Latest ArticlesHere, silica microspheres were decorated with two-dimensional metal–organic frameworks (2D MOFs) nanosheets and ionic liquids, and evaluated as the mixed-mode stationary phase for chromatographic separation. The ionic liquids were used to assist the synthesis of 2D MOFs nanosheets, and also acted as adhesives among the nanosheets and silica. In contrast with the 2D MOFs-based column without ionic liquids and commercial columns, the prepared column exhibited enhanced chromatographic separation performance for partially hydrophilic compounds such as alkaloids, sulfonamides and antibiotics, etc. In addition to excellent chromatographic repeatability and stability, it has also been verified that the composites could be easily and repeatedly prepared. The relative standard deviation of the retention time of the same type of analyte between the three batches of materials was ranging from 0.21% to 1.7%. In short, these results indicated that the synthesized composites were promising separation material for liquid chromatography, which made it possible to broaden the application of 2D MOFs in the field of chromatography.
Two novel uranium-containing selenotungstates Na3[H19(UO2)2(μ2-O)(Se2W14O52)2]·41H2O (U2) and (NH4)10[H4(SeO)2(UO2)2(H2O)2(H2Se2W14O52)(Se2W14O52)]·66H2O (Se2U2) based on the {Se2W14O52} unit were successfully prepared and fully characterized. To our knowledge, the uranium is firstly introduced into the selenotungstates. Moreover, it is notable that U2 exhibits excellent Lewis acid-base catalytic activities in the condensation cyclization of sulfonyl hydrazides with diketones to synthesize polysubstituted pyrazoles. All the desired products were obtained in moderate to good yields (up to 99%).
Designing a carbon material with a unique composition and surface functional groups for offering high specific capacity in a wide voltage window is of great significance to improve the energy density for the supercapacitor in a cheap and eco-friendly aqueous electrolyte. Herein, we develop an efficient strategy to synthesize a N, O co-doped hierarchically porous carbon (NODPC-1.0) with moderate specific surface area and pore volume as well as rich heteroatoms using a deep eutectic solvent (DES) as an activator. It is found that NODPC-1.0 with a large proportion of pseudocapacitive functional groups (pyrrole-N, pyridine-N and carbonyl-quinone) can work stable in an acidic 2 mol/L Li2SO4 (pH 2.5) electrolyte, exhibiting specific capacities of 375 and 186 F/g at the current densities of 1.0 and 100 A/g, respectively. Also, the assembled symmetric capacitor using the NODPC-1.0 as the active material and 2 mol/L acidic Li2SO4 (pH 2.5) as the electrolyte shows an outstanding energy density of 74.4 Wh/kg at a high power density of 1.44 kW/kg under a broad voltage window (2.4 V). Relevant comparative experiments indicate that H+ of the acidic aqueous electrolyte plays a crucial part in enhancement the specific capacity, and the abundant pseudocapacitive functional groups on the surface of the NODPC-1.0 sample play the key role in the improvement of electrochemical cycle stability under a broad voltage window.
Hydrogen evolution reaction (HER) catalytic electrodes under actual working conditions show interesting mass transfer behaviors at solid (electrode)/liquid (electrolyte)/gas (hydrogen) three-phase interfaces. These behaviors are essential for forming a continuous and effective physical contact region between the electrolyte and the electrode and require further detailed understanding. Here, a case study on 1T-2H phase molybdenum disulfide (MoS2)/carbon fiber paper (CFP) catalytic electrodes is performed. Rapid gas-liquid mass transfer at the interface for enhancing the working area stability and capillarity for increasing the electrode working area is found. The real scenario, wherein the energy utilization efficiency of the as-prepared non-noble metal catalytic electrode exceeds that of the noble metal catalytic electrode, is disclosed. Specifically, a fluid dynamics model is developed to investigate the behavior mechanism of hydrogen bubbles from generation to desorption on the catalytic electrode surface with different hydrophilic and hydrophobic properties. These new insights and theoretical evidence on the non-negligible three-phase interface behaviors will identify opportunities and motivate future research in high-efficiency, stability, and low-cost HER catalytic electrode development.
Developing high-performance electrocatalysts for CO2 reduction reaction (CO2RR) is crucial since it is beneficial for environmental protection and the resulting value-add chemical products can act as an alternative to fossil feedstocks. Nonetheless, the direct reduction of CO2 into long-chain hydrocarbons and oxygenated hydrocarbons with high selectivity remains challenging. Copper (Cu) shows a distinctive advantage that it is the only pure metal catalyst for reducing CO2 into multi-carbon (C2+) products and the certain facets (e.g., (100), (111), (111)) of Cu nanocrystals exhibit relatively low energy barriers for the formation of specific products (e.g., CO, HCOOH, CH4, C2H4, C2H5OH, and other C2+ products). Therefore, extensive studies have been carried out to explore the relationship between the facets of Cu nanocrystals and corresponding catalytic products. In this review, we will discuss the crystal facet-dependent electrocatalytic CO2RR performance in metallic Cu catalysts, meanwhile, the detailed reaction mechanisms will be systematically summarized. In addition, we will provide a personal perspective for the future research directions in this emerging field. We believe this review is helpful to guide the design of high-selectivity Cu-based electrocatalysts for CO2RR.
