Latest ArticlesWater electrolysis is considered to be an effective and promising technology to make high-purity H2, however, the relationship between anion species and catalytic performance of electrocatalysts is still not completely clear. Herein, we report an anion engineering strategy to tune electrocatalytic water oxidation activity for Co-based materials. Novel hierarchical Co-based oxide/selenide/phosphide (Co-A, A = O, Se, P) hexagrams have been chosen as model materials. Electrochemical results and theoretical calculations reveal that the electron configuration, the electrical conductivity, and the oxidation potential of Co element in Co-A hexagrams could be moderated by the substitution of P atoms, which leads to the superior OER performance. Particularly, Co-P hexagram displays a low overpotential (η = 269 mV) at j = 10 mA/cm2 for the oxygen evolution reaction (OER) compared to Co-O hexagram (η = 399 mV) and Co-Se hexagram (η = 347 mV). This work is of great importance in understanding coordination atoms (O, Se and P) induced electrocatalytic properties of hierarchical Co-based materials.
Although magnetic stirring is frequently used to enhance the kinetics for adsorption, chemical and biochemical reactions, the introduction of stirrers inevitably leads to the adsorption of analytes and thus interferes with the efficiency of the chemical process or reaction. In this work, magnetic Fe3O4 nanorods with tunable length-to-diameter ratio were synthesized via a hydrothermal method and used as templates for the in-situ depositing of MIL-100(Fe) and gold nanoparticles. Such nanorod-based material can not only function as an adsorbent, nanozyme, and a heterogeneous catalyst for corresponding applications but also serve as a magnetic nanostirrer to enhance kinetics. As a proof-of-concept, the capture of bacteria pathogen, mimic-peroxidase-based colorimetric detection of hydrogen peroxide, and the catalytic reduction of selected organic pollutants were conducted using the as-synthesized Fe3O4@MIL-100(Fe)-Au nanostirrer with and without magnetic field. The results show that the rates of bacteria capture, mimetic enzyme reaction and catalysis were tremendously expedited. We believe this magnetic field-assisted approach holds great promise for future applications, because, not only does it eliminate the use of external magnetic stirrers and thereby decrease the risk of foreign pollution but also, is adaptable for nanoscale reaction systems where conventional stirring is not applicable due to size limitations.
Covalent DNA–protein cross-links are toxic DNA lesions that interfere with essential biological processes, which can cause serious biological consequences, such as genomic instability and protein misexpression. 5-Formyluracil (5fU) as an important modification in DNA, which is mainly from oxidative damage, exists in a variety of cells and tissues. We have reported that 5fU mediated DNA–protein conjugates could exist in human cells [Zhou et al. CCS Chem. 2 (2020) 54-63]. We now aimed to explore its potential biological effects in vitro and in vivo. In this paper, we firstly reported that 5fU intermediated DNA–peptide or DNA–protein conjugates (both were called DPCs) could inhibit different polymerases bypass or cause mutations. Then we further investigated the functional impacts caused by 5fU-mediated DPCs, which appeared in different gene expression components [in the promoter sequence or 5′-untranslated regions (UTR)]. These results together may contribute to a broader understanding of DNA–protein interactions as well as the biological functions associated with 5fU.
Three phthalide-derived analogues, oxaspiroangelioic acids A–C (1–3), were isolated as minor components of an aqueous extract of the Angelica sinensis root heads (guitou). Oxaspiroangelioic acids A and B were racemates separated into enantiomers by chiral HPLC. Their structures including absolute configurations were determined by spectroscopic data analysis, single crystal X-ray diffraction, exciton chirality method and electronic circular dichroism (ECD) calculation. These compounds share an undescribed carbon skeleton, for which biosynthetic pathways are proposed. Compound 1 and its enantiomers showed almost identical activity inhibiting Tandem of P domains in a weak inwardly rectifying K+ channel 1 (TREK-1).
The composite photoanodes composed by cobalt phosphate catalyst (Co−Pi) modified semiconductor have been widely used for solar water splitting, but the improvement mechanism has not been experimentally confirmed. Here we use transient photoelectrochemical measurements and impedance spectroscopy to investigate the effect of Co−Pi catalyst on hematite nanowire photoanode. It is found that under illumination the Co−Pi catalyst can efficiently promote the transfer of photo-generated holes to the Co−Pi layer by increasing the electrical conductivity of the composite structure under a low potential. The Co−Pi catalyst can recombine with photo-generated electrons to reduce the surface recombination efficiency of photo-generated holes and electrons under a high potential. These results provide important new understanding of the performance improvement mechanism for the Co−Pi-modified semiconductor nanowire composite photoanodes.
Electrochemical overall water splitting is attracting a broad focus as a promising strategy for converting the electrical output of renewable resources into chemical fuels, specifically oxygen and hydrogen. However, the urgent challenge in water electrolysis is to search for low-cost, high-efficiency catalysts based on earth-abundant elements as an alternative to the high-cost but effective noble metal-based catalysts. The transition metal-based catalysts are more appealing than the noble metal catalysts because of its low cost, high performance and long stability. Some recent advances for the development in overall water splitting are reviewed in terms of transition metal-based oxides, carbides, phosphides, sulfides, and hybrids of their mixtures as hybrid bifunctional electrocatalysts. Concentrating on different catalytic mechanisms, recent advances in their structural design, controllable synthesis, mechanistic insight, and performance-enhancing strategies are proposed. The challenges and prospects for the future development of transition metal-based bifunctional electrocatalysts are also addressed.
The composite catalytic materials based on the mineral kaolinite are considered to be a potential approach for solving global energy scarcity and environmental pollution, which have excellent catalytic performance, low cost and excellent chemical stability. However, pure kaolinite does not have visible light absorption ability and cannot be used as a potential photocatalytic material. Fortunately, the unique physical and chemical properties of kaolinite can be acted as a good semiconductor carrier. Herein, this paper firstly presents the mineralogical characteristics of kaolinite. Next, kaolinite-based photocatalysts (such as TiO2/kaolinite, g-C3N4/kaolinite, g-C3N4/TiO2/kaolinite, ZnO) are discussed in detail from the formation of heterostructures, synthesis-modification methods, photocatalytic mechanisms, and electron transfer pathways. Furthermore, the specific role of kaolinite in photocatalytic materials is summarized and discussed. In addition, the photocatalytic applications of kaolinite-based photocatalysts in the fields of water decomposition, pollutant degradation, bacterial disinfection are reviewed. However, the modification of kaolinite is hard, the manufacture of a large number of kaolinite-based photocatalysts is difficult, the cost of doping noble metals is expensive, and the utilization rate of visible light is low, which limits its application in industrial practice. Finally, this paper presents some perspectives on the future development of kaolinite-based photocatalysts.
The analysis of endogenous glycoproteins and glycopeptides in human body fluids is of great importance for screening and discovering disease biomarkers with clinical significance. However, the presence of interfering substances makes the direct quantitative detection of low-abundance glycoproteins and glycopeptides in human body fluids one of the great challenges in analytical chemistry. Magnetic solid phase extraction (MSPE) has the advantages of easy preparation, low cost and good magnetic responsiveness. Magnetic adsorbents are the core of MSPE technology, and magnetic adsorbents based on different functional materials are widely used in the quantitative analysis of glycoproteins and glycopeptides in human body fluids, making it possible to analyze glycoproteins and glycopeptides with low abundance as well as multiple types, which provides a technical platform for screening and evaluating glycoproteins and glycopeptides in body fluids as disease biomarkers. In this paper, we focus on the recent advances in the application of MSPE technology and magnetic adsorbents for the separation and enrichment of glycoproteins and glycopeptides in human body fluids, and the future trends and application prospects in this field are also presented.
In recent years, lanthanum-based nanomaterials (La-NMs) are selected as an efficient nano-adsorbent for phosphate removal because La3+ has a strong affinity with oxygen-donor atoms from phosphate. Additionally, there are a broad interest and literature base for the effect of different synthesis optimization and environmental parameters on the adsorption performance of La-NMs. A considerable amount of research has also investigated the regeneration and application of La-NMs to real wastewater in a laboratory scale. Based on the literature survey, it was found that La-NMs are often produced via co-precipitation and hydrothermal methods. Moreover, phosphate's adsorption process and behavior onto La-NMs are described well with the pseudo-second-order model and Langmuir model. The interaction mechanism between phosphate and La-NMs are dominated by ligand exchange, surface complexation and electrostatic attraction. Furthermore, phosphate could easily desorb from La-NMs due to the weak H-bonding interaction between phosphate and the H-bond acceptor groups on the surface of La-NMs. Despite the wealth of literature available in this area, there is a lack of systematic review to evaluate the gaps in the use of La-NMs to eliminate phosphate in water. In this review, we mainly summarize and discuss the role and the effect of the synthesis techniques on the physicochemical properties and the adsorption behavior of La-NMs. The possible adsorption mechanism, regeneration efficiency, and the application of La-NMs to the real environmental samples are also presented and highlighted.
MXenes are a group of recently discovered 2D materials and have attracted extensive attention since their first report in 2011; they have shown excellent prospects for energy storage applications owing to their unique layered microstructure and tunable electrical properties. One major feature of MXenes is their tailorable surface terminations (e.g., −F, −O, −OH). Numerous studies have indicated that the composition of the surface terminations can significantly impact the electrochemical properties of MXenes. Nonetheless, the underlying mechanisms are still poorly understood, mainly because of the difficulties in quantitative analysis and characterization. This review summarizes the latest research progress on MXene terminations. First, a systematic introduction to the approaches for preparing MXenes is presented, which generally dominates the surface terminations. Then, theoretical and experimental efforts regarding the surface terminations are discussed, and the influence of surface terminations on the electronic and electrochemical properties of MXenes are generalized. Finally, we present the significance and research prospects of MXene terminations. We expect this review to encourage research on MXenes and provide guidance for usingthese materials for batteries and supercapacitors.
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