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Gas molecules, as a family of unique polyatomic building blocks, have long been considered hard to involve in molecular assembly or construct assembled materials due to their structural simplicity yet paucity of defined interacting sites. To solve this non-trivial challenge, a core idea is to break the limit of current ways of bonding gas molecules, endowing them with new modes of interactions that match the basic requirements of molecular assembly. In recent years, a new concept, named the dynamic gas-bridged bond (DGB), has emerged, which allows for gas molecules to constitute a dynamic bridging structure between other building blocks with the aid of frustrated Lewis pairs. This makes it possible to harness gas in a supramolecular or dynamic manner. Herein, this perspective discusses distinct dynamic natures of DGBs and manifests their particular functions in various fields, including the control of molecular/polymeric self-assembly nanostructures, creation of multidimensional assembled materials, and recyclable catalysts. The future research direction and challenges of dynamic gas-bridged chemistry toward gas-programmed self-assembly and gas-constructed adaptive materials are highlighted.

Like any other thermosetting material, polyurethane foams (PUFs) contain permanent cross-links that hinder their reprocessability and make their recyclability a tedious and environmentally unfriendly process. Herein, we introduce acetoacetyl-formed amides, formed by the reaction of isocyanates with acetoacetate groups, as dynamic units in the backbone of PUFs. By extensive variation of the foam composition, optimum parameters have been found to produce malleable foams above temperatures of 130 °C, without the requirement of any solvent during the foaming process. The PU cross-linked material can be compression-molded at least three times, giving rise to PU elastomers and thus maintaining a cross-linked network structure. Characterization of the original foams shows comparable properties to standard PUFs, for example, having a density of 32 kg/m 3 , while they show similar chemical and thermal properties upon reprocessing to strong PU elastomers, exhibiting T g ranging from -42 to -48 °C. This research provides a straightforward method to produce thermally reprocessable PUFs as a promising pathway to address the recycling issues of end-of-life foams.

Developing photopolymerizable polymeric materials offers many opportunities to process materials in a remote and controllable manner. However, most photopolymerizable technologies require the external introduction of photoabsorbing units, whereas designing intrinsically photopolymerizable polymers is still highly challenging. Here, we report that a natural small-molecule disulfide, thioctic acid, can be directly transformed into a poly(disulfides) network under the irradiation of visible light without any external additives. The resulting polymer network exhibits optical transparency, mechanical stretchability and toughness, ambient self-healing ability, and especially strong adhesive ability to different surfaces. The dynamic covalent backbones of the poly(disulfides) endow the depolymerization ability to recycle the material in a closed-loop manner. We foresee that this facile and robust photopolymerization system is of great promise toward low-cost and high-performance photocuring coatings and adhesives.

Magnetically actuated micro/nanoscale pillars have attracted significant research interest recently because of their dynamic properties. These structures can be used for various applications, such as dry adhesion, cell manipulation, and sensors or actuators in microfluidics. Magnetically actuated structures can be fabricated by mixing magnetic particles and polymers to yield a favorable combination of magnetic permeability and mechanical compliance. However, the pillar density of demonstrated structures is relatively low, which limits the potential applications in active surface manipulation of microscale objects. Here, we demonstrate active periodic nanostructures with a pillar density of 0.25 pillar/μm 2 , which is the highest density for magnetically actuated pillars so far. Having a structure period of 2 μm, diameter of 600 nm, and high aspect ratio of up to 11, this structure can be magnetically actuated with a displacement of up to 200 nm. The behaviors of the pillars under various cyclic actuation modes have been characterized, demonstrating that the actuation can be well controlled. This work can find potential applications in particle manipulation and tunable photonic elements.

Dynamic metal-organic frameworks (MOFs) that respond to external stimuli have recently attracted great attention. However, the subtle control of dynamic processes as well as the illustration of the underlying mechanism, which is crucial for the targeted construction and modulation purpose, is extremely challenging. Herein, we report the achievement of simultaneous kinetic and thermodynamic modulation of the structure transformation processes of a family of cobalt(II)-organic frameworks, through the rational combination of coligand replacement, solvent molecule substitution, and ligand-based solid solution strategies. On the basis of the systematic investigation of the structural transformation behaviors, the underlying response mechanism and principles for modulation were illustrated. It is expected that this work can provide valuable hints for the study and further development of dynamic materials.