Latest ArticlesRare earth luminescence has attracted widespread attention for several decades, among which near-infrared (NIR) light-related up-conversion luminescence and NIR-Ⅱ luminescence are widely used in the biomedical field. The NIR-related luminescence is widely studied due to the excellent performance, such as good biocompatibility, deep tissue penetration depth, low self-fluorescence and minimal light damage to organisms. In this review, we mainly introduce the mechanism for rare earth up-conversion luminescence, NIR-Ⅱ luminescence and conclude their advantages compared with traditional luminescence. These excellent priorities provide the basis for NIR-related luminescence bioimaging in vivo. Additionally, we hilglight the scheme for the sensitive detection of substances in organisms and various methods for biological therapy. In spite of the existing research, it is outlined that NIR-related luminescence has great potential to be applied in different aspects, expanding perspectives and future challenges of research in related fields. Based on the current scientific achievements, this review can provide reference for research in the areas mentioned above, expand the research direction and arouse a broad interest in different disciplines to pay attention to rare earth luminescence.
Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer, regulate adsorption energy of reaction intermediates, and provide additional active sites, which are regarded as valid means for improving catalytic activity. However, the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains unclear. Herein, the growth of a bifunctional NiCo/NiCoP Mott-Schottky electrode with abundant phosphorus vacancies on foam nickel (NF) has been synthesized through continuous phosphating and reduction processes. The obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities, and the overpotentials for OER and HER are as low as 117 and 60 mV at 10 mA/cm2 in 1 mol/L KOH, respectively. Moreover, as both the cathode and anode of overall water splitting, the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10 mA/cm2, which are far exceeding the benchmark commercial electrodes. DFT theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor, tailor the electronic structure of the metal centers and lower the Gibbs free energy of the intermediates. Furthermore, the unique self-supported integrated structure is beneficial to facilitate the exposure of the active site, avoid catalyst shedding, thus improving the activity and structural stability of NiCo/NiCoP. This study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.
Microfluidic combined with magnetic field have been demonstrated to be the promising solutions for fast and low-damage particles separation. However, the difficulties in the precise layout of magnets and accurate prediction of particle trajectories lead to under and over separation of target particles. A novel particle separation lab-on-chip (LOC) prototype integrated with microstructures and micropolar arrays is designed and characterized. Meanwhile, a numerical model for the separation of magnetic particles by the synergistic effect of geometry-induced hydrodynamics and magnetic field is constructed. The effect of geometry and magnetic field layout on particle deflection is systematically analyzed to implement accurate prediction of particle trajectories. It is found that the separation efficiency of magnetic particles increased from 50.2% to 91.7% and decreased from 88.6% to 85.7% in the range of depth factors from 15 µm to 27 µm and width factors from 30 µm to 60 µm, respectively. In particular, the combined effect of the offset distance of permanent magnets and the distance from the main flow channel exhibits a significant difference from the conventional perception. Finally, the developed LOC prototype was generalized for extension to arbitrary systems. This work provides a new insight and robust method for the microfluidic separation of magnetic particles.
The construction of hydrogels with good mechanical properties and phosphorescent properties is full of challenges. Herein, we report a supramolecular phosphorescent hydrogel with long lifetime, high tensile strength and self-healing property, which can be easily constructed through in-situ thermal-initiated polymerization of isocyanatoethyl acrylate-modified β-cyclodextrin (β-CD-DA) and acrylate-modified adamantane (Ad-DA), acrylic acid (AA), followed by the non-covalent association with carbon dots (CNDs). The lifetime of phosphorescent hydrogel can reach 1261 ms at room temperature, and the quantum yield is 11%. Importantly, through the efficient triplet to singlet Förster resonance energy transfer (TS-FRET), the phosphorescent hydrogel shows the good phosphorescence energy transfer property for organic dyes Rhodamine B and Eosin Y with the delayed fluorescence lifetime up to 730 ms and 585 ms as well as the energy transfer efficiency (ΦET) up to 99.9% and 99.3%, respectively. Moreover, owing to the host-guest interactions between β-CD-DA and Ad-DA, the three-dimensional cross-linked network phosphorescent hydrogel can be easily stretched to 18 times of its original length, and can achieve self-healing of the cut surfaces within 30 min. These results will expand the scope of phosphorescent materials and provide new ideas and opportunities for materials science.
Stimuli-responsive smart materials exhibit reverse chemical/physical changes in response to external stimuli and research on stimuli-responsive smart materials with self-powered properties is still uncultivated ground. Here, we report perovskite crystalline self-powered multiple stimuli-responsive materials triggered by chemical and thermal stimuli. [HMEP]PbI3·(H2O) (1; HMEP is a hydroxytris(1-methylethyl)phosphorus cation) crystallizes in a chiral space group P21 at 293 K and has the piezoelectric reaction (d33 = 10 pC/N and output voltage = 1 V) of self-powered modes, this value is larger than the value of 3 pC/N for the classical piezoelectric material ZnO. Piezoelectric materials can generate energy due to mechanical deformation, and using thermal heating to lose water, [HMEP]PbI3 (2) can be obtained. 2 crystallizes in the non-centrosymmetric space group, undergoes two reversible phase transitions at 243/255 K and 315/348 K, and shows second harmonic generation switching. Interestingly, 2 can return to the hydrated form 1 after absorbing water. This work will lay the foundation for self-powered stimuli-responsive compounds and contribute to the construction of novel organic-inorganic hybrid materials with second harmonic generation switching.