Self-supported transition-metal single-atom catalysts (SACs) facilitate the industrialization of electrochemical CO2 reduction, but suffer from high structural heterogeneity with limited catalytic selectivity. Here we present a facile and scalable approach for the synthesis of self-supported nickel@nitrogen-doped carbon nanotubes grown on carbon nanofiber membrane (Ni@NCNTs/CFM), where the Ni single atoms and nanoparticles (NPs) are anchored on the wall and inside of nitrogen-doped carbon nanotubes, respectively. The side effect of Ni NPs was further effectively inhibited by alloying Ni with Cu atoms to alter their d-band center, which is theoretically predicted and experimentally proved. The optimal catalyst Ni9Cu1@NCNTs/CFM exhibits an ultrahigh CO Faradic efficiency over 97% at −0.7 V versus reversible hydrogen electrode. Additionally, this catalyst shows excellent mechanical strength which can be directly used as a self-supporting catalyst for Zn-CO2 battery with a peak power density of ~0.65 mW/cm2 at 2.25 mA/cm2 and a long-term stability for 150 cycles. This work opens up a general avenue to facilely prepare self-supported SACs with unitary single-atom site for CO2 utilization.
The natural hematite (α-Fe2O3) is stable and abundant on the earth, as well as with strange electronic band structure and good visible light absorption properties. However, the composition and catalytic performance of natural hematite should be explored. In this study, the photo-assisted hematite nanoparticles activated persulfate (H-NPs/PS/vis) system was constructed. As detected, H-NPs had an irregular agglomerate structure with abundant internal pore and were mainly composed of Fe2O3, SiO2 and TiO2. The system was applied to removing various antibiotic (i.e., lomefloxacin, ciprofloxacin and enrofloxacin with initial concentration of 10 mg/L), achieving high degradation performance of 82.0%, 81.2% and 82.2% after 120, 330 and 240 min, respectively. Moreover, H-NPs had excellent reusability with low metal leaching (Ti leaching percentage lower than 0.01%, Fe dissolution percentage was 0.48%) and stable structure. At last, a possible reaction mechanism of H-NPs/PS/vis system was proposed that lomefloxacin (LOM) was efficiently removed via the synergistic process of components contained in H-NPs with PS and light, involving the generation of •O2−, •OH and SO4•−. Above all, this paper provided a novel application scheme of natural hematite through in-depth and comprehensive experimental exploration.
Genomic deoxyribonucleic acid (DNA) is selected as the ideal carrier for preserving and transmitting the genetic information over the course of evolution. However, the genomic DNA is constantly exposed to various endogenous and environmental threats, causing a diversity of damaged bases, lesions, mismatches and base-pair modifications in the genome, eventually leading to genomic instability and cancers. Base excision repair (BER) is the most important repair mechanism, repairing a variety of DNA damages arising from oxidation, alkylation, methylation, deamination, and hydrolysis reactions. DNA glycosylases are responsible for initiating the first step of the BER pathway through cleaving the N-glycosidic bond between the damaged base and the DNA backbone. However, abnormal DNA glycosylases are associated with a variety of diseases such as cancer, cardiovascular disease, neurological disease and inflammation, suggesting the important role of DNA glycosylases in cancer diagnosis and treatment. Therefore, it is highly desirable to monitor the activity of DNA glycosylases, gaining a deep understanding of the restoration process of damaged DNA and clinical diagnosis. Recently, a series of novel DNA glycosylases detection methods with excellent performance have been developed. In this minireview, we summarize the recent advances in DNA glycosylase assays including amplification-free assay and amplification-assisted assay. Firstly, a brief introduction of amplification-free assay for DNA glycosylase is given. Then, amplification-assisted assays for DNA glycosylases are discussed in detail. Ultimately, the conclusion and prospects of the directions of DNA glycosylase assays are provided.
The solar-driven photocatalytic technology has shown great potential in nitrate (NO3−) pollutants reduction, however, it has been greatly hindered by the complex preparation and high cost of photocatalysts. Herein, a relatively low-cost photocatalyst, rutile and anatase mixed phase TiO2 was synthesized by a facile microwave-hydrothermal method. Meanwhile, oxygen vacancy is successfully generated, leading to an acidic surface for strong adsorption towards NO3−, which further improved the reduction activity. Compared with the commercial P25, a higher NO3− conversion of ca. 100% and nitrogen (N2) selectivity of 87% were achieved under UV (365 nm) irradiation within 2 h. This research provides a promising strategy for designing efficient noble metal free photocatalyst in the NO3− reduction.
The multiple sensing provides booming options to eliminate interference and ensure the accuracy of detection by mutually coupling and validating multiple data sets. Here, we integrate the jigsaw-like multifunctional mini-pillar platform to perform multi-mode (electrochemical, fluorescence, surface-enhanced Raman scattering (SERS) and colorimetric) sensing in individual microdroplets. Each mini-pillar connector can parallelize together by specific concave-convex interface to form integrated jigsaw-like platform for multi-mode sensing, and each specific mini-pillar can be modified into the individual sensing unit to read the prescribed signals. We successfully implemented electrochemical, fluorescence, SERS and colorimetric detection by multiple signals coupling to reduce the false positive analysis. Such platform brings a promising clue of in-situ analysis and point-of-care testing for disease diagnosis and health monitoring.
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