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Metal-organic frameworks (MOFs) hold great promise for diverse applications when combined with polymers. However, a persistent challenge lies in the susceptibility of exposed MOF pores to molecule and polymer penetration, compromising the porosity and overall performance. Here, we design a molecular-caged MOF (MC-MOF) to achieve contracted window without sacrificing the MOF porosity by torsional conjugated ligands. These molecular cages effectively shield against the undesired molecule penetration during polymerization, thereby preserving the pristine porosity of MC-MOF and providing outstanding light and thermal management to the composites. The polymer containing 0.5 wt % MC-MOF achieves an 83% transmittance and an exceptional haze of 93% at 550 nanometers, coupled with remarkable thermal insulation. These MC-MOF/polymer composites offer the potential for more uniform daylighting and reduced energy consumption in sustainable buildings when compared to traditional glass materials. This work delivers a general method to uphold MOF porosity in polymers through molecular cage design, advancing MOF-polymer applications in energy and sustainability.

Phonon-assisted photon upconversion holds great potential for numerous applications, e.g., optical refrigeration. However, traditional semiconductors face energy gain limitations due to thermal energy, typically achieving only ~25 milli-electron volts at room temperature. Here, we demonstrate that quasi-two-dimensional perovskites, with a soft hybrid organic-inorganic lattice, can efficiently upconvert photons with an anti-Stokes shift exceeding 200 milli-electron volts. By using microscopic transient absorption measurements and density functional theory calculations, we explicate that the giant energy gain stems from strong lattice fluctuation leading to a picosecond timescale transient band energy renormalization with a large energy variation of around ±180 milli-electron volts at room temperature. The motion of organic molecules drives the deformation of inorganic framework, providing energy and local states necessary for efficient upconversion within a time constant of around 1 ps. These results establish a deep understanding of perovskite-based photon upconversion and offer previously unknown insights into the development of various upconversion applications.

Electronic skin (e-skin), a new generation of flexible electronics, has drawn interest in soft robotics, artificial intelligence, and biomedical devices. However, most existing e-skins involve complex preparation procedures and are characterized by single-sensing capability and insufficient scalability. Here, we report on a one-step strategy in which a thermionic source is used for the in situ molecularization of bacterial cellulose polymeric fibers into molecular chains, controllably constructing an ionogel with a scalable mode for e-skin. The synergistic effect of a molecular-scale hydrogen bond interweaving network and a nanoscale fiber skeleton confers a robust tensile strength (up to 7.8 MPa) and high ionic conductivity (up to 62.58 mS/cm) on the as-developed ionogel. Inspired by the tongue to engineer the perceptual patterns in this ionogel, we present a smart e-skin with the perfect combination of excellent ion transport and discriminability, showing six stimulating responses to pressure, touch, temperature, humidity, magnetic force, and even astringency. This study proposes a simple, efficient, controllable, and sustainable approach toward a low-carbon, versatile, and scalable e-skin design and structure-performance development., Competing Interests: The authors declare that they have no competing interests., (Copyright © 2022 Geyuan Jiang et al.)