Mesoporous silica nanoparticles (MSNs), one of the important porous materials, have garnered interest owing to their highly attractive physicochemical features and advantageous morphological ...attributes. They are of particular importance for use in diverse fields including, but not limited to, adsorption, catalysis, and medicine. Despite their intrinsic stable siliceous frameworks, excellent mechanical strength, and optimal morphological attributes, pristine MSNs suffer from poor drug loading efficiency, as well as compatibility and degradability issues for therapeutic, diagnostic, and tissue engineering purposes. Collectively, the desirable and beneficial properties of MSNs have been harnessed by modifying the surface of the siliceous frameworks through incorporating supramolecular assemblies and various metal species, and through incorporating supramolecular assemblies and various metal species and their conjugates. Substantial advancements of these innovative colloidal inorganic nanocontainers drive researchers in promoting them toward innovative applications like stimuli (light/ultrasound/magnetic)‐responsive delivery‐associated therapies with exceptional performance in vivo. Here, a brief overview of the fabrication of siliceous frameworks, along with discussions on the significant advances in engineering of MSNs, is provided. The scope of the advancement in terms of structural and physicochemical attributes and their effects on biomedical applications with a particular focus on recent studies is emphasized. Finally, interesting perspectives are recapitulated, along with the scope toward clinical translation.
Mesoporous silica nanoparticles (MSNs) have garnered enormous interest owing to their highly advantageous physicochemical and morphological attributes. Collectively, progression has been made by modifying the surface of the siliceous frameworks through incorporating diverse supramolecular assemblies. An overview of the fabrication of MSNs and discussions on significant advances in engineering of MSNs, along with their scope toward clinical translation, is provided.
Advanced redox‐polymer materials offer a powerful platform for integrating electroseparations and electrocatalysis, especially for water purification and environmental remediation applications. The ...selective capture and remediation of trivalent arsenic (As(III)) is a central challenge for water purification due to its high toxicity and difficulty to remove at ultra‐dilute concentrations. Current methods present low ion selectivity, and require multistep processes to transform arsenic to the less harmful As(V) state. The tandem selective capture and conversion of As(III) to As(V) is achieved using an asymmetric design of two redox‐active polymers, poly(vinyl)ferrocene (PVF) and poly‐TEMPO‐methacrylate (PTMA). During capture, PVF selectively removes As(III) with exceptional uptake (>100 mg As/g adsorbent), and during release, synergistic electrocatalytic oxidation of As(III) to As(V) with >90% efficiency can be achieved by PTMA, a radical‐based redox polymer. The system demonstrates >90% removal efficiencies with real wastewater and concentrations of arsenic as low as 10 ppb. By integrating electron‐transfer through the judicious design of asymmetric redox‐materials, an order‐of‐magnitude energy efficiency increase can be achieved compared to non‐faradaic, carbon‐based materials. The study demonstrates for the first time the effectiveness of asymmetric redox‐active polymers for integrated reactive separations and electrochemically mediated process intensification for environmental remediation.
Redox‐active polymer materials are exploited for the reactive separation of arsenic oxyanions. The molecular selectivity of a metallopolymer is combined with the electrocatalytic properties of a radical‐based organic electrode to achieve exceptional separation factors and redox‐mediated transformation. This work paves the way for advanced redox‐materials to be used in synergistic electrochemical processes for water purification, chemical and environmental process intensification, and electrocatalysis.
Programmable locomotion of responsive hydrogels has gained increasing attention for potential applications in soft robotics, microfluidic components, actuators, and artificial muscle. Modulation of ...hydrogel pore structures is essential for tailoring their mechanical strength, response speeds, and motion behaviors. Conventional methods forming hydrogels with homogeneous or stepwise‐distributed pore structures are limited by the required compromise to simultaneously optimize these aspects. Here, a heterobifunctional crosslinker enabled hydrothermal process is introduced to synthesize responsive hydrogels with well‐defined gradient pore construction. According to gradient porosity controls, the hydrogels simultaneously exhibit rapid responses to external stimuli, high elasticity/compressibility, and programmable locomotion capability. By incorporating polypyrrole nanoparticles as photothermal transducers, photo/thermal responsive composite hydrogels are formed to enable programmable control of locomotion such as bending, curving, twisting, and octopus‐like swimming under near‐infrared laser stimulation. The tunable pore structures, mechanical properties, and locomotion of this new class of materials make these gradient porous hydrogels potentially suitable for a variety of applications.
Gradient porous elastic hydrogels with rapid and programmable locomotion to thermal‐/photostimulation are obtained through an effective hydrothermal route. According to the gradient porosity control, the hydrogels simultaneously exhibit rapid responses, high elasticity, and anisotropic locomotion. The hydrothermally induced hydrogelation mechanism is applicable to other thermal‐responsive monomers and crosslinkers, opening new avenues for modulating the pore structures of soft materials.
