Higher-order Functional Mesostructures

Nanoarchitectonics concept is essential to bridge the gaps between biology and materials chemistry. Based on this fundamental principle, this review article provides pore-engineered nanoarchitectonics for cancer therapy by integrating basic descriptions and exemplifying therapy applications. This review paper briefly summarizes pore-engineered nanoarchitectonics basics according to classification based on material porosity and composition. We discuss how to design mesoporous material and highlight the appealing points of the progress in the clinical translation of mesoporous materials for cancer treatment. Nanoarchitectonics could be an important key concept for future advanced life technologies as well as currently required cancer therapy.

The exquisite structures of biological ion channels provide inspiration for designing and constructing artificial ion channels to achieve analogous functions. Hierarchically engineered heterogeneous nanochannels with excellent ion rectification, selectivity, and gating properties have attracted more and more attention. In this review, we briefly review the recent advances of hierarchically engineered nanochannel systems in terms of pore-on-pore and pore-in-pore structures, with an emphasis on the promising applications, including ion-selective transport, osmotic energy harvesting, separation, and biosensing.

This review highlights the recent advances in the bioapplications of higher-order DNA origami structures at multiple scales. After a brief introduction to the development of DNA origami, we describe the use of DNA origami structures to assist in single-molecule studies, manipulate lipid membranes, direct cell behaviors, and deliver drugs as smart nanocarriers. Our opinions on the current challenges and future directions are also shared.

Due to their unique physical characteristics, surfactants containing fluorocarbon chains form hierarchical patterns of two-dimensional mesoscopic/microscopic self-assemblies on the surface of water. This review describes the overarching physical mechanism, the competitive interplay of line tension and dipole interaction and discusses several key experimental and analytical techniques characterizing the shape, size, correlation, and viscoelasticity of mesoscopic/microscopic self-assemblies on water, which is often non-trivial. Some of the recent biomedical applications, including biomimetic surface coating, contrast agents in multimodal imaging, and controlled delivery, are introduced to highlight how the unique physicochemical properties of fluorinated self-assemblies can be applied in materials science.

2D Ni/ITQ-2-co material prepared by ligand-chelating impregnation approach shows outstanding activity and stability in the conversion of bio-derived triglycerides (TGs) or free fatty acids (FFAs) to diesel range alkanes, beneficially from the highly dispersive Ni nanoclusters and immobilization effect of 2D zeolite.

A freestanding three-dimensional graphdiyne-hollowed FeCoNi Prussian blue analog electrode (h-FeCoNi PBA@GDY) with highly selective and active interfaces was synthesized by in situ growth of GDY layer on the surface of h-FeCoNi PBA for electrocatalytic nitrate reduction reaction (ECNtRR) at ambient temperatures and pressures. Experimental results demonstrate the presence of the unique incomplete charge transfer between metal atoms and GDY can effectively enhance the intrinsic activity and the ability to increase the active sites of the electrocatalyst, promote fast redox switching, and high-density charge transport at the interface resulting in high reaction selectivity, activity and stability for ammonia production.

Gyroid-structured nanoporous chitosan is successfully fabricated by templated crosslinking reaction using nanoporous polymer as a template. A multiple pore-filling process is developed for templated synthesis to give well-ordered nanoporous chitosan. Bio-mimicking from the structural coloration of butterfly wing structure, the nanoporous chitosan with gyroid texture is highly appealing in the application of high reflective materials for UV optical devices.

A core/shell structured hybrid film comprised of N-doped carbon covering on single-wall carbon nanotubes (SWCNTs) were synthesized by a rapid electropolymerization method, which not only contains abundant exposed pyridinic N that leads to excellent catalytic activity for both ORR and OER, but also perfectly inherits the high conductivity, excellent flexibility, and porous structure of original SWCNT film, making it a desirable integrated oxygen electrode for Zn-air batteries.

In this work, we developed a novel fabrication strategy to construct elastic carbon framework electrocatalysts using nanocellulose fibers (CNFs) and carbon nanotubes (CNTs) by directional freeze casting and interfacial assembly to prepare self-supporting flexible air electrodes. The obtained carbon framework has a directional porous structure, and N and S heteroatoms are uniformly doped in the carbon skeleton, showing excellent mechanical flexibility and excellent ORR performance. Moreover, we assembled an all-solid-state flexible zinc-air battery (FZAB), offering a smaller charge/discharge voltage gap and excellent cycling stability. These results demonstrate the potential of flexible carbon frameworks for the utilization and modification of flexible energy storage devices.

