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Electron-Deficient Mo2C Nanoclusters Embedded B, N Co-Doped Hollow Carbon Fibers for Electrocatalytic Nitrate
Ruifang He1, Lu Sun1, Ke Ren1
1State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China.
Abstract:
Ammonia (NH3) production from electrocatalytic nitrate reduction reaction (NO3RR) is anticipated as a promising route to achieve both sustainable NH3 generation and nitrate water pollution removal. Herein, the molybdenum carbide (Mo2C) nanoclusters embedded in boron, nitrogen co-doped hollow carbon fibers (Mo2C@BNHCFs) electrocatalyst is fabricated for NO3RR by coaxial electrospinning and pyrolysis method. The uniformly dispersed Mo2C nanoclusters and the B, N doped-carbon layer provide more adsorption sites for nitrate reduction, effectively improving the activity and long-term stability of Mo2C@BNHCFs. Mo2C@BNHCFs-2 achieves a maximum NH3 yield of 6487.43 μg h-1 mgcat. -1 and Faradaic efficiency of 74.5% at -1.1 V (vs. reversible hydrogen electrode). Electrochemical in situ characterizations identify the formation of intermediates and products during the electrocatalytic NO3 - reduction process. Meanwhile, theoretical calculations indicate that electrons transfer from Mo2C nanoclusters to carbon supports can induce the creation of electron-deficient Mo2C, thus effectively activating the NO3 - and facilitating the electrochemistry process.
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