Halogenated Ti3C2 MXenes Prepared by Microwave Molten Salt for Hg0 Photo-Oxidation

Ti₃C₂ MXenes with different halogen modifications are prepared rapidly and efficiently by microwave molten salt method, and the MXene surface functional group modification is successfully achieved to address the problems of low purity, complex functional groups, and uncontrollable energy band structure of MXenes obtained by traditional liquid phase etching. Among them, the modification of the iodine (I) functional group onto the surface of Ti₃C₂ changes the energy band structure and band gap, resulting in easier photoexcitation and more photogenerated carriers. The increased Fermi energy is closer to the conduction band, the decreased surface work function weakens the electron confinement ability. The photogenerated carriers can migrate to the surface of the material more easily with extended lifetime, so the activity of the catalyst is improved. Further, for gaseous monomeric mercury (Hg⁰) photo-oxidative removal, Ti₃C₂-I₂ exhibits 85.5% efficiency of Hg⁰ photo-oxidative removal under visible light. Based on the experimental characterization and density functional theory calculations, a mechanism for the photo-oxidative removal of Hg° from Ti₃C₂-I₂ MXene is proposed, which provides a valuable strategy for studying Ti₃C₂ MXenes in the field of photocatalysis.     

Frontiers in Circularly Polarized Phosphorescent Materials

Circularly polarized luminescence (CPL) materials have received increasing attention in recent years. Amongst various CPL materials, circularly polarized phosphorescence (CPP) materials featuring long life-time represent a novel research frontier and exhibit promising applications in various fields. Herein, the state-of-the-art advances of CPP materials are systematically summarized, as classified into transition metal complexes, organic small molecules, polymers, and organic/inorganic hybrid materials. Besides, the recent applications of CPP materials in organic light-emitting diodes and encryption display are also summarized. Furthermore, the current challenges and future perspectives are put forward. It is expected that this review will offer more inspirations for the future rational design of advanced CPP materials, thus further promoting their future practical applications.     

Pre-Activation of CO2 at Cobalt Phthalocyanine-Mg(OH)2 Interface for Enhanced Turnover Rate

Cobalt phthalocyanine (CoPc) anchored on heterogeneous scaffold has drawn great attention as promising electrocatalyst for carbon dioxide reduction reaction (CO₂RR), but the molecule/substrate interaction is still pending for clarification and optimization to maximize the reaction kinetics. Herein, a CO₂RR catalyst is fabricated by affixing CoPc onto the Mg(OH)₂ substrate primed with conductive carbon, demonstrating an ultra-low overpotential of 0.31 ± 0.03 V at 100 mA cm⁻² and high faradaic efficiency of >95% at a wide current density range for CO production, as well as a heavy-duty operation at 100 mA cm⁻² for more than 50 h in a membrane electrode assembly. Mechanistic investigations employing in situ Raman and attenuated total reflection surface-enhanced infrared absorption spectroscopy unravel that Mg(OH)₂ plays a pivotal role to enhance the CO₂RR kinetics by facilitating the first-step electron transfer to form anionic *CO₂⁻ intermediates. DFT calculations further elucidate that introducing Lewis acid sites help to polarize CO₂ molecules absorbed at the metal centers of CoPc and consequently lower the activation barrier. This work signifies the tailoring of catalyst-support interface at molecular level for enhancing the turnover rate of CO₂RR.     

Magnetic Large-Mesoporous Nanoreactors Enable Enzymatically Regulated Background-Free and Persistently Signalling Diseases Diagnosis

Diverse diseases and increasing prevalence pose a serious threat to public health. Point-of-care testing (POCT) techniques have imposed superior requirements over sensitivity, selectivity, robustness, affordability, and high-throughput. However, transient signal, complex sample pretreatment, and low signal-to-noise ratio make POCT severely limited in detection accuracy, efficiency, and sensitivity. Here, an enzyme-assisted magnetic large-mesoporous nanoreactor (FS) is constructed for achieving persistent-chemiluminescence signal output and eliminating matrix interference in disease diagnosis. The core-shell structured FS synthesized via an interface coassembly method exhibits uniform size, large and open mesopores (≈22 nm), and intrinsic magnetic separability. Such unique FS acts as efficient nanoreactor for confined cascade reactions enable efficient persistent-chemiluminescence (pCL) signal transduction and high-SNR chromogenic analysis of diverse biomarkers. The developed pCL assays facilitate high-sensitive determination of chronic disease biomarkers glucose and uric acid with detection limits (DL) of 5.4 mg L⁻¹ and 151.2 ng L⁻¹, respectively. The proposed chromogenic immunoassay enables an ultrasensitive and visual determination of alpha-fetoprotein with a DL of 1.2 ng L⁻¹, which is superior to previously published immunoassays. The feasibility of the developed methods for real-world applications are demonstrated in 159 clinical serum samples, and the determination results agree well with the clinical data. The proposed technique is expected to promote highly sensitive disease diagnosis in primary medical institutions and resource-limited areas since not relying on expensive automatic sampling and testing instruments. The good flexibility of the customizable nanoreactor makes it a powerful tool for developing various POCT techniques for rapid, sensitive, and accurate diseases diagnosis.     

