Zebao Rui

Robust underwater adhesives hold high application value, yet are restricted by the challenges of room-temperature underwater curing and negative effect of interfacial water. Inspired by mussels that form firm underwater bonds via catechol-containing byssus proteins, herein, the six-membered cyclic dithioacetal epoxy curing agent (DM-1) is synthesized via the condensation reaction between bio-based protocatechualdehyde and dihydrolipoic acid for constructing advanced underwater epoxy adhesives by dynamic dithioacetal-driven stepwise curing. During curing, DM-1 first generates linear polydithioacetal through a dynamic dithioacetal-driven ring-opening reaction, followed by the reaction of the generated terminal thiol groups with epoxy groups. Subsequently, the side-chain carboxyl groups continue to react with epoxy groups, accompanied by the dissociation-recombination process of dithioacetal bonds to achieve cross-linking. Benefiting from the synergistic effect of the interfacial strength provided by hydrophobic polydithioacetal chains and catechol groups, and the cohesive strength derived from multiple underwater curing processes, the adhesive exhibits superior underwater adhesive bonding strength on stainless steel (11.2 MPa) to that achieved in air (3.7 MPa), environmental tolerance and recyclability, providing a feasible strategy for the development of high-performance underwater epoxy adhesives.

The pursuit of durable and eco-friendly antifouling surfaces has become a critical challenge across engineered systems, ranging from architectural coatings to marine infrastructure. Herein, we propose an innovative stepwise physicochemical antifouling mechanism through the rational integration of hierarchical superamphiphobic architectures with bactericidal copper oxide nanoparticles. The designed coating operates via a sequential defense protocol: physical antiadhesion enabled by a superamphiphobic surface exhibiting ultralow surface energy, coupled with a chemical antibacterial effect through controlled Cu²⁺ ion release from embedded CuO nanoparticles. When the action time reaches 24 h, the coating shows excellent antibacterial effects against Gram-negative Escherichia coli (E. coli), Pseudomonas aeruginosa (P. aeruginosa), and Gram-positive Staphylococcus aureus (S. aureus). A scalable spray-coating technique was developed using 3-aminopropyltriethoxysilane (APTES)-functionalized CuO/SiO₂ nanocomposites with 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PFDTES) modification for the coating fabrication. Systematic characterization combining Cassie-Baxter modeling, X-ray Photoelectron Spectroscopy (XPS) analysis, and bacterial viability assays confirms the mechanistic coupling between topographical liquid repellency and chemical bactericidal activity. The contact angle (CA) value of CuO-SiO₂/APTES@PFDTES calculated by dynamic density functional theory (DDFT) is 165.5°. This work provides a promising strategy for the rational design of advanced superamphiphobic antifouling coatings through physicochemical antibacterial strategies.

In N₂ photoreduction, photogenerated holes and electrons are involved in H₂O photolysis for proton supply and the weakening of the N≡N triple bond for N₂ activation, respectively. Rationally regulating the structure-activity relationship of these catalytic sites for available generation of charge carriers is crucial for optimizing N₂-to-NH₃ conversion efficiency. Herein, a robust photothermal catalyst carboxyl-enriched supramolecular (perylene tetracarboxylic acid, PTA) functionalized MIL-125(Ti)/MXene having dynamic proton extraction sites is designed for efficient N₂ photoreduction. Among these, MIL-125(Ti), PTA, and Ti₃C₂ MXene are, respectively, responsible for N₂ activation, reliable proton supply through interconversion between Brønsted acid and its conjugated base, and a photothermal response for accelerated reaction kinetics. The synergistic collaboration of these functionally distinct modules enhances light harvesting and responsiveness for dynamic multielectron/proton extraction, thereby facilitating feasible photothermal catalytic ammonia production. Remarkably high solar-to-ammonia conversion rates of 314.5-654.7 μmol g^-1 h^-1 are achieved under 100-500 mW cm^-2 illumination. This work provides insights into the rational design of an efficient solar ammonia synthesis system.

Herein, an innovative two-stage curing strategy based on poly(thioctic acid) is proposed for developing robust underwater epoxy adhesives. The epoxy curing agent with an adaptive molecular architecture is first synthesized via solvent-free ring-opening polymerization of naturally occurring thioctic acid propelled by dynamic thiol-disulfide exchange. Upon combining the epoxy resin with poly(thioctic acid), the water-resistant long-chain polymers that effectively expel interfacial water and establish multiple interfacial interactions are formed by the first-stage curing via a click reaction between thiol and epoxy groups initiated by the thiol-disulfide exchange mechanism. Subsequently, the second-stage curing is triggered via carboxyl-epoxy reactions and leads to the formation of cross-linked networks. This strategy endows the developed underwater epoxy adhesive with underwater bonding strength up to 16.4 MPa and green recyclability that can be repeatedly disassembled.

A robust TiO ₂ -supported carbon quantum dot (CQD) and CuAg bimetallic nanoparticle (CQDs/CuAg/TiO ₂ ) ternary composite catalyst is developed for improving photothermal catalytic VOCs degradation performance via micro-environmental modulation.

A relay reaction system design strategy, i.e. , the combination between outer active site synergy and inner active site synergy, is proposed to construct an efficient reaction system for selective catalytic reduction of nitrogen oxides with methane.

Plasmonic photochemical N₂ fixation has received widespread attention owing to the attractive plasmonic enhancement effects in improving solar‐to‐NH₃ conversion efficiency. However, the weak N₂ adsorption affinity in metallic plasmonic photocatalysts and insurmountable interfacial barriers in metal–semiconductor plasmonic photocatalysts lead to rapid charge carrier recombination instead of participating in N₂‐to‐NH₃ conversion. Herein, a photothermal catalyst Fe‐dispersed MoO_3−x/MXene with synergistic plasmon resonance hybridization structure is fabricated for photothermal N₂ fixation. The hybrid plasmon resonance effects derived from MXene and MoO_3−x induce a strong optical response across the ultraviolet–visible‐near‐infrared range and generation of energetic charge carriers, and the induced photothermal effect further accelerates electron extraction, transport, and surface reaction kinetics. Moreover, the abundant oxygen vacancies and Fe sites can intensify the N₂ adsorption and donate the energetic electrons into the anti‐bonding system for the stimulative NH coupling process. A high NH₃ formation rate of 87.1 μmol g⁻¹ h⁻¹ is achieved under solar‐level illumination.

A rational design of WO _{3− x} /ZnFe ₂ O _{4− x} broken-gap heterojunction achieved higher charge carrier separation, light-harvesting ability, and good surface reaction, as an all-in-one photocatalyst for H ₂ generation.