Electro-assisted Molecular Assembly Giving Atomic-Scale Catalytic Active-Site Detection

The artificially accurate design of nonmetal electrocatalysts’ active site has been a huge challenge because no pure active species with the specific structure could be strictly controlled by traditional synthetic methods. Species with a multiconfiguration in the catalyst hinder identification of the active site and the subsequent comprehension of the reaction mechanism. We have developed a novel electro-assisted molecular assembly strategy to obtain a pure pentagon ring on perfect graphene avoiding other reconstructed structures. More importantly, the active atom was confirmed by the subtle passivation process as the topmost carbon atom. Recognition of the carbon-defect electrocatalysis reaction mechanism was first downsized to the single-atom scale from the experimental perspective. It is expected that this innovative electro-assisted molecular assembly strategy could be extensively applied in the active structure-controlled synthesis of nonmetal electrocatalysts and verification of the exact active atom.     

Synthesis and properties of side-chain liquid crystalline polymers grafted with chiral dimers containing cholesteryl groups

ABSTRACT

Two series of novel side-chain liquid crystal (LC) polysiloxanes grafted with chiral liquid crystalline dimers containing cholesteryl mesogens were synthesised. The chemical structure and LC properties of comonomers and polymers were characterised by FTIR, ¹H-NMR, DSC, TGA, POM and XRD. M₁ and M₂ were chiral nematic (N*) dimers, and M₃ was an achiral LC monomer displaying nematic mesophase in a narrow mesomorphic temperature range, while the copolymers exhibited N* mesophase whose mesomorphic temperature ranges were much wider than those of the comonomers. Moreover, the glass transition temperatures and isotropization temperatures of the polymers all decreased with decreasing the dimer components. Reflection spectra showed that P_a series tend to attain wide-band selective reflection at long wavelengths, while P_b series were more potential at short wavelengths with narrow bandwidths. Decreasing the dimer components led the wavelength of the selective reflection to blue shift, which was an abnormal phenomenon in chiral mixture system.     

A unified approach to error bounds for structured convex optimization problems

Error bounds, which refer to inequalities that bound the distance of vectors in a test set to a given set by a residual function, have proven to be extremely useful in analyzing the convergence rates of a host of iterative methods for solving optimization problems. In this paper, we present a new framework for establishing error bounds for a class of structured convex optimization problems, in which the objective function is the sum of a smooth convex function and a general closed proper convex function. Such a class encapsulates not only fairly general constrained minimization problems but also various regularized loss minimization formulations in machine learning, signal processing, and statistics. Using our framework, we show that a number of existing error bound results can be recovered in a unified and transparent manner. To further demonstrate the power of our framework, we apply it to a class of nuclear-norm regularized loss minimization problems and establish a new error bound for this class under a strict complementarity-type regularity condition. We then complement this result by constructing an example to show that the said error bound could fail to hold without the regularity condition. We believe that our approach will find further applications in the study of error bounds for structured convex optimization problems.     

Engineering Plasmonic Environments for 2D Materials and 2D-Based Photodetectors

Two-dimensional layered materials are considered ideal platforms to study novel small-scale optoelectronic devices due to their unique electronic structures and fantastic physical properties. However, it is urgent to further improve the light–matter interaction in these materials because their light absorption efficiency is limited by the atomically thin thickness. One of the promising approaches is to engineer the plasmonic environment around 2D materials for modulating light–matter interaction in 2D materials. This method greatly benefits from the advances in the development of nanofabrication and out-plane van der Waals interaction of 2D materials. In this paper, we review a series of recent works on 2D materials integrated with plasmonic environments, including the plasmonic-enhanced photoluminescence quantum yield, strong coupling between plasmons and excitons, nonlinear optics in plasmonic nanocavities, manipulation of chiral optical signals in hybrid nanostructures, and the improvement of the performance of optoelectronic devices based on composite systems.     

超导磁体螺栓结合面低温振动特性研究

振动特性对于超导磁体的各类工程应用具有重要意义,螺栓法兰盘连接是超导磁体系统的一种常见的支撑结构类型,然而螺栓结合面在低温条件下振动特性的相关研究目前尚少见报道.本研究中设计加工了简化的连接结构,在室温和液氮温度对其螺栓结合面进行振动特性的测试分析.接下来,采用集中质量法进行建模,并利用振型、频率与质量矩阵、刚度矩阵的关系求解了不同螺栓预紧力情况下的刚度矩阵,得到了系统总刚度和结合面刚度.使用上述方法对振动测量数据计算发现,该结构的系统总刚度与结合面刚度都随着预紧力增大而增大,同时液氮低温条件可使系统总刚度和结合面刚度进一步增大.     

Presodiation Strategies for the Promotion of Sodium-Based Energy Storage Systems

Nowadays sodium-based energy storage systems (Na-based ESSs) have been widely researched as it possesses the possibility to replace traditional energy storage media to become next generation energy storage system. However, due to the irreversible loss of sodium ions in the first cycle, development of Na-based ESSs is limited. Presodiation, as a strategy of adding excess sodium ions to the system in advance, accomplishes the enhancement of electrochemical performance. In this minireview, different presodiation strategies applied in sodium-based energy storage systems will be summarized in detail, their functions and corresponding mechanisms will be discussed as well. Furthermore, the current novel application of presodiation method in other aspects of Na-based ESSs will be mentioned additionally. At last, in the view of present research status of presodiation, issues that can be mitigated are put forward and guidelines are given on how to deliberate in-depth presodiation technology in the future, dedicating to promote the further development of Na-based ESSs.     

Reconstructing Hydrogen Bond Network Enables High Voltage Aqueous Zinc-Ion Supercapacitors

High-voltage aqueous rechargeable energy storage devices with safety and high specific energy are hopeful candidates for the future energy storage system. However, the electrochemical stability window of aqueous electrolytes is a great challenge. Herein, inspired by density functional theory (DFT), polyethylene glycol (PEG) can interact strongly with water molecules, effectively reconstructing the hydrogen bond network. In addition, N, N-dimethylformamide (DMF) can coordinate with Zn²⁺, assisting in the rapid desolvation of Zn²⁺ and stable plating/stripping process. Remarkably, by introducing PEG400 and DMF as co-solvents into the electrolyte, a wide electrochemical window of 4.27 V can be achieved. The shift in spectra indicate the transformation in the number and strength of hydrogen bonds, verifying the reconstruction of hydrogen bond network, which can largely inhibit the activity of water molecule, according well with the molecular dynamics simulations (MD) and online electrochemical mass spectroscopy (OEMS). Based on this electrolyte, symmetric Zn cells survived up to 5000 h at 1 mA cm⁻², and high voltage aqueous zinc ion supercapacitors assembled with Zn anode and activated carbon cathode achieved 800 cycles at 0.1 A g⁻¹. This work provides a feasible approach for constructing high-voltage alkali metal ion supercapacitors through reconstruction strategy of hydrogen bond network.