Field-Enhanced Nanoconvection Accelerated Electrocatalytic Conversion of Water Contaminants and Electricity Generation.

Abstract

The development of high-performance electrocatalytic systems for the extraction of energy from contaminants in wastewater are urgently needed in emerging renewable energy technologies. However, given that most of the contaminants are present in low concentrations, the heterogeneous catalytic reactions often suffer from slow kinetics due to mass transfer limitations. Here, we report that localized free convection induced by enthalpy change of the reaction can enhance interfacial mass transport. This phenomenon can be found around high-curvature nanosized tips. The finite-element numerical simulation shows that the heat of reactions can produce temperature gradients and subsequently lead to fluid motion at the interfaces, which facilitates the rate-limiting step (mass transfer). To demonstrate the effects of localized field-enhanced mass transport in electrocatalytic conversion of aqueous dilute species, a galvanic cell is constructed with a vertically aligned polyaniline array with sharp tips (as cathode) for the detoxification of a low concentration of carcinogenic chromate and synchronous electricity generation, which show lower overpotential (0.17 V decreased), higher reaction rate (increased by 28%), and power density (22.3 W m-2 in 2 mM chromate). The power output can be scaled up (open voltage of ∼3.7 V and volumetric power density of 840.1 W m-3) by using a continuous flow-through cell with stacked electrodes for further improve the mass transport.