Thermal‐Conductive MOFs@BN Self‐Supporting Foams for Synchronously Boosting CO₂ Adsorption/Desorption

Abstract Synchronous boosting adsorption and desorption efficiency is a great challenge for CO₂ adsorption capture, especially for metal–organic frameworks (MOFs) having high adsorption uptakes. Herein, a novel “self‐supporting foam” strategy is proposed to fabricate a thermally conductive MOFs@boron nitride nanosheets (BNNS) composite foam (MOFs@BNNS‐PEI) via polyethyleneimine (PEI) cross‐linkage. The “rebar” BNNS and the “aggregate” MOFs are packed against each other to form a self‐supporting structure, effectively reducing the reliance on polymers to maintain high MOFs loading. Furthermore, this approach enables the successful fabrication of three different types of typical MOFs, including HKUST‐1, MIL‐100(Fe), and ZIF‐8. This unique design maintains a high specific surface area (SSA) of the MOFs foam and generates nitrogen‐rich microporosity contributing to CO₂ adsorption. Additionally, PEI serves as a thermal bridge to reduce the interfacial thermal resistance between BNNS and MOFs, accelerating the thermal desorption of CO₂ within the MOFs foam. Benefiting from these advantages, the MOFs@BNNS‐PEI exhibits a higher CO₂ adsorption capacity (1.35–1.42 times that of pure MOFs) and a significant increase in the desorption rate for CO₂ (5.0–5.7 times that of pure MOFs). Thus, the thermally conductive MOFs foam can be a viable option for efficient CO₂ capture in practical applications.