Metal-Organic Frameworks-derived Indium Clusters/Carbon Nanocomposites for Efficient CO2 Electroreduction

Electrochemical reduction of carbon dioxide into value-added products is a promising way to recycle the greenhouse gas, thus solving the crisis of global warming. Pressing challenges remain in regulating the catalytic selectivity. In this work, we demonstrated a metal-organic frameworks-assisted approach to synthesizing In species loaded on the surface of N doped carbon matrix. By controlling the particle sizes, the catalytic selectivity can be easily altered. The obtained In_c/NC possesses the outstanding capability for converting CO₂ into CO. And 80.09% Faraday efficiency (FE) of CO can be achieved at 0.8 V vs. RHE. While the In₂O₃/C exhibits different catalytic behaviors, the main product is formic acid and the FE is more than 50% at 0.8 V vs. RHE. The selectivity reversal can be attributed to the strong interactions between In clusters and N atoms of carbon supports, which efficiently inhibits the formation of the by-product, formic acid. Our research has paved a new way to modulate catalytic selectivity by manipulating the fine structures of the catalysts.     

Sigma-1 Receptor Agonist TS-157 Improves Motor Functional Recovery by Promoting Neurite Outgrowth and pERK in Rats with Focal Cerebral Ischemia

Sigma-1 (σ-1) receptor agonists are considered as potential treatment for stroke. TS-157 is an alkoxyisoxazole-based σ-1 receptor agonist previously discovered in our group. The present study describes TS-157 profile in a battery of tests for cerebral ischemia. Initial evaluation demonstrated the compound’s safety profile and blood–brain barrier permeability, as well as its ability to induce neurite outgrowth in vitro. The neurite outgrowth was shown to be mediated via σ-1 receptor agonism and involves upregulation of ERK phosphorylation (pERK). In particular, TS-157 also significantly accelerated the recovery of motor function in rats with transient middle cerebral artery occlusion (tMCAO). Overall, the results herein support the notion that σ-1 receptor agonists are potential therapeutics for stroke and further animal efficacy studies are warranted.     

紫外光辐照对TiO2纳米线电输运性能的影响及磁阻效应研究

采用溶胶凝胶法以及静电纺丝法, 利用热处理工艺, 成功制备出了多晶锐钛矿型TiO₂纳米线, 通过两线法在室温下测试单根TiO₂纳米线的V-I曲线来研究其电输运性能及磁阻效应. 结果表明: 在无光照环境下其V-I曲线为不过零点的直线, 零场电阻较大, 在磁场作用下电阻下降, 表现出负磁阻效应; 紫外光辐照环境下TiO₂纳米线载流子浓度增加使得电阻变小, 然而在磁场作用下电阻增大, 表现为正磁阻效应. 紫外光辐照导致的载流子浓度变化, 使得负磁阻转变为正磁阻, 我们将磁阻变化归结为d电子局域导致的负磁阻与能带劈裂导致的正磁阻两种机理相互竞争的结果.     

Tomonaga-Luttinger liquid features in ballistic single-walled carbon nanotubes: conductance and shot noise

We study the electrical transport properties of well-contacted ballistic single-walled carbon nanotubes in a three-terminal configuration at low temperatures. We observe signatures of strong electron-electron interactions: the conductance exhibits bias-voltage-dependent amplitudes of quantum interference oscillation, and both the current noise and Fano factor manifest bias-voltage-dependent power-law scalings. We analyze our data within the Tomonaga-Luttinger liquid model using the nonequilibrium Keldysh formalism and find qualitative and quantitative agreement between experiment and theory.     

Investigation of viscoelastic focusing of particles and cells in a zigzag microchannel

Microfluidic particle focusing has been a vital prerequisite step in sample preparation for downstream particle separation, counting, detection, or analysis, and has attracted broad applications in biomedical and chemical areas. Besides all the active and passive focusing methods in Newtonian fluids, particle focusing in viscoelastic fluids has been attracting increasing interest because of its advantages induced by intrinsic fluid property. However, to achieve a well-defined focusing position, there is a need to extend channel lengths when focusing micrometer-sized or sub-microsized particles, which would result in the size increase of the microfluidic devices. This work investigated the sheathless viscoelastic focusing of particles and cells in a zigzag microfluidic channel. Benefit from the zigzag structure of the channel, the channel length and the footprint of the device can be reduced without sacrificing the focusing performance. In this work, the viscoelastic focusing, including the focusing of 10 μm polystyrene particles, 5 μm polystyrene particles, 5 μm magnetic particles, white blood cells (WBCs), red blood cells (RBCs), and cancer cells, were all demonstrated. Moreover, magnetophoretic separation of magnetic and nonmagnetic particles after viscoelastic pre-focusing was shown. This focusing technique has the potential to be used in a range of biomedical applications.     

