Latest ArticlesAccurate detection of uric acid (UA) is crucial for diagnosing gout, yet traditional sweat-based UA sensors continue to face challenges posed by complex and costly electrode fabrication methods, as well as weakly hydrophilic substrates. Here, we designed and developed simple, low-cost, and hydrophilic sweat UA detection sensors constructed by carbon electrodes and cellulose paper substrates. The carbon electrodes were made by carbonized polyimide films through a simple, one-step laser engraving method. Our electrodes are porous, possess a large specific surface area, and are flexible and conductive. The substrates were composed of highly hydrophilic cellulose paper that can effectively collect, store, and transport sweat. The constructed electrodes demonstrate high sensitivity of 0.4 µA L µmol−1 cm−2, wide linear range of 2–100 µmol/L. In addition, our electrodes demonstrate high selectivity, excellent reproducibility, high flexibility, and outstanding stability against mechanical bending, temperature variations, and extended storage periods. Furthermore, our sensors have been proven to provide reliable results when detecting UA levels in real sweat and on real human skin. We envision that these sensors hold enormous potential for use in the prognosis, diagnosis, and treatment of gout.
Geminal diboronates and diarylmethyl boronates are versatile building blocks in synthetic chemistry. We here reported a highly efficient approach for the synthesis of gem-bisborylalkanes and diarylmethyl boronates via cobalt-catalyzed deoxygenative borylation of diaryl ketones. This borylation protocol is compatible with a broad range of functionalized aryl groups, providing access to a wide array of boronic esters. The resulting boronic esters can be further transformed to various cross-coupling products and TPEs that represent important structural motifs in organic chemistry and materials science.
The interpretation of heterometallic bonding nature is a basic work of inorganic chemistry. By means of intermetallic substitution of germylene anions with iron halide complexes CpFe(CO)2I and β-diketiminato FeⅡ chloride, the ferrogermylene complexes 3a, 3b and 4a were synthesized and structurally characterized. The structural and IR characterizations show the presence of the Ge←Fe π backbonding in molecules 3a, 3b and 4a. The computational works on frontier molecular orbitals and their comparison of energy states confirmed that σ donation and π backbonding are both weak in these molecules, despite three complexes have longer Ge-Fe bonds, whose strength decreases slightly with the degressive electron density around Fe environment in a sequence from 3a, 3b to 4a.
A meso-molecular muscle was prepared by capping the [c2]daisy chain based on a mono-functionalized copillar[5]arene with an imidazolium group in its axle. From its crystal structure, we observed that it was a cyclic dimer composed of two mirror image subcomponents, a pR- and a pS-copillar[5]arene. Their conformations were fixed by the doubly interlocked mechanical bond. By comparison of the 1H NMR and COSY spectra, we found that the length of this meso-molecular muscle could be controlled not only by the solvents, but also by the counter anions.
Organic electrochemical transistors (OECTs) have emerged as one type of promising building block for neuromorphic systems owing to their capability of mimicking the morphology and functions of biological neurons and synapses. Currently, numerous kinds of OECTs have been developed, while self-healing performance has been neglected in most reported OECTs. In this work, the OECTs using self-healing polymer electrolytes as dielectric layers are proposed. Several important synaptic behaviors are simulated in the OECTs by doping the channel layers with ions from the electrolytes. Benefitting from the dynamic hydrogen bonds in the self-healing polymer electrolytes, the OECTs can successfully maintain their electrical performance and the ability of emulating synaptic behaviors after self-healing compared with the initial state. More significantly, the sublinear spatial summation function is demonstrated in the OECTs and their potential in flexible electronics is also validated. These results suggest that our devices are expected to be a vital component in the development of future wearable and bioimplantable neuromorphic systems.
