Latest ArticlesAqueous zinc metal batteries are considered as promising candidates for next-generation electrochemical energy storage devices, especially for large-scale energy storage, due to the advantages of high-safety, high energy density and low cost. As the bridge connecting cathode and anode, electrolyte provides a realistic operating environment. In alkaline and neutral aqueous zinc metal batteries, issues associated with electrolyte and anode are still intractable. In this review, we reveal the development and evolution of electrolytes for aqueous zinc metal batteries from alkaline to neutral via the description of fundamentals and challenges in terms of comparison and connection. We also elaborate the strategies in electrolytes regulation and highlight the basic roles and progresses in additives engineering.
So far, a clear understanding about the relationship of variable energy band structure with the corresponding charge-discharge process of energy storage materials is still lacking. Here, using optical spectroscopy (red-green-blue (RGB) value, reflectivity, transmittance, UV–vis, XPS, UPS) to study α-Co(OH)2 electrode working in KOH electrolyte as the research object, we provide direct experimental evidence that: (1) The intercalation of OH– ions will reduce the valence/conduction band (VB and CB) and band gap energy (Eg) values; (2) The deintercalation of OH– ions corresponds with the reversion of VB, CB and Eg to the initial values; (3) The color of Co(OH)2 electrode also exhibit regular variations in RGB value during the charge-discharge process.
Bone metastasis, a life-threatening complication of advanced breast cancer, is often accompanied by debilitating pain (cancer-induced bone pain, CIBP) that severely impairs life quality and survival. The concurrent treatment of bone metastases and CIBP remains a clinical challenge because the therapeutic options are limited. In this study, we construct a near-infrared light-activated nano-therapeutic system to meet this conundrum. In detail, sorafenib (SRF) and photosensitizer (chlorin e6, Ce6) are encapsulated into mesoporous hydroxyapatite nanoparticles (HANPs), which are further functionalized with hyaluronic acid (HA) to obtain HA-SRF/Ce6@HANPs system. The designed nanoplatform destroys tumor cells in vitro and in vivo via the synergism of SRF (interrupting the exchange of cystine/glutamate by inhibiting SLC7A11) and photodynamic therapy (PDT, inducing reactive oxygen species generation). The decrease in tumor burden and reduction of extracellular glutamate significantly attenuate CIBP in mice model with developing bone cancer. Moreover, the combination of HA-SRF/Ce6@HANPs and PDT inhibit osteoclasts activation, promote osteoblast differentiation and accelerate bone repair. Overall, the nanoagent with good biocompatibility may provide an effective therapy method for the concurrent treatment of breast cancer bone metastasis and CIBP.
The presence of alkali metals in exhaust gas from stationary resources causes a grand challenge for the practical application of selective catalytic reduction (SCR) of NOx with NH3. Here, alkali-resistant NOx reduction has been successfully implemented via tailoring the electron transfer over Fe and V species on FeVO4/TiO2 catalysts. The strong interaction between Fe and V induced electron transfer from V to Fe and strengthened the adsorption and activation of NH3 and NO over active VOx sites. In the presence of K2O, the strong electron withdrawing effect of Fe offset the electron donating effect of K on the VOx species, thus protecting the active species VOx to maintain the NOx reduction ability. The enhanced adsorption and activation of NH3 allowed SCR reaction to proceed via E-R mechanism even after K2O poisoning. This work elucidated the electronic effects on the alkali metals resistance of traditional ferric vanadate SCR catalysts and provided a promising strategy to design SCR catalysts with superior alkali resistance.
Understanding the relationship between structure and properties is critical to the development of solid-state luminescence materials with desired characteristics and performance optimization. In this work, we elaborately designed and synthesized a pair of mononuclear iridium(Ⅲ) complexes with similar structures but different degrees of cationization. [Ir2-f][2PF6] with two counterions is obtained by simple N-methylation of the ancillary ligand of [Ir1-f][PF6] which is a classic cationic iridium(Ⅲ) complex. Such a tiny modification results in tremendously different optical properties in dilute solutions and powders. [Ir1-f][PF6] exhibits weak light in solution but enhanced emission in solid-state as well as poly(methyl methacrylate) matrix, indicative of its aggregation-induced emission (AIE) activity. On the sharp contrary, [Ir2-f][2PF6] is an aggregation-caused quenching (ACQ) emitter showing strong emission in the isolated state but nearly nonemissive in aggregation states. Benefiting from the appealing characteristics of mechanochromic luminescence and AIE behavior, [Ir1-f][PF6] has been successfully applied in reversible re-writable data recording and cell imaging. These results might provide deep insights into AIE and ACQ phenomenon of iridium(Ⅲ) complexes and facilitate the development of phosphorescent materials with promising properties.
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.
Due to its simplicity, high efficiency, and chemo-selectivity, bioorthogonal chemistry has shown a great application potential in pre-targeting. Currently, four bioorthogonal pairs as targeting tools, including (strept)avidin/biotin, antibody/antigen, oligonucleotide hybridization and IEDDA tools, have been developed and applied in targeted delivery. Nevertheless, all of these tools still suffer from some limitations, such as difficult modification, biochemical fragility and larger molecular weight for biological association tools, as well as chemical instability for IEDDA tools. Synthetic host-guest pairs with relatively small molecular sizes not only possess strong chemical stability, but also have the features of fast conjugation rate, tunable binding affinity, easy modification, and high chemo-selectivity. Consequently, they can be used as a novel non-covalent bioorthogonal tool for pre-targeting. In order to further promote the development of host-guest pairs as novel bioorthogonal tools for pre-targeted delivery, we firstly calculate their conversion rate to make researcher aware of their unique advantages; next, we summarize the recent research progress in this area. The future perspectives and limitations of these unique tools will be discussed. This review will provide a systemic overview of the development of synthetic host-guest pairs as novel bioorthogonal tools for pre-targeting, and may serve as a "go for" resort for researchers who are interested in searching for new synthetic tools to improve pre-targeting.
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.
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.
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