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CO2 capture and storage have been regarded as promising concepts to reduce anthropogenic CO2 emissions. However, the high cost, inferior adsorption capacity, and higher effective activation temperature of traditional sorbents limit their practical application in efficient CO2 capture. Here, a C‐S‐H@ZIF‐8 (C‐S‐Z) sorbent is fabricated by in situ growth of the ZIF‐8 shell on the C‐S‐H (calcium‐silicate‐hydrate) surface for ultra‐high CO2 adsorption and storage. Among the C‐S‐Z, the outer ZIF‐8 shell acts as a transport channel that promotes CO2 absorption toward the underlying C‐S‐H substrate for accelerated carbonation while preventing nitrogen and water from reaching the interior C‐S‐H. As a consequence, C‐S‐Z possesses the merits of ample pyrrolic nitrogen, porous structure, and ultra‐high surface area (577.18 m2 g−1), that contribute to an ultra‐high CO2 capture capacity, reaching 293.6 mg g−1. DFT calculations show a high CO2 adsorption energy and the mineral carbonation is dominant by the adsorption process. In particular, the advantages of the outstanding adsorption capacity, low cost, and high CO2 selectivity make this C‐S‐H‐based sorbent hold great potential in the practical application for direct air CO2 capture and storage. [ABSTRACT FROM AUTHOR]

Smart materials and devices play an increasingly important role in improving modern life due to their richer functions, enhanced controllability, and improved biocompatibility. Herein, calcium silicate hydration (C–S–H) is integrated with layered [Co(NCS)2(pyrazine)2]n metal–organic frameworks (Co–MOF) and polymeric skeleton to fabricate the smart building material (M–C–S–H). C–S–H was anchored on the polymeric skeleton to reinforce the network structure for enhanced mechanical strength and toughness. Simultaneously, the highly porous skeleton structure enables the uniform distribution of layered Co–MOF, which could maintain its molecular form to endow the M–C–S–H with the photoresponsive color‐switching performance. The M–C–S–H as a smart building material exhibits the color change between light blue and black blue upon near‐infrared illumination on/off within a wide temperature range to achieve personalized wall and building decoration. Taking advantage of the low cost, rapid response, outstanding reversibility, and good color stability, M–C–S–H could provide lively, dynamic, and changeable decorating effects for walls and buildings. [ABSTRACT FROM AUTHOR]