Highly Twisted Conformation Thiopyrylium Photosensitizers for In Vivo Near Infrared-II Imaging and Rapid Inactivation of Coronavirus

Despite significant effort, a majority of heavy-atom-free photosensitizers have short excitation wavelengths, thereby hampering their biomedical applications. Here, we present a facile approach for developing efficient near-infrared (NIR) heavy-atom-free photosensitizers. Based on a series of thiopyrylium-based NIR-II (1000–1700 nm) dyads, we found that the star dyad HD with a sterically bulky and electron-rich moiety exhibited configuration torsion and significantly enhanced intersystem crossing (ISC) compared to the parent dyad. The electron excitation characteristics of HD changed from local excitation (LE) to charge transfer (CT)-domain, contributing to a ≈6-fold reduction in energy gap (ΔE_ST), a ≈10-fold accelerated ISC process, and a ≈31.49-fold elevated reactive oxygen species (ROS) quantum yield. The optimized SP@HD-PEG_2K lung-targeting dots enabled real-time NIR-II lung imaging, which precisely guided rapid pulmonary coronavirus inactivation.     

High Valence State Sites as Favorable Reductive Centers for High-Current-Density Water Splitting

Electrochemical water splitting is a promising approach for producing sustainable and clean hydrogen. Typically, high valence state sites are favorable for oxidation evolution reaction (OER), while low valence states can facilitate hydrogen evolution reaction (HER). However, here we proposed a high valence state of Co³⁺ in Ni_9.5Co_0.5−S−FeO_x hybrid as the favorable center for efficient and stable HER, while structural analogues with low chemical states showed much worse performance. As a result, the Ni_9.5Co_0.5−S−FeO_x catalyst could drive alkaline HER with an ultra-low overpotential of 22 mV for 10 mA cm⁻², and 175 mV for 1000 mA cm⁻² at the industrial temperature of 60 °C, with an excellent stability over 300 h. Moreover, this material could work for both OER and HER, with a low cell voltage being 1.730 V to achieve 1000 mA cm⁻² for overall water splitting at 60 °C. X-ray absorption spectroscopy (XAS) clearly identified the high valence Co³⁺ sites, while in situ XAS during HER and theoretical calculations revealed the favorable electron capture at Co³⁺ and suitable H adsorption/desorption energy around Co³⁺, which could accelerate the HER. The understanding of high valence states to drive reductive reactions may pave the way for the rational design of energy-related catalysts.     

钒硅沸石中钒的存在状态研究

合成了四种不同Si／V比的V－ZSM－5分子筛，并根据XPS、ESR、TPR及DRS测试，分析了钒在沸石中的存在状态，结果表明，沸石中的钒有两种价态，每一种价态的钒又有两种存在形式，即骨架外高分散的钒（包括沸石外表面上和孔道内的钒）及存在于骨架上的钒。     

ICP-MS测定元素活动态中金的分析方法研究

金的元素活动态是用来指示隐伏金矿床的有效方法,将各相态金完全提取、准确定量分析,可以清晰、明显的指示地壳深部金矿床的有效信息。金的元素活动态提取液经过王水处理后,采用泡塑吸附-硫脲解脱的方式将金分离富集,解脱溶液一般采用石墨炉原子吸收光谱法(GF-AAS)测定,该方法效率低、检出限高、精密度差,数据可信度降低。采用电感耦合等离子体质谱法(ICP-MS)测定可以有效避免GF-AAS法的缺点,实验采用低浓度的硫脲解脱液(0.2g/L),能够将1000ng的金完全解脱,低浓度的硫脲溶液也保证了仪器的长期稳定性;标准溶液采用和提取溶液一致的处理方法(王水分解+泡塑吸附+硫脲解脱),提高了测定结果的准确度。该方法得到了水溶态、粘土吸附态、有机结合态、铁锰氧化物态的检出限：0.012、0.006、0.006、0.014μg/kg,方法精密度：4.63%~18.17%,各相态加和结果和全量的相对误差的绝对值均小于4.94%,表明提取方法和分析方法准确可靠。     

