Abstract

Fabrication of freestanding nanostructured aerogel monoliths with multifunctionality on a large scale represents a great challenge due to the limited scalable methods for synthesis and assembly of multi-component nanostructures into one single gel body. Here, we report a scalable solvothermal-based in situ gelation method for synthesizing mechanically stable cobalt-based layered inorganic-organic hybrid nanobelt (Co-LIOHN) aerogel monoliths with a density as low as 2.8 mg/cm 3 , an ultralow thermal conductivity of 25 mW/(mK), and extraordinary adsorption capacities of 51–145 g/g for various solvents. Moreover, the aerogel exhibits reversible thermochromic behavior originating from the changing of the coordination environment of the Co 2+ caused by the loss and uptake of coordinating molecular water upon heating and cooling. The Co-LIOHN aerogels integrate unique features of the aerogel and intrinsic properties of the hybrid nanobelts, giving access to a truly multifunctional material that has great potential for applications in thermal insulation, environmental remediation, sensing, and camouflage. • A scalable in situ gelation method is developed for producing Co-LIOHN aerogels • The gelation is enabled by self-crosslinking of nanobelts via van der Waals forces • The Co-LIOHN aerogel shows excellent oil removal and thermal insulation capability • The Co-LIOHN aerogel demonstrates unprecedented thermochromic properties Li et al. report a facile and scalable in situ gelation method for the fabrication of macroscopic freestanding cobalt-based layered inorganic-organic hybrid nanobelt aerogel monoliths that exhibit outstanding oil removal, thermal insulation, and thermochromic properties.

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