Latest ArticlesThe rational design of strong affinity adsorbents for heavy metal ions removal remains a critical challenge for water treatment. In this study, amorphous molybdenum sulfide composites (EDTA-MoSx (x=2, 3)) were fabricated via a facile hydrothermal method mediated by EDTA, which was applied to heavy metal ions (Cu2+, Cd2+, Pb2+, Zn2+ and Ni2+) removal from aqueous solutions. A case study for Cu2+ ions showed that the adsorption capacity of EDTA-MoSx (x=2, 3) was superior to crystalline phase MoS2 at pH 6.0 with an initial concentration of 200 mg/L. Adsorption mechanisms of different sulfide groups and －COOH of EDTA-MoSx (x=2, 3) were verified systematically via a series of experiments, characterizations, and density functional theory (DFT) calculations. Both bridging S22− and －COOH covalently bonded with Cu2+ ions were ascribed to the critical factors for this enhanced removal efficiency on the surface of EDTA-MoSx (x=2, 3). This work offers a new method to enhance the adsorption performance of molybdenum sulfide-based materials by controlling crystallinity mediated with an organic complex small molecule.
As an important component of the atmosphere, ammonia (NH3) plays a very important role in maintaining the balance of environment. However, it is also one of the most toxic gases that can cause damage to the human respiratory system and mucous membranes even at low concentrations. As such, development of highly sensitive and selective NH3 sensors is of high significance for environmental monitoring and health maintenance. Herein, we have synthesized Au@Ag@AgCl core-shell nanoparticles (NPs) by oxidative etching and precipitating Au@Ag core-shell NPs using FeCl3 and further used them as optical probes for the colorimetric detection of NH3. The sensing mechanism is based on the fact that the etching of NH3 on AgCl and Ag shell leads to the variations of ingredients and core-to-shell ratio of the Au@Ag@AgCl NPs, thereby inducing noticeable spectral and color changes. By replacing the outmost layer of Ag with AgCl, not only is the stability of the sensor against oxygen significantly enhanced, but also is the sensitivity of the method improved. The method exhibits good linear relationship for the detection of NH3 from 0 to 5000 μmol/L with the limit of detection of 6.4 μmol/L. This method was successfully applied to the detection of simulated air polluted by NH3, indicating its practical applicability for environmental monitoring. This method shows great potential for on-site NH3 detection particularly in remote area, where a simple, fast, low-cost, and easy-to-handle method is highly desirable.
As a kind of environmentally benign reagents, α-keto acids have been extensively employed as key starting materials in organic synthesis. Organic electrosynthesis has the advantages of reducing byproduct generation, improving the cost-efficiency of synthetic processes, and accessing reactive intermediates under mild conditions. Inspired by the merits of organic electrosynthesis, α-keto acids have shown many synthetic applications in electrochemical acylation, cyclization, and reductive amination reactions with improved efficiencies and selectivities. This review covers the recent breakthroughs achieved in the electrochemical transformations of α-keto acids, aimed at highlighting these electrochemical reactions' features and mechanistic rationalisations. Meanwhile, the practicalities and limitations of these transformations are also presented where possible.
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.
Metal nanocrystals have been recognized as the main catalytic materials in many fields, but insufficient activity and stability, as well as high prices, have limited their large-scale potential applications. As one of the extremely promising alternatives toward metal in boosting their catalytic performance, nonmetallic atoms-doped metal nanocrystals have recently received extensive attention because of their high efficiency, chemical and structural durability, abundant reserve, and low cost. In this review, we highlight the most recent progress in this field and provide insights into their catalytic applications. The metal-nonmetal nanocrystals prepared by doping metal nanocrystals with nonmetallic atoms are introduced and classified based on the types of nonmetallic atoms, including metal hydrides, borides, carbides, nitrides, oxides, phosphides, and chalcogenides. Besides, their applications in catalysis, especially in electrocatalysis and organic catalysis, have been summarized and discussed. Finally, the conclusions and perspectives are given for the catalysis-driven rational design of metal-nonmetal nanocrystals in this minireview.
Different from traditional metal-support heterogenous catalysts, inverse heterogeneous catalysts, in which the surface of metal is decorated by metal oxide, have recently attracted increasing interests owing to the unique interfacial effect and electronic structure. However, a deep insight into the effect of metal-oxide interaction on the catalytic performance still remains a great challenge. In our work, an inverse hematite/palladium (Fe2O3/Pd) hybrid nanostructure, i.e., the active Fe2O3 ultrathin oxide layers partially covering on the surface of Pd nanoparticles (NPs), exhibited superior electrocatalytic performance towards methanol oxidation reaction (MOR) as compared to the bare Pd NPs based on density functional theory calculation. The charge could transfer from Pd to Fe2O3 driven by the built-in potential at the interface of Pd and Fe2O3, which favors the downshift of d band center of Pd. With the assistance of interfacial hydroxyl OH*, the cleavage of OH and CH in CH3OH could take place much easily with lower barrier energy on Fe2O3/Pd than that on pure Pd via two electrons transferring reaction pathways. Our results highlight that the synergy of Pd and Fe2O3 at the interface could facilitate the electrochemical transformation of methanol into formaldehyde assisted with interfacial hydroxyl OH*.