Singlet-Triplet Energy Inversion in Carbon Nitride Photocatalysts

Time-resolved EPR (TR-EPR) demonstrates the formation of well-defined spin triplet excitons in carbon nitride. This permits to experimentally probe the extent of the triplet wavefunction which delocalizes over several tri-s-triazine units. Analysis of the temperature dependence of the TR-EPR signal reveals the mobility of the triplet excitons. By employing monochromatic light excitation in the range 430–600 nm, the energy of the spin triplet is estimated to be ≈0.2 eV above the conduction band edge, proving that the triplet exciton lies above the corresponding singlet. Comparison between amorphous and graphitic forms establishes the singlet-triplet inversion as a general feature of carbon nitride materials.     

Nonlinear denoising of transient signals with application to event-related potentials

We present a new wavelet-based method for the denoising of event-related potentials (ERPs), employing techniques recently developed for the paradigm of deterministic chaotic systems. The denoising scheme has been constructed to be appropriate for short and transient time sequences using circular state space embedding. Its effectiveness was successfully tested on simulated signals as well as on ERPs recorded from within a human brain. The method enables the study of individual ERPs against strong ongoing brain electrical activity.     

Extended Kalman filters using explicit and derivative-free local linearizations

We propose three variants of the extended Kalman filter (EKF) especially suited for parameter estimations in mechanical oscillators under Gaussian white noises. These filters are based on three versions of explicit and derivative-free local linearizations (DLL) of the non-linear drift terms in the governing stochastic differential equations (SDE-s). Besides a basic linearization of the non-linear drift functions via one-term replacements, linearizations using replacements through explicit Euler and Newmark expansions are also attempted in order to ensure higher closeness of true solutions with the linearized ones. Thus, unlike the conventional EKF, the proposed filters do not need computing derivatives (tangent matrices) at any stage. The measurements are synthetically generated by corrupting with noise the numerical solutions of the SDE-s through implicit versions of these linearizations. In order to demonstrate the effectiveness and accuracy of the proposed methods vis-à-vis the conventional EKF, numerical illustrations are provided for a few single degree-of-freedom (DOF) oscillators and a three-DOF shear frame with constant parameters.     

Potential energy curve of Be2 in its ground electronic state

The potential energy curve of Be₂ in its ground electronic state is constructed by morphing accurate MR-CI ab initio potentials from the literature to available experimental ro-vibrational data within the framework of the reduced potential curve (RPC) approach of Jen? and Plíva [Adv. At. Mol. Phys. 19 (1983) 265-307]. The resulting potential energy curves are in close harmony with experiment allowing thus for reliable prediction of the so-far experimentally unprobed part of the molecular potential energy function.     

Delay-dependent stability for 2D systems with time-varying delay subject to state saturation in the Roesser model

This paper addresses the problem of delay-dependent stability of 2D systems with time-varying delay subject to state saturation in the Roesser model. By introducing diagonally dominant matrices, new delay-dependent conditions are obtained in terms of linear matrix inequalities (LMIs) where the lower and upper delay bounds along horizontal and vertical directions, respectively, are known. numerical examples are provided to demonstrate the proposed results.     

Uniformly exponentially stable approximation for the transmission line with variable coefficients and its application

We analyze an ideal transmission line, which is defined by the telegraph equation with variable coefficients, from the perspectives of numerical analysis and control theory in this note. Because the spatially semi-discrete scheme of the original system is insufficient for discussing uniform exponential stability, we apply a similar transform to the continuous system and produce an intermediate system that may be easily analyzed. To begin, we discuss uniform exponential stability for the intermediate system using an so called average central-difference semi-discrete scheme and the direct Lyapunov function approach. The proof is the same as in the continuous case. The Trotter-Kato Theorem is used to demonstrate the stability and consistency of numerical approximation scheme. Finally, we propose a semi-discrete strategy for the original system through an inverse transform. All results on intermediate system are then translated into the original system. The numerical state reconstruction problem is addressed as an essential application of the main results. Furthermore, several numerical simulations are used to validate the effectiveness of the numerical approximating algorithms.