Latest ArticlesOxygen evolution reaction (OER) is admitted to an important half reaction in water splitting for sustainable hydrogen production. The sluggish four-electron process is known to be the bottleneck for enhancing the efficiency of OER. In this regard, tremendous efforts have been devoted to developing effective catalysts for OER. In addition to Ir- or Ru-based oxides taken as the benchmark, transition metal carbides have attracted ever-increasing interest due to the high activity and stability as low-cost OER electrocatalysts. In this review, the transition metal carbides for water oxidation electrocatalysis concerning design strategies and synthesis are briefly summarized. Some typical applications for various carbides are also highlighted. Besides, the development trends and outlook are also discussed.
A convenient and regioselective sulfonylation/cyclization of 1,6-enynes with arylazo sulfones has been developed to access a series of sulfonylated γ-butyrolactams. The present reaction could be efficiently conducted under catalyst- and additive-free conditions, in which C—S and C—C bonds were selectively constructed in one-pot procedure.
Integrating silica with organic nanoparticles can generate unique properties. Here pillar[5]arene/silica hybrid vesicles were constructed based on the amphiphilic and rigid properties of pillararenes, as well as the catalytic hydrolysis of tetraethoxysilane. Such vesicles exhibited the high strength of silica and unique molecular recognition of pillararenes, both of which could tune the pH-triggered release behavior. Furthermore, a rhodamine B derivative with hexyl group (RhB-C6) was synthesized, which can form a complex with the pillar[5]arene. Based on the host-guest interaction and high strength of silica, the hybrid vesicles could load more RhB-C6 and the rhodamine B was released more slowly compared with the organic vesicles.
Low-cost silicon microparticles (SiMP), as a substitute for nanostructured silicon, easily suffer from cracks and fractured during the electrochemical cycle. A novel n-type conductive polymer binder with excellent electronic and ionic conductivities as well as good adhesion, has been successfully designed and applied for high-performance SiMP anodes in lithium-ion batteries to address this problem. Its unique features are attributed to the strong electron-withdrawing oxadiazole ring structure with sulfonate polar groups. The combination of rigid and flexible components in the polymer ensures its good mechanical strength and ductility, which is beneficial to suppress the expansion and contraction of SiMP s during the charge/discharge process. By fine-tuning the monomer ratio, the conjugation and sulfonation degrees of the polymer can be precisely controlled to regulate its ionic and electronic conductivities, which has been systematically analyzed with the help of an electrochemical test method, filling in the gap on the conductivity measurement of the polymer in the doping state. The experimental results indicate that the cell with the developed n-type polymer binder and SiMP (~0.5 μm) anodes achieves much better cycling performance than traditional non-conductive binders. It has been considered that the initial capacity of the SiMP anode is controlled by the synergetic effect of ionic and electronic conductivity of the binder, and the capacity retention mainly depends on its electronic conductivity when the ionic conductivity is sufficient. It is worth noting that the fundamental research of this work is also applicable to other battery systems using conductive polymers in order to achieve high energy density, broadening their practical applications.
A Si-substituted rhodamine based water-soluble fluorescent probe bearing a tetrathia-azacrown was designed for fluorescence imaging of Cu+ with substantial affinity and selectivity. In physiological condition, the developed probe with outstanding water-solubility exhibits ultrahigh sensitivity to Cu+, ensuring the reliable fluorescence imaging in vivo.
Porous carbon spheres represent an ideal family of electrode materials for supercapacitors because of the high surface area, ideal conductivity, negligible aggregation, and ability to achieve space efficient packing. However, the development of new synthetic methods towards porous carbon spheres still remains a great challenge. Herein, N-doped hollow carbon spheres with an ultrahigh surface area of 2044 m2/g have been designed based on the phenylenediamine-formaldehyde chemistry. When applied in symmetric supercapacitors with ionic electrolyte (EMIBF4), the obtained N-doped hollow carbon spheres demonstrate a high capacitance of 234 F/g, affording an ultrahigh energy density of 114.8 Wh/kg. Excellent cycling stability has also been achieved. The impressive capacitive performances make the phenylenediamine-formaldehyde resin derived N-doped carbon a promising candidate electrode material for supercapacitors.
