Yucheng Wu,Yanli Yu,Wei Shen,Yimin Jiang,Rongxing He,Ming Li
It is a promising pathway to use anions to regulate electronic structures, reasonably design and construct highly efficient catalysts for water splitting. Herein, a N-regulated Co cluster catalyst confined in carbon nanotubes, N-Co NCNTs, was constructed successfully. Nitrogen anions played a crucial role in optimizing the electronic structures of Co clusters and enhancing localization of electrons, resulting in polarized cobalt clusters. The N-induced electronic localization and the resulting polarized Co clusters are responsible for the improvement of catalytic activity. N-Co NCNTs exhibited ultra-low overpotentials of 178 mV and 92 mV for the OER and HER to achieve 10 mA cm−2 in an alkaline electrolyte, respectively. Its long-term catalytic durability is mainly attributed to the obstacle to the surface oxidation of Co clusters caused by N-regulation. N-Co NCNTs maintained a stable current density for 160 h at 10 mA cm−2. DFT computations confirmed the decisive role played by nitrogen anions in regulating the electronic structure. This work provides a pathway for understanding and designing highly efficient anion-regulated catalysts.
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising and green process, which urgently demands high-performance catalysts. In this work, a nitrogen-modulated NiMoO4 growth on Ni foam (N-NiMoO4/NF) is prepared via the treatment of NiMoO4 in 1% NH3 at 500 °C. Compared with NiMoO4, the nitrogen-modulated NiMoO4 promotes electro-oxidation of HMF to FDCA and exhibits almost 100% HMF conversion, 97% FDCA yield, and 91% faradaic efficiency. N-NiMoO4 has a higher electrochemical surface area and lower charge transfer resistance than NiMoO4, which enhances the activity of the catalyst for electrocatalytic oxidation of HMF to FDCA. This work gives enlightenment on the nitrogen modulation method to tune the activity of electrocatalysts for biomass refineries.
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