NIR photothermal enhancement to achieve high-efficiency nitrogen reduction to ammonia by polyoxometalates@Fe-polydopamine

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.