisite of this sustainable synthetic route
We found out that the boron-doped carbon (B–C) system has nearly-zero overpotential from the thermodynamic point of view, while the barrier towards 2e− pathway is lower than the 4e− counterpart from constantpotential molecular dynamics
Summary
Oxygen reduction reaction towards hydrogen peroxide (H2O2) provides a green alternative route for H2O2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. We report a boron-doped carbon (B–C) as highly selective and active 2e−-ORR to H2O2 catalyst, especially under large current densities.
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