Chirality is a fascinating and essential feature of life and highly associated with many significant pharmaceutical, chemical, and biological processes. The construction of chiral recognition platform is a hot research topic and challenging assignment. Herein, we report an electrochemical method by differential pulse voltammetry (DPV) for the enantioselective recognition of chiral drug propranolol (R/S-PPL) through a nanochannel platform based on the N-acetyl-L-cysteine functionalized Pillar[5]arenes derivative NALC-P5 and the porous polycarbonate membrane. The chiral discrimination depends on the difference in the supramolecular host-guest interaction between the chiral NALC-P5 and the R/S-PPL. The transmission rate of the R/S-PPL can be regulated in the nanochannel and we can achieve the selective transport of the chiral drugs. This simple electrochemical technique has potential applications as a general platform for the recognition of chiral molecules.
Polymeric nanomedicine is a promising and rapidly evolving field. Among the different polymeric carriers, polymeric micelle (PM) with nanoscale size exhibit potent physical and biological advantages including excellent solubility and pharmacokinetics, enhanced efficacy and lower toxicity. PM has garnered increasing interest in research and in the clinic. This review will highlight the clinical outcomes of several PM-based formulations, and further summarized their preparation methods, strengths and challenges.
The conversion of chemical feedstock materials into high value-added products accompanied with dehydrogenation is of great value in the chemical industry. However, the catalytic dehydrogenation reaction is inhibited by a limited number of expensive noble metal catalysts and lacks understanding of dehydrogenation mechanism. Here, we report the use of heterogeneous non-noble metal iron nanoparticles (NPs) incorporated mesoporous nitrogen-doped carbon to investigate the dehydrogenation mechanism based on experiment observation and density functional theory (DFT) method. Fe NPs catalyst displays excellent performance in the dehydrogenation of 1, 2, 3, 4-tetrahydroquinoline (THQ) with 100% selectivity and 100% conversion for 10-12 h at room temperature. The calculated adsorption energy implies that THQ prefers to adsorb on Fe NPs as compared with absence of Fe NPs. What is more, the energy barrier of transition state is relatively low, illustrating the dehydrogenation is feasible. This work provides an atomic scale mechanism guidance for the catalytic dehydrogenation reaction and points out the direction for the design of new catalysts.
In this research, a hydroxyl group functionalized metal-organic framework (MOF), UiO-66-(OH)2, was synthesized as a "on-off-on" fluorescent switching nanoprobe for highly sensitive and selective detection of Fe3+, ascorbic acid (AA) and acid phosphatase (ACP). UiO-66-(OH)2 emits yellow-green light under ultraviolet light, when Fe3+ was added, Fe3+ was chelated with hydroxyl group, the electrons in the excited state S1 of the MOF transferred to the half-filled 3d orbits of Fe3+, resulting in fluorescence quenching because of the nonradiative electron/hole recombination annihilation. AA could reduce Fe3+ to Fe2+, which can destroy the electron transfer between UiO-66-(OH)2 and Fe3+ after AA adding, resulted in nonoccurrence of the nonradiative electron transfer, leading to the recovery of UiO-66-(OH)2 fluorescence intensity. The probe can also be used to detect ACP based on the enzymolysis of 2-phospho-L-ascorbic acid (AAP) to produce AA. Benefitting from the hydroxyl group and the characteristics of UiO-66, including the high porosity and large surface area, the developed UiO-66-(OH)2 showed extensive advantages as a fluorescent probe for detection of multi-component, such as high sensitivity and selectivity, colorimetric detection, fast response kinetics and easy to operate, economical and secure. This is the first time to use active group functionalized MOFs as a multi-component sensor for these three substances detection.
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