In this work, a photodynamic therapy system based on conjugated polymers (CPs) is developed to inhibit the infection of RNA viruses. Three cationic CPs with different backbone structures fluorene-co-phenylene (PFP), thiophene (PMNT), and phenylene vinylene (PPV) exhibit different photoinactivation effects. PPV and PMNT cause effective inactivation of viruses under light irradiation, while SARS-CoV-2 pseudotyped viruses keep infectious after treated by PFP, which is determined by the interactions between CPs with the proteins and gene of viruses. This work preliminarily reveals the effect of CP-virus interactions on their photoinactivation activity and would be beneficial to develop high-efficient antiviral PDT agents.

High-order 3D nanotube arrays (NTAs) arranged from mesoporous 2D N, B, P co-doped carbon network (NBP-CNW) were synthesize by a facile, well-controllable, eco-friendly and sustainable strategy using task-specific ionic liquids as precursors. NBP-CNW-NTAs modified flexible microelectrode was embed in microfluidic electrochemical biosensor chip for real-time tracking H₂O₂ secreted from different cancer cells (i.e., breast cancer cells, hepatoma cells and cervical cancer cells) with or without radiotherapy treatment. Furthermore, the functional microelectrode has been integrated into an implantable probe for in situ minimally invasive detection of surgically resected human breast specimens to identify the tumor tissues from the normal one.

MOFs uniquely combine metal-atom centers and developed organic-based structures. Both features are attractive for catalysis. However, their isolating nature prevents them from effective use in electrocatalysis processes. Modifying the chemical structure to gain electric conductivity often harms its natural advantages. In this study, Borenstein et al. present a new approach to overcoming the non-conductivity of MOF b growing MOF nanoparticles in a conductive carbon host. The host’s porosity controls the MOF nanoparticles’ size and their electric properties while preserving their structure. As a result, the composition efficiently electro-catalyzes carbon dioxide into formic acid at low overpotentials.

A high-performance bacterial cellulose/carbon nanotubes conductive fiber is developed through the in-situ biosynthesis. Through mimicking the structure of muscle fascicles, the composite fiber integrates high strength, high stiffness, high fatigue resistance, and stable electrical performance into one material. Based on those excellent properties, the muscle-inspired fiber is competitive to play a key role in the fields of intelligent fiber-based composites and devices.

Microstructures in organisms are often in quasiordered distribution, which brings specific functions and performance stability. Here, a numerical model was built to demonstrate the structural whiteness caused by the quasiordered state of the tubular architectures in Morpho theseus wing scales. The method is beneficial to tailored disorder in periodic structures to achieve better properties.

We developed a ROS-responsive and controllable nanocarrier (GC-EB) that efficiently delivered a clinically used antifungal drug, voriconazole (VOR). GC-EB-VOR exhibited high penetration through corneal barriers, good retention in the cornea and controllable drug release under low concentrations of ROS. Mechanistically, the successful delivery and accumulation of GC-EB-VOR in the cornea followed by the inhibition of oxidative stress and of the inflammatory response contributed to the therapeutic effect of GC-EB-VOR against fungal keratitis.

An interfacial co-assembly strategy for synthesizing gradient mesoporous hollow silica sheets is reported. The SO₄²⁻ and NH₄⁺ were aggregated by protonated amphiphilic polymer PVP and formed (NH₄)₂SO₄ crystals at the n-pentanol-water interface. Negatively charged silica oligomers can be confined on the (NH₄)₂SO₄ crystal surface by the Coulomb interaction of NH4⁺ and co-assembled with CTAB under the catalysis of ammonia molecules. After removing the (NH₄)₂SO₄ cores and CTAB template by washing and extraction, the first layer of mesoporous hollow silica was formed. Modulating the n-pentanol-water interface to n-hexane-water interface, n-hexane swelled CTAB micelle co-assembled with silica oligomers and formed the second layer of mesoporous silica with larger pore size. The finally obtained gradient mesoporous silica sheet shows remarkable gradient rejection rates for molecules with different sizes.