Biomass pyrolysis oil can be improved effectively by electrocatalytic hydrogenation (ECH). However, the unclear interactions among different components lead to low bio-oil upgrading efficiency in the conversion process. Herein, benzaldehyde and phenol, as common compounds in bio-oil, were chosen as model compounds. The interactions between the two components were explored in the ECH process by combining experiments and theoretical calculations. Results showed that phenol could accelerate the conversion of benzaldehyde in the ECH. The selectivity of benzyl alcohol was increased from 60.9% of unadded phenol to 99.1% with 30 mmol/L phenol concentration at 5 h. Benzaldehyde inhibited the ECH of phenol. In the presence of benzaldehyde, the conversion rate of phenol was below 10.0% with no cyclohexanone and cyclohexanol formation at 5 h. The density functional theory (DFT) calculations revealed that the phenol could promote the adsorption of benzaldehyde and facilitate the targeted conversion of benzaldehyde on the active site by lowering the reaction energy barrier. The research on the interaction between phenol and benzaldehyde in the ECH provides a theoretical basis for the application of ECH in practical bio-oil upgrading.
Two-dimensional (2D) carbon nitride sheets (CNs) with atomically thin structures are regarded as one of the most promising materials for solar energy conversion. However, due to their substantially enlarged bandgap caused by the strong quantum size effect and their incomplete polymerisation with a large number of non-condensed surface amino groups, the practical applicability of CNs in photocatalysis is limited. In this study, CNs with broad visible-light absorption were synthesised using a 5-min fast thermal annealing. The removal of uncondensed amine groups reduces the bandgap of CNs from 3.06 eV to 2.60 eV, increasing their absorption of visible light. Interestingly, the CNs were distorted after annealing, which can differentiate the spatial positions of electrons and holes, enhancing the visible-light absorption efficiency. As a result, when exposed to visible light, the photocatalytic hydrogen production activity of atomically thin 2D CNs rose by 8.38 times. This research presents a dependable and speedy method for creating highly effective visible-light photocatalysts with narrowed bandgaps and improved visible-light absorption.
Predictive modeling of photocatalytic NO removal is highly desirable for efficient air pollution abatement. However, great challenges remain in precisely predicting photocatalytic performance and understanding interactions of diverse features in the catalytic systems. Herein, a dataset of g-C3N4-based catalysts with 255 data points was collected from peer-reviewed publications and machine learning (ML) model was proposed to predict the NO removal rate. The result shows that the Gradient Boosting Decision Tree (GBDT) demonstrated the greatest prediction accuracy with R2 of 0.999 and 0.907 on the training and test data, respectively. The SHAP value and feature importance analysis revealed that the empirical categories for NO removal rate, in the order of importance, were catalyst characteristics > reaction process > preparation conditions. Moreover, the partial dependence plots broke the ML black box to further quantify the marginal contributions of the input features (e.g., doping ratio, flow rate, and pore volume) to the model output outcomes. This ML approach presents a pure data-driven, interpretable framework, which provides new insights into the influence of catalyst characteristics, reaction process, and preparation conditions on NO removal.
Nicotinamide adenine dinucleotide (NADH) regeneration is necessary for the sustainable application of enzymatic industry. The Rh-based complex [Cp*Rh(bpy)(H)]+ has been widely used as an important mediator in NADH regeneration systems, but it is limited by complexity and high cost. Here, a Z-scheme was constructed by loading Rh onto carbon nitride nanosheets/carbon nitride quantum dots (CN-CNQD). The resultant catalyst achieved a high yield of NADH in a mediator-free (M-free) system of 0.283 mmol L−1 g−1 min−1, which is 5.29 times that of pure CN. ADH enzyme introduction experiments confirmed that the enzyme active product 1,4-NADH could reach 34.21% selectivity in the M-free system. Mechanism research revealed that the heterojunction between CNs and CNQDs improved the NADH regeneration activity in the traditional M-involved system, while Rh loading was proved to optimize the yield and selectivity of 1,4-NADH in M-free system. The immobilized Rh shows more competitiveness than [Cp*Rh(bpy)(H)]+. This study contributes to the construction of an M-free system for further application in greener, lower-cost enzymatic processes.
Photoreduction of CO2 to solar fuels has caused great interest, but suffers from low catalytic efficiency and poor selectivity. Herein, we designed a S-scheme heterojunction (Cu-TiO2/WO3) with Cu single atom to significantly boost the photoreduction of CO2. Notably, the developed Cu-TiO2/WO3 achieved the solar-driven conversion of CO2 to CH4 with an evolution rate of 98.69 µmol g−1 h−1, and the electron selectivity of CH4 reached 88.5%. The yield was much higher than those of pristine WO3, TiO2/WO3 and Cu-TiO2 samples. Experimental and theoretical analysis suggested that the S-scheme heterojunction accelerated charge migration and inhibited the recombination of electron-hole pairs. Importantly, the charge separation effect of the heterojunction meliorated the position of the d-band. The uplifted d-band centers of Cu and Ti on Cu-TiO2/WO3 not only improved the electron interaction between Cu single atoms and substrate-TiO2, accelerated the adsorption and activation of CO2 on the active sites of Cu single atom, but also optimized the Gibbs free energies of CH4 formation pathway, leading to excellent selectivity toward CH4. This work provides new insights into the design of photocatalyst systems with high photocatalytic performance.
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