纤维素直接催化转化制乙二醇及其他化学品:从基础研究发现到潜在工业应用(英)

纤维素直接催化转化制乙二醇是一条极具吸引力的生物质转化途径,有助于减轻化石能源资源的消耗。综述了从该反应途径的发现到获得高效、高稳定性催化剂的快速发展过程。基于对钨基催化剂的大量研究结果,本文讨论了反应机制,明确了反应路径、催化剂状态、钨物种及加氢催化活性中心各自在串联反应中的作用。围绕该反应过程的工业化应用需要,讨论了有关原生木质纤维素生物质催化转化以及高效反应过程的发展策略。在此基础上,将纤维素催化转化制乙二醇过程与生物质发酵制丙酮-丁醇-乙醇的生物炼制路线进行整合,构建出一个理想的反应过程潜在应用范例。最后,对纤维素催化转化制乙二醇反应过程进行了总结和前景展望.     

Stepwise Assembly of Turn-on Fluorescence Sensors in Multicomponent Metal–Organic Frameworks for in Vitro Cyanide Detection

The controlled synthesis of multicomponent metal–organic frameworks (MOFs) allows for the precise placement of multiple cooperative functional groups within a framework, leading to emergent synergistic effects. Herein, we demonstrate that turn-on fluorescence sensors can be assembled by combining a fluorophore and a recognition moiety within a complex cavity of a multicomponent MOF. An anthracene-based fluorescent linker and a hemicyanine-containing CN⁻-responsive linker were sequentially installed into the lattice of PCN-700. The selective binding of CN⁻ to hemicyanine inhibited the energy transfer between the two moieties, resulting in a fluorescence turn-on effect. Taking advantage of the high tunability of the MOF platform, the ratio between anthracene and the hemicyanine moiety could be fine-tuned in order to maximize the sensitivity of the overall framework. The optimized MOF-sensor had a CN⁻-detection limit of 0.05 μm , which is much lower than traditional CN⁻ fluorescent sensors (about 0.2 μm ).     

Cross-Link-Functionalized Nanoparticles for Rapid Excretion in Nanotheranostic Applications

Most NIR-IIb fluorophores are nanoparticle-based probes with long retention (≈1 month or longer) in the body. Here, we applied a novel cross-linked coating to functionalize core/shell lead sulfide/cadmium sulfide quantum dots (PbS/CdS QDs) emitting at ≈1600 nm. The coating was comprised of an amphiphilic polymer followed by three crosslinked amphiphilic polymeric layers (P³ coating), imparting high biocompatibility and >90 % excretion of QDs within 2 weeks of intravenous administration. The P³-QDs were conjugated to an engineered anti-CD8 diabody (Cys-diabody) for in vivo molecular imaging of CD8+ cytotoxic T lymphocytes (CTLs) in response to anti-PD-L1 therapy. Two-plex molecular imaging in combination with down-conversion Er nanoparticles (ErNPs) was performed for real-time in vivo monitoring of PD-L1 positive tumor cells and CTLs with cellular resolution by non-invasive NIR-IIb light sheet microscopy. Imaging of angiogenesis in the tumor microenvironment and of lymph nodes deep in the body with a signal-to-background ratio of up to ≈170 was also achieved using P³-QDs.     

A Single-Atom Manipulation Approach for Synthesis of Atomically Mixed Nanoalloys as Efficient Catalysts

Synthesis of well-defined atomically mixed alloy nanoparticles on desired substrates is an ultimate goal for their practical application. Herein we report a general approach for preparing atomically mixed AuPt, AuPd, PtPd, AuPtPd NAs(nanoalloys) through single-atom level manipulation. By utilizing the ubiquitous tendency of aggregation of single atoms into nanoparticles at elevated temperatures, we have synthesized nanoalloys on a solid solvent with CeO₂ as a carrier and transition-metal single atoms as an intermediate state. The supported nanoalloys/CeO₂ with ultra-low noble metal content (containing 0.2 wt % Au and 0.2 wt % Pt) exhibit enhanced catalytic performance towards complete CO oxidation at room temperature and remarkable thermostability. This work provides a general strategy for facile and rapid synthesis of well-defined atomically mixed nanoalloys that can be applied for a range of emerging techniques.