Zn or O? An Atomic Level Comparison on Antibacterial Activities of Zinc Oxides

For the first time, the influence of different types of atoms (Zn and O) on the antibacterial activities of nanosized ZnO was quantitatively evaluated with the aid of a 3D‐printing‐manufactured evaluation system. Two different outermost atomic layers were manufactured separately by using an ALD (atomic layer deposition) method. Interestingly, we found that each outermost atomic layer exhibited certain differences against gram‐positive or gram‐negative bacterial species. Zinc atoms as outermost layer (ZnO?Zn) showed a more pronounced antibacterial effect towards gram‐negative E. coli (Escherichia coli), whereas oxygen atoms (ZnO?O) showed a stronger antibacterial activity against gram‐positive S. aureus (Staphylococcus aureus). A possible antibacterial mechanism has been comprehensively discