| Summary: | Pursuing novel materials with efficient photothermal conversion under irradiation at the near-infrared region windows (NIR, 750–850 nm; NIR-I and NIR-II, 1000–1320 nm)) is of great importance due to their irreplaceable applications, especially in the biomedical field. Herein, on the basis of a coordination chemistry strategy, an iron-based metal-organic framework (MOF) of [N(CH<sub>3</sub>)<sub>4</sub>]<sub>2</sub>[Fe<sub>3</sub>(NDC)<sub>4</sub>]·DMF·3H<sub>2</sub>O (<b>Fe-NDC</b>, 1,4-H<sub>2</sub>NDC = 1,4-naphthalenedicarboxylic acid, N(CH<sub>3</sub>)<sub>4</sub><sup>+</sup> = tetramethyl-ammonium, and DMF = N,N-dimethylformamide) was prepared and characterized. Due to the <i>d</i>-<i>d</i> transition effect introduced by coordination with the transition-metal ion of iron and the highly conjugated naphthalenic moiety in 1,4-H<sub>2</sub>NDC, guaranteeing an energy transfer between iron and the organic module, <b>Fe-NDC</b> shows a remarkable broad absorption, which could be extended into the NIR-II section. As a result, <b>Fe-NDC</b> could be irradiated by NIR laser (both 808 and 1064 nm) to achieve photothermal conversion. This work sets a good example to inspire the future designation of NIR light-irradiated photothermal materials based on the first-row transition metals.
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