A Catalytically Accessible Polyoxometalate in a Porous Fiber for Degradation of a Mustard Gas Simulant.

Polyoxometalates (POMs) are versatile materials for chemical catalysis due to their tunable acidity and rich redox properties. While POMs have attracted significant attention in homogeneous catalysis, challenges regarding aggregation and instability in solvents often prevent the wide implementation of POMs as heterogeneous catalysts. Therefore, the successful incorporation of a POM into a solid support, such as a polymer, is desirable for practical applications where unique functionalities of the POM combine with the advantages of the polymer. In this work, we showcase how polymers of intrinsic microporosity (PIMs) can serve as matrices for anchoring a pure inorganic Keggin-type POM (H3PW12O40) to fabricate PIM-based composite materials. Specifically, we found that PIMs installed with amidoxime functionalities could successfully attach POMs (PW12@PIM-1-AO) without self-segregation. Furthermore, we fabricated porous fibrous mats via electrospinning of the PIM-POM composites. Comprehensive characterization confirmed the integrity of the POM in the composite material. Following this, we demonstrated that the incorporated POMs in the composite fibers maintained their innate catalytic activity for the oxidative degradation of 2-chloroethyl ethyl sulfide, a sulfur mustard simulant, in the presence of hydrogen peroxide as the oxidant. Ultimately, our work highlights that PIM-based hybrid materials provide a potential route for implementing these reactive fiber mats into protective equipment.

Sponge-like loose and porous SnO2 microspheres with rich oxygen vacancies and their enhanced room-temperature gas-sensing performance.

Structure and surface modification of semiconductor materials are of great importance in gas sensors. In this study, a facile citric acid-assisted solvothermal method via a precise calcination process was leveraged to synthesize sponge-like loose and porous SnO2 microspheres with rich oxygen vacancies (denoted as LP-SnO2-Ov). When this material was used in a gas sensor, it exhibited an extremely high response to 10 ppm hydrogen sulfide gas at room temperature (Ra/Rg = 9688), which was 54 times higher than that of commercial SnO2. Furthermore, the response time of LP-SnO2-Ov was 5 s, while the recovery time was 177 s. Moreover, it displayed such high selectivity and stability for hydrogen sulfide gas that its properties remained almost unchanged after 1 month. This method paves a new way to fabricate materials possessing a sponge-like loose and porous structure with oxygen vacancies, which is promising for many other scientific fields such as lithium-ion batteries and photocatalysis.

Bacterial Genotoxin Accelerates Transient Infection-Driven Murine Colon Tumorigenesis.

Chronic and low-grade inflammation associated with persistent bacterial infections has been linked to colon tumor development; however, the impact of transient and self-limited infections in bacterially driven colon tumorigenesis has remained enigmatic. Here we report that UshA is a novel genotoxin in attaching/effacing (A/E) pathogens, which include the human pathogens enteropathogenic Escherichia coli, enterohemorrhagic E. coli, and their murine equivalent Citrobacter rodentium (CR). UshA harbors direct DNA digestion activity with a catalytic histidine-aspartic acid dyad. Injected via the type III secretion system (T3SS) into host cells, UshA triggers DNA damage and initiates tumorigenic transformation during infections in vitro and in vivo. Moreover, UshA plays an indispensable role in CR infection-accelerated colon tumorigenesis in genetically susceptible Apc MinΔ716/+ mice. Collectively, our results reveal that UshA, functioning as a bacterial T3SS-dependent genotoxin, plays a critical role in prompting transient and noninvasive bacterial infection-accelerated colon tumorigenesis in mice. SIGNIFICANCE: We identified UshA, a novel T3SS-dependent genotoxin in A/E pathogens that possesses direct DNA digestion activity and confers bacterially accelerated colon tumorigenesis in mice. Our results demonstrate that acute and noninvasive infection with A/E pathogens harbors a far-reaching impact on the development of colon cancer.This article is highlighted in the In This Issue feature, p. 1.

Limited Cross-Linking of 4-1BB by 4-1BB Ligand and the Agonist Monoclonal Antibody Utomilumab.

Monoclonal antibodies (mAbs) targeting the co-stimulatory molecule 4-1BB are of interest for tumor immunotherapy. We determined the complex structures of human 4-1BB with 4-1BB ligand (4-1BBL) or utomilumab to elucidate the structural basis of 4-1BB activation. The 4-1BB/4-1BBL complex displays a typical TNF/TNFR family binding mode. The structure of utomilumab/4-1BB complex shows that utomilumab binds to dimeric 4-1BB with a distinct but partially overlapping binding area with 4-1BBL. Competitive binding analysis demonstrates that utomilumab blocks the 4-1BB/4-1BBL interaction, indicating the interruption of ligand-mediated signaling. The binding profiles of 4-1BBL and utomilumab to monomeric or dimeric 4-1BB indicate limited cross-linking of 4-1BB molecules. These findings provide mechanistic insight into the binding of 4-1BB with its ligand and its agonist mAb, which may facilitate the future development of anti-4-1BB biologics for tumor immunotherapy.