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Increased Oxygen Vacancies in CeO2 for Improved Electrocatalytic Nitrogen Reduction Performance.

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Electrochemical nitrogen fixation is a sustainable and economical strategy to produce ammonia. However, fabricating efficient electrocatalysts for nitrogen fixation is still challenging. Theoretical predictions prove that the oxygen vacancy is… Click to show full abstract

Electrochemical nitrogen fixation is a sustainable and economical strategy to produce ammonia. However, fabricating efficient electrocatalysts for nitrogen fixation is still challenging. Theoretical predictions prove that the oxygen vacancy is able to modulate the electronic state of CeO2 and enhance its electrical conductivity, thus promoting the electrochemical nitrogen reduction reaction (NRR) process. Herein, CeO2 with high oxygen vacancy concentration was prepared via a two-step pyrolysis strategy of Ce metal-organic frameworks (MOFs, denoted H-CeO2). Compared to CeO2 with low oxygen vacancy concentration synthesized via one-step pyrolysis of Ce-MOFs (denoted L-CeO2), H-CeO2 exhibits a large NH3 yield rate (25.64 μg h-1 mgcat-1 at -0.5 V vs reversible hydrogen electrode, RHE) and high faradaic efficiency (FE, 6.3% at -0.4 V vs RHE).

Keywords: oxygen vacancy; nitrogen reduction; increased oxygen; oxygen; nitrogen

Journal Title: Inorganic chemistry
Year Published: 2022

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