Despite their advantageous morphological attributes and attractive physicochemical properties, mesoporous silica nanoparticles (MSNs) are merely supported as carriers or vectors for a reason. ...Incorporating various metal species in the confined nanospaces of MSNs (M‐MSNs) significantly enriches their mesoporous architecture and diverse functionalities, bringing exciting potentials to this burgeoning field of research. These incorporated guest species offer enormous benefits to the MSN hosts concerning the reduction of their eventual size and the enhancement of their performance and stability, among other benefits. Substantially, the guest species act through contributing to reduced aggregation, augmented durability, ease of long‐term storage, and reduced toxicity, attributes that are of particular interest in diverse fields of biomedicine. In this review, the first aim is to discuss the current advancements and latest breakthroughs in the fabrication of M‐MSNs, emphasizing the pros and cons, the confinement of various metal species in the nanospaces of MSNs, and various factors influencing the encapsulation of metal species in MSNs. Further, an emphasis on potential applications of M‐MSNs in various fields, including in adsorption, catalysis, photoluminescence, and biomedicine, among others, along with a set of examples is provided. Finally, the advances in M‐MSNs with perspectives are summarized.
Despite their captivating physicochemical properties, mesoporous silica nanoparticles are only supported as carriers. To enrich their performance, various metal species are encapsulated in their nanospaces for diverse functionalities. This review provides an overview highlighting the attractive features of these innovative constructs and a synopsis of the current advancements and latest breakthroughs in their potential catalytic and various biomedical applications.
•Enhancement of arsenic removal was achieved by capacitive deionization.•Electrosorption of As(V) is ascribed to electrical double-layer charging.•Removal of As(III) may involve its oxidation to ...As(V) on the anode electrode.•The presence of NaCl or natural organic matter reduces the degree of arsenic removal.
The feasibility of the electro-removal of arsenate (As(V)) and arsenite (As(III)) from aqueous solutions via capacitive deionization was investigated. The effects of applied voltage (0.0–1.2V) and initial concentration (0.1–200mgL−1) on arsenic removal were examined. As evidenced, an enhancement of arsenic removal can be achieved by capacitive deionization. The capacity to remove As(V) at an initial concentration of 0.2mgL−1 on the activated carbon electrode at 1.2V was determined to be 2.47×10−2mgg−1, which is 1.8-fold higher than that of As(III) (1.37×10−2mgg−1). Notably, the possible transformation of arsenic species was further characterized. The higher effectiveness of As(V) removal via electrosorption at 1.2V was attributed to the formation of an electrical double layer at the electrode/solution interface. The removal of As(III) could be achieved by the oxidation of As(III) to As(V) and subsequent electrosorption of the As(V) onto the electrode surface of the anode. The presence of sodium chloride or natural organic matter was found to considerably decrease arsenic removal. Single-pass electrosorption-desorption experiments conducted at 1.2V further demonstrated that capacitive deionization is a potential means of effectively removing arsenic from aqueous solutions.
All‐inorganic CsPbX3 (X=I, Br, Cl) perovskite quantum dots (PQDs) have been investigated because of their optical properties, such as tunable wavelength, narrow band, and high quantum efficiency. ...These features have been used in light emitting diode (LED) devices. LED on‐chip fabrication uses mixed green and red quantum dots with silicone gel. However, the ion‐exchange effect widens the narrow emission spectrum. Quantum dots cannot be mixed because of anion exchange. We address this issue with a mesoporous PQD nanocomposite that can prevent ion exchange and increase stability. We mixed green quantum‐dot‐containing mesoporous silica nanocomposites with red PQDs, which can prevent the anion‐exchange effect and increase thermal and photo stability. We applied the new PQD‐based LEDs for backlight displays. We also used PQDs in an on‐chip LED device. Our white LED device for backlight display passed through a color filter with an NTSC value of 113 % and Rec. 2020 of 85 %.
Points of light: Green CsPbBr3 perovskite quantum dots (PQDs), embedded in mesoporous silica (MP), were mixed with red CsPb(Br0.4I0.6)3 quantum dots in a silicone resin and placed on an InGaN blue chip. The green and red QDs were excited by blue light with λ=450 nm. The resulting PQD white light emitting diode (LED) exhibits a wide color gamut because of its narrow emission wavelength.
The success of laser-foil-printing (LFP) additive manufacturing depends critically on the laser welding of sheet metals onto the substrate or the previous layer during the part fabrication process. ...The welding can be generally categorized into two modes: conduction mode and keyhole mode. In this study, 304L stainless steel parts fabricated by the LFP process using the two laser welding modes are compared. The porosity, microstructure, and tensile properties of the fabricated parts in these two modes are measured and compared in the laser scanning direction (
X
) and part building direction (
Z
). The parts fabricated in the conduction mode have a higher density than those fabricated in the keyhole mode. On the tensile properties, both yield strength (YS) and ultimate tensile strength (UTS) have insignificant differences statistically based on the ANOVA analysis between the tensile specimens fabricated with the two welding modes by the LFP process. However, the conduction-mode parts have higher elongation than the keyhole-mode parts in both the
X
and
Z
directions, and the difference is especially significant in the
Z
direction. By using the electron backscattered diffraction (EBSD), it was found that the much higher ductility for the conduction-mode parts in the
Z
-axis direction is mainly due to the distinct grain boundary interface density in the
Z
-axis direction between the two welding modes.
