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In-situ plasmonic tracking oxygen evolution reveals multistage oxygen diffusion and accumulating inhibition

Jun-Gang Wang, Lifang Shi, Yingying Su, Liwei Liu, Zhenzhong Yang, Rong Huang, Jing Xie, Yang Tian, Di Li

2021Nature Communications21 citationsDOIOpen Access PDF

Abstract

Understanding mass transfer processes concomitant with electrochemical conversion for gas evolution reactions at the electrode-electrolyte interface plays a key role in advancing renewable energy storage and conversion. However, due to the complicated diffusion behavior of gas at the dynamic catalytic interfaces, it is still a great challenge to accurately portray mass transfer of gas during electrocatalysis process. Here, we track the diffusion of dissolved oxygen on Cu nanostructured plasmonic interface, which reveals multistage oxygen diffusion behaviors, including premature oxygen accumulation, spontaneous diffusion and accelerated oxygen dissipation. This work uncovers an accumulating inhibition effect on oxygen evolution arising from interfacial dissolved oxygen. With these knowledges, we develop a programmable potential scan strategy to eliminate interfacial gas products, which alleviates the concentration polarization, releases accessible actives sites and promotes electrocatalytic performance. Our findings provide a direct observation of the interfacial mass transfer processes that governs the kinetics of gas-involved multiphases catalysis.

Topics & Concepts

Oxygen evolutionOxygenChemical physicsElectrocatalystElectrolyteMass transferDiffusionGas diffusion electrodePolarization (electrochemistry)CatalysisChemical engineeringElectrodeMaterials scienceElectrochemistryConcentration polarizationNanotechnologyGaseous diffusionChemistryThermodynamicsPhysical chemistryChromatographyMembraneOrganic chemistryBiochemistryPhysicsEngineeringElectrocatalysts for Energy ConversionElectrochemical Analysis and ApplicationsAdvanced Memory and Neural Computing