Spidermen Strategy for Stable 24% Efficiency Perovskite Solar Cells

The interface energetics-modification plays an important role in improving the power conversion efficiency (PCE) among the perovskite solar cells (PSCs). Considering the low carrier mobility caused by defects in PSCs, a double-layer modification engineering strategy is adopted to introduce the “spiderman” NOBF₄ (nitrosonium tetrafluoroborate) between tin dioxide (SnO₂ and perovskite layers. NO⁺, as the interfacial bonding layer, can passivate the oxygen vacancy in SnO₂, while BF₄⁻ can optimize the defects in the bulk of perovskite. This conclusion is confirmed by theoretical calculation and transmission electron microscopy (TEM). The synergistic effect of NO⁺ and BF₄⁻ distinctly heightens the carrier extraction efficiency, and the PCE of PSCs is 24.04% with a fill factor (FF) of 82.98% and long-term stability. This study underlines the effectiveness of multifunctional additives in improving interface contact and enhancing PCE of PSCs.     

Circularly polarized patch antenna with simultaneously wide frequency tuning range and high gain performance

A tunable circularly polarized square patch antenna with parasitic elements is designed for a wide frequency tuning range and high gain characteristics. The proposed antenna is constructed by one main patch and four semi-elliptic parasitic units. By loading four varactor diodes and adjusting their capacitance values, the tunable feature is performed to reallocate the corresponding working frequency. Moreover, the diagonal corners of the antenna are cut and loaded with varactor diodes, which provide the appropriate perturbation between the two orthogonality modes of the antenna, so as to ensure the circular polarization characteristic in the entire operating tuning band. The experimental results demonstrate that the reflection coefficient and axial ratio are less than −13 dB and 3 dB, respectively. The proposed antenna features a relatively wide continuously tuning range of 24% within 1.9-2.3 GHz and a stable gain of over 7 dBi with a radiation efficiency of above 85%.     

基于分段电容阵列的改进型逐次逼近型ADC

为缩短高速模数转换器(ADC)中高位(MSB)电容建立时间以及减小功耗,提出了一种基于分段式电容阵列的改进型逐次逼近型(SAR)ADC结构,通过翻转小电容阵列代替翻转大电容阵列以产生高位数字码,并利用180 nm CMOS工艺实现和验证了此ADC结构。该结构一方面可以缩短产生高位数码字过程中的转换时间,提高量化速度;另一方面其可以延长大电容的稳定时间,减小参考电压的负载。通过缩小比较器输入对管的面积以减小寄生电容带来的误差,提升高位数字码的准确度。同时,利用一次性校准技术减小比较器的失配电压。最终,采用180 nm CMOS工艺实现该10 bit SAR ADC,以验证该改进型结构。结果表明,在1.8 V电源电压、780μW功耗、有电路噪声和电容失配情况下,该改进型SAR ADC得到了58.0 dB的信噪失真比(SNDR)。     

Entrapment of both glucose oxidase and peroxidase in regenerated silk fibroin membrane

Two enzmyes, glucose oxidase and peroxidase, were for the first time simultaneously immobilized in regenerated silk fibroin membrane. The structure and morphology of the regenerated silk fibroin membrane containing both glucose oxidase and peroxidase were investigated with IR spectra and SEM. The bienzymes do not change the structures of the regenerated silk fibroin in the membrane, which has an islands-sea structure. For the first time, an amperometric methylene green mediating sensor for glucose based on co-immobilization of both glucose oxidase and peroxidase in regenerated silk fibroin was constructed. Cyclic voltammetry and amperometry were used to test the suitability of methylene green shuttling electrons between peroxidase and the glassy carbon electrode. The bienzyme-based system offers fast response and high sensitivity of the sensor to glucose. The effects of pH, temperature, and the concentration of the mediator on the response current were evaluated, and the dependence of the Michaelis-Menten constant K_m^app on the concentration of the mediator was investigated.