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The advanced thermal insulation materials with low cost and high mechanical properties play an important role in transport packaging and thermal protection fields. An inorganic/organic composite aerogel was prepared through hydrogen bonds and chemical crosslinking among silica aerogel particles, gelatin (GA), and hydroxyethyl cellulose (HEC). The as‐prepared GA/HEC‐SiO2 composite aerogels were characterized by compression tests, scanning electron microscopy, Fourier transform infrared, thermogravimetric analyzer, and contact angle tests to investigate the chemical composition and physical structure. The GA/HEC‐SiO2 composite aerogels exhibited a strong mechanical strength (0.53–4.01 MPa), a high compression modulus (1.33–11.52 MPa), a lower volume density (0.035–0.081 g/cm3), thermal conductivity as low as 0.035 W/[m K]), a porosity of more than 93%, and hydrophobic angle as high as 150.01° after hydrophobic modification. These results indicate that biopolymer composite aerogels embedded with SiO2 aerogel particles display a bright future in thermal insulation.

This work presents the preparation and property characterization of a biomass gelatin (GA)-based aerogel. Halloysite nanotubes (HNTs) were used to improve the mechanical strength, pore size distribution, and thermal stability of the aerogel. Polyethyleneimine (PEI) and (3-glycidyloxypropyl)­trimethoxysilane (GPTMS) were utilized to increase the interfacial interaction between HNTs and GA through chemical cross-linking. Green, sustainable, and low-cost composite aerogels were prepared by “cogel” and freeze-drying techniques. The experimental results show that the HNTs/GA composite aerogel has a low density (31.98–57.48 mg/cm3), a high porosity (>95%), a low thermal conductivity (31.85–40.16 mW m–1 K–1), and superior moldability. In addition, the mechanical strength and thermal insulation properties of the HNTs/GA composite aerogels with a “thorn”-like lamellar porous network structure are different in the axial direction versus the radial direction. The maximum compressive strength, maximum compressive modulus, and corresponding specific modulus in the axial direction were 1.81 MPa, 5.45 MPa, and 94.8 kN m kg–1, respectively. Therefore, the biomass/clay composite aerogel will be a sustainable and renewable functional material with high mechanical strength and thermal insulation properties, which is expected to further promote biomass and clay for high value utilization.