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Abstract:
Two-dimensional (2D) metal-organic framework nanosheets (MOF NSs) play a vital role in catalysis, but the most preparation is ultrasonication or solvothermal. Herein, a liquid-liquid interfacial synthesis method has been developed for the efficient fabrication of a series of 2D Ni MOF NSs. The active sites could be modulated by readily tuning the ratios of metal precursors and organic linkers (R-M/L). The Ni MOF NSs display highly R-M/L dependent activities towards 2e oxygen reduction reaction (ORR) to hydrogen peroxide (H2O2), where the Ni MOF NSs with the R-M/L of 6 exhibit the optimal near-zero overpotential, ca. 98 % H2O2 selectivity and production rate of ca. 80 mmol g(cat)(-1) h(-1) in 0.1 M KOH. As evidenced by X-ray absorption fine structure spectroscopy, the coordination environment of active sites changed from saturation to unsaturation, and the partially unsaturated metal atoms are crucial to create optimal sites for enhancing the electrocatalysis.
