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A coordination nanosheet composed of [Fe(tpy)2]2+ (tpy = 2,2':6',2''-terpyridine) units, showing reversible electrochromism at the ligand-based cathodic potential, has been prepared through a liquid/liquid interfacial synthesis. The noble metal-free nanosheet exhibited a CO evolution rate of 114.3 mmol·g−1·h−1 with the selectivity up to 99.3% under visible light irradiation in the presence of water, which is in the front rank of heterogeneous catalysis for CO2 photoreduction. Such robust photocatalytic performance is due to efficient ligand-based electron transfer through long-lived π radical anion tpy·− with a lifetime more than 25 min, as evidenced by in situ electron paramagnetic resonance (EPR) and ultraviolet–visible–near infrared (UV–vis–NIR) spectroscopy studies. Fe(II) cation in [Fe(tpy)2]2+ mainly contributes to enhancing reduction potentials of ligand and stabilizing π radical anion tpy·−. This ligand-based electron transfer with the aid of metal cation represents a promising strategy for selective CO2 photoreduction, especially towards gaining CO from CO2.
This work was supported by the Natural Science Foundation of Ningbo (No. 202003N4077) and the Scientific Research Fund of Zhejiang Provincial Education Department (No. Y202146152).