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An ideal interfacial microreactor requires a large interfacial area and robust mechanical properties. Bicontinuous emulsion gels, facilitating reactions at the interface of immiscible fluids, are promising candidates, yet their structural stability remains a challenge. A key issue lies in balancing small domain sizes with mechanical strength, hindered by the inherent trade-off between interfacial free-energy reduction and domain-size minimization. Using coarse-grained molecular dynamics, we compared two surfactant systems: in situ-formed nanoparticlepolymer surfactants (NP-PL surfactants) and Janus nanoparticle surfactants (Janus NPs). Our study presents distinct structural evolution pathways and their impact on gel properties. While some Janus NPs may assemble into micelle-like structures that do not contribute to the bicontinuous network, both surfactants enable small domain sizes (∼200 nm), further reducible with increased concentration. Notably, NP-PL surfactants yield gels with superior thermal and kinetic stability, making them more viable for continuous microreactor applications. These findings offer insights for optimizing bicontinuous emulsion gels as effective microreactors.

Janus hydrogel bioelectronic interfaces have long been challenged by complex fabrication procedures, poor controllability of asymmetric properties and weak interlayer bonding strength. Herein, we fabricated a Janus hydrogel with dual structural and compositional gradients in one step via Molecular Competition Induction mechanism. Unilateral UV light-driven competitive reactions between distinct monomers induce spatiotemporal progressive polymerization, facilitating heterogeneous distribution of polymer segments and gradient-structure formation. The unique configuration effectively addresses issues of weak interfacial bonding and interlayer slippage in Janus hydrogels. Associated with the programmed directional (upward) migration of adhesive groups during fabrication, the Janus hydrogel achieved a 14.6-fold disparity in interfacial adhesion. After self-assembling patterned polypyrrole conductive percolation network on adhesive side, the Janus hydrogel bioelectronic interface enables robust and efficient bidirectional bioelectrical transduction via mechanical-electrical coupling for electroceutical modulation of abdominal wall injury and electrophysiological signals acquisition. This study provides a facile and universal approach for creating bio-adaptive Janus hydrogel interfaces.

Polymerisation-induced self-assembly (PISA) has emerged as a highly efficient method for synthesising polymeric nanoparticles with diverse and well-defined morphologies for a range of applications. While extensive research has focused on solution-based PISA mediated by conformationally free macro-stabilisers, the process of PISA on planar surfaces using surface-tethered macro-stabilisers with constrained mobility, namely surface PISA, remains largely unexplored. Investigating this process is significant to further advance PISA technology and expand its applications. In this work, we explore surface PISA through both experimental and computational approaches, revealing key differences from conventional solution-based PISA. We also demonstrate that surface PISA offers an innovative approach for controlling surface topography and modulating material-bio interactions. Specifically, we showcase its versatile application in creating slippery liquid-infused porous surfaces (SLIPS) and encapsulating antibiotics, endowing material surfaces with enhanced antifouling and antimicrobial properties. We believe this work is a significant step forward for PISA technology and will create new opportunities for its broader applications.

The rapid synthesis of large-sized single-crystalline two-dimensional (2D) covalent organic frameworks (COFs) remains a formidable challenge with current synthetic techniques. A thorough microscopic comprehension of the dynamic processes that govern crystal growth from the perspective of defect formation/repair is imperative. Here, molecular dynamics simulations combined with a dynamic bond model are employed to track the real-time defect evolution in the growth of 2D COFs on surfaces. Our results indicate that defects at grain boundaries, caused by the random orientation of monomers, serve as critical barriers to crystal growth. During the growth process, defects evolve through multiple pathways, involving dynamic reorganization and selfrepair. We demonstrate that the interplay between activation energy and binding energy influences defect repair and, thereby, crystal growth and product morphology. Enhancing both forward and reverse reaction rates, achieved by reducing activation and binding energies within a narrow knife-blade parameter space, facilitates rapid defect repair and promotes single-crystal growth. These findings provide mechanistic insights into defect dynamics and inform the rational design of the reaction conditions for the synthesis of high-quality 2D COFs.