Checkpoint immunotherapy that inhibits tumour immune evasion has demonstrated significant clinical success. However, the therapeutic response is limited to certain patient populations, and ...immunotoxicity as well as autoimmunity have compromised the therapeutic benefits. Here, we report on an inherently therapeutic fucoidan-dextran-based magnetic nanomedicine (IO@FuDex
) conjugated with a checkpoint inhibitor (anti-PD-L1) and T-cell activators (anti-CD3 and anti-CD28). IO@FuDex
can repair the immunosuppressive tumour microenvironment by reinvigorating tumour-infiltrating lymphocytes, while targeting the nanomedicine via magnetic navigation to the tumour to minimize off-target effects. Treatment that combines IO@FuDex
and magnetic navigation reduces the occurrence of adverse events and extends the median survival from 32 to 63 days with less than 1 per cent dose compared with soluble anti-PD-L1. Thus, we demonstrate the potential of integrating anti-PD-L1 and T-cell activators as a form of inherently therapeutic nanomedicine to augment the therapeutic index of combination checkpoint immunotherapy.
The detection of ultratrace analytes is highly desirable for the non‐invasive monitoring of human diseases. However, a major challenge is fast, naked‐eye, high‐resolution ultratrace detection. ...Herein, a rectangular 3D composite photonic crystal (PC)‐based optoelectronic device is first designed that combines the sensitivity‐enhancing effects of PCs and optoelectronic devices with fast and real‐time digital monitoring. A crack‐free, centimeter‐scale, mechanically robust ellipsoidal composite PCs with sufficient hardness and modulus, even exceeding most plastics and aluminum alloys, are developed. The high mechanical strength of ellipsoidal composite PCs allows them to be hand‐machined into rectangular geometries that can be conformally covered with the centimeter‐scale flat light‐detection area without interference from ambient light, easily integrating 3D composite PC‐based optoelectronic devices. The PC‐based device's signal‐to‐noise ratio increases dramatically from original 30–40 to ≈60–70 dB. Droplets of ultratrace analytes on the device are identified by fast digital readout within seconds, with detection limits down to 5 µL, enabling rapid identification of ultratrace glucose in artificial sweat and diabetes risk. The developed 3D PC‐based sensor offers the advantages of small size, low cost, and high reliability, paving the way for wider implementation in other portable optoelectronic devices.
A photonic crystal‐based optoelectronic device is developed for rapid and real‐time digital monitoring of ultratrace analytes with detection limits down to 5 µL, which is highly desirable for the non‐invasive monitoring of human diseases, such as the quick identification of diabetes from ultratrace glucose in sweat.
Possible association between diabetes mellitus (DM) and Alzheimer's disease (AD) has been controversial. This study used a nationwide population-based dataset to investigate the relationship between ...DM and subsequent AD incidence.
Data were collected from Taiwan's National Health Insurance Research Database, which released a cohort dataset of 1,000,000 randomly sampled people and confirmed it to be representative of the Taiwanese population. We identified 71,433 patients newly diagnosed with diabetes (age 58.74 ± 14.02 years) since January 1997. Using propensity score, we matched them with 71,311 non-diabetic subjects by time of enrollment, age, gender, hypertension, hyperlipidemia, and previous stroke history. All the patients were followed up to December 31, 2007. The endpoint of the study was occurrence of AD.
Over a maximum 11 years of follow-up, diabetic patients experienced a higher incidence of AD than non-diabetic subjects (0.48% vs. 0.37%, p<0.001). After Cox proportional hazard regression model analysis, DM (hazard ratio HR, 1.76; 95% confidence interval CI, 1.50-2.07, p<0.001), age (HR, 1.11; 95% CI, 1.10-1.12, p<0.001), female gender (HR, 1.24; 95% CI, 1.06-1.46, p=0.008), hypertension (HR, 1.30; 95% CI, 1.07-1.59, p=0.01), previous stroke history (HR, 1.79; 95% CI, 1.28-2.50, p<0.001), and urbanization status (metropolis, HR, 1.32; 95% CI, 1.07-1.63, p=0.009) were independently associated with the increased risk of AD. Neither monotherapy nor combination therapy with oral antidiabetic medications were associated with the risk of AD after adjusting for underlying risk factors and the duration of DM since diagnosis. However, combination therapy with insulin was found to be associated with greater risk of AD (HR, 2.17; 95% CI, 1.04-4.52, p=0.039).
Newly diagnosed DM was associated with increased risk of AD. Use of hypoglycemic agents did not ameliorate the risk.