The design and syntheses of metal-organic cages (MOCs) based on polyoxometalates (POMs) building blocks have attracted increasing attention due to their intriguing molecular architectures and physicochemical properties. In this work, we have successfully synthesized and systematically characterized a tetrahedral polyoxometalate-based organic cage (POC), K3Na17H12[(C4H6O6)6[Ni4(OH)3(A-α-SiW9O34)]4]·96H2O (Ni16L6(SiW9)4), using tritopic Ni4-substituted Keggin cluster (Ni4SiW9) as nodes and flexible L-(+)-tartaric acid ligands as linkers. The resulting POC tetrahedron has been firstly investigated as efficient catalyst for visible-light-driven hydrogen production, achieving a turnover number of 15,500 after 96-h photocatalysis. Such high catalytic performance of Ni16L6(SiW9)4 POC catalyst could be attributed to its unique cage structure, thereby offering more efficient catalytic component accessibility. In addition, spectroscopic analyses illustrated the photocatalytic mechanism and the structural stability of the TBA-Ni16L6(SiW9)4 catalyst during the photocatalytic process.
Artificial Z(S)-scheme photocatalytic water splitting systems have attracted extensive attention due to their advantages such as wide light absorption range, high charge separation efficiency and strong carrier redox ability. However, it is still challenging to design and prepare Z(S)-scheme photocatalysts with low-cost and highly stability for efficiently photocatalytic overall water splitting using solar energy. This review mainly introduces various strategies to improve the photocatalytic water splitting performance of Z(S)-scheme systems. These strategies mainly focus on enhancing or extending the range of light absorption, promoting charge separation, and enhancing surface redox reaction in Z(S)-scheme systems. Finally, the main challenges of Z(S)-scheme photocatalytic water splitting systems and their future development directions are pointed out. This review would be beneficial to understanding the challenges and opportunities faced by the research field of Z(S)-scheme photocatalytic systems, and has important guiding significance for the development and utilization of high-performance Z(S)-scheme photocatalytic reaction system in the future.
Biomass is the most bountiful renewable carbon resource on earth. Photocatalytic transformation is a promising method to utilize biomass to obtain high-value-added chemicals and it has more obvious advantages compared with thermochemical and biological processes due to the milder operational conditions, fewer reagents and equipment. Semiconductor material is one of the most common kinds of heterogeneous biomass photocatalysts, which has the advantages of high selectivity, stable catalytic performance, long activation time, and low cost. In this paper, the significant research progress on the photocatalytic transformation of biomass with semiconductor materials to produce high-value-added chemicals is reviewed, and the three most typical semiconductor photocatalysts (TiO2, CdS, and g-C3N4) are detailed. The photocatalytic mechanism and photocatalytic system optimization including structural modification, metal co-catalyst loading, and introduction of heterojunction are presented. Besides, the main problems, the development direction and trend of semiconductor materials in photocatalytic transformations of biomass in the future are prospected, which provide guidance and inspiration for the further development of semiconductor photocatalysts and make contributions to the progress in efficient utilization of biomass.
A new strategy for the metal-free coordination–insertion ring-opening polymerization of tetrahydrofuran by the central metalloid Boron has been first identified. Bis(pentafluorophenyl)(phenoxy)borane was used as a catalyst for the polymerization reaction system. And polytetrahydrofuran with high molecular weight and narrow molecular weight distribution could be obtained. The proposed mechanism was studied by MALDI-TOF, ESI-MS and O-18 isotope labeling analyses as a metal-free coordination insertion mechanism.
Nitrene transfer reactions are powerful tools in synthetic organic chemistry. In recent years, transition-metal catalyzed nitrene transfer reactions with carbamates as the nitrene precursors have been widely pursued. Such species undergoes facile C−H amination, aziridination, and bifunctionalization of alkenes under the catalysis of different transition metals including Rh, Fe, Ru and others, enabling the efficient construction of various nitrogen-containing molecules. In this review, the recent developments in nitrene transfer reactions with carbamates via N−O bond cleavage were introduced based on different types of reaction, and the key mechanistic information and synthetic applications of the methodologies were discussed.
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