Microbial fuel cells (MFCs) have various potential applications. However, anode is a main bottleneck that limits electricity production performance of MFCs. Herein, we developed a novel anode based on a stainless steel cloth (SC) modified with carbon nanoparticles of Chinese ink (CI) using polypyrrole (PPy) as a building block (PPy/CI/SC). After modification, PPy/CI/SC showed a 30% shorten in start-up time (36.4 ± 3.3 h vs. 52.3 ± 1.8 h), 33% increase in the maximum current (12.4 ± 1.4 mA vs. 9.3 ± 0.95 mA), and 2.3 times higher in the maximum power density of MFC (61.9 mW/m2 vs. 27.3 mW/m2), compared to Ppy/SC. Experimental results revealed that carbon nanoparticles were able to cover SC uniformly, owing to excellent dispersibility of carbon nanoparticles in CI. The attachment of carbon nanoparticles formed a fluffy layer on SC increased the electrochemically-active surface area by 1.9 times to 44.5 cm2. This enhanced electron transfer between the electrode and bacteria. Further, embedding carbon nanoparticles into the PPy layer significantly improved biocompatibility as well as changed functional group contents, which were beneficial to bacteria adhesion on electrodes. Taking advantage of high mechanical strength and good conductivity, a large-size PPy/CI/SC was successfully prepared (50 × 60 cm2) demonstrating a promising potential in practical applications. This simple fabrication strategy offers a new idea of developing low cost and scalable electrode materials for high-performance energy harvesting in MFCs.
CO2 capture is considered as one of the most ideal strategies for solving the environmental issues and against global warming. Recently, experimental evidence has suggested that aluminum double bond (dialumene) species can capture CO2 and further convert it into value-added products. However, the catalytic application of these species is still in its infancy. Both the dynamics mechanism of CO2 fixation and the detailed structures of catalytic intermediates are not well understood. In this work, we investigate the structure dependent resonance Raman (RR) signals for different reaction intermediates. Ab-initio simulations of spontaneous resonance Raman (spRR) and time-domain stimulated resonance Raman (stRR) give spectral signatures correlated to the existence of different intermediates during the CO2-dialumene binding process. The unique Raman vibronic features contain rich structural information with high temporal resolution, enabling to monitor the transient catalytic intermediates under reaction conditions. Our work shows that RR can be used to monitor intermediates during the dialumene based CO2 capture reaction. The spectral features not only provide insight into the structural information of intermediate species, but also allow a deeper understanding of the dynamical details of this kind of catalytic process.
MnOx-CeO2 catalysts are developed by hydrolysis driving redox method using acetate precursor (3Mn1Ce-Ac) and nitrate precursor (3Mn1Ce-N) for the selective catalytic reduction (SCR) of NOx by NH3. A counterpart sample (Cop-3Mn1Ce) was prepared by the NH3·H2O co-precipitation method for comparison purpose. Combining the results of physicochemical properties characterization and performance test, we find that the 3Mn1Ce-Ac catalyst with some nanorod structures is highly active for the deNOx process. The SCR activity of the 3Mn1Ce-Ac catalyst is more admirable than the 3Mn1Ce-N and the Cop-3Mn1Ce catalysts due to plentiful Lewis acid sites, excellent low-temperature reducibility, and superior surface area resulted from O2 generation during the preparation procedure. The 3Mn1Ce-Ac still exhibits the greatest performance for the deNOx process when gaseous acetone is in the SCR feed gas. The NOx conversion and N2 selectivity over the 3Mn1Ce-Ac are both improved by gaseous acetone above 150 ℃ due to the inhibition of SCR undesired side reactions (NSCR & C-O reactions) and "slow-SCR" process.
DNA methyltransferase (DNMT) and histone deacetylase (HDAC) are well recognized epigenetic targets for discovery of antitumor agents. In this study, we designed and synthesized a series of nucleoside base hydroxamic acid derivatives as DNMT and HDAC dual inhibitors. MTT assays and enzymatic inhibitory activity tests indicated that compound 204 exhibited potent DNMT1 and HDAC1/6 inhibitory potency simultaneously in enzymatic levels and at cellular levels, inducing hypomethylation of p16 and hyperacetylation of histones H3K9 and H4K8. Besides, 204 remarkably inhibited proliferation against cancer cells U937 by prompting G0/G1 cell cycle arrest. Molecular docking models explained the functional mechanism of 204 inhibiting DNMT1 and HDAC. Preliminary studies on metabolic profiles revealed that 204 showed desirable stability in liver microsomes. Our study suggested that 204 inhibiting DNMT and HDAC concurrently can be a potential lead compound for epigenetic cancer therapy.
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