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The development of atmospheric pressure N2 reduction to NH3 is attracting much attention in green chemistry, yet it is still a challenge to obtain satisfactory activity under mild conditions. Herein, an efficient near-infrared (NIR) photothermal catalysis reduction of N2 constitutes an occurrence is reported. With or without V-substitute polyoxometalates (POMs) loaded on the surface of Fe-chelated polydopamine (Fe-PDA) photothermal support through the electrostatic interactions, NIR photothermal catalysts POMs@Fe-PDA are fabricated. The induction of “FeV” cofactor facilitates electron transfer between V(V)/V(IV)&Fe(III)/Fe(II) and N2, thereby activating N2 molecule. The synergy between the catalytic activity of V-POMs and the local NIR photothermal effect of Fe-PDA dramatically enhances N2 reduction. Noticeably, PMo10V2@Fe-PDA exhibits a significantly enhanced NH3 production rate of 181.1 μmol·L−1 with a turnover frequency of 1006.1 mmol·M−1·h−1 under 808 nm NIR laser radiation, being the highest values reported at atmospheric pressure. We expect that this work could provide an alternative approach for photothermal catalysis N2 reduction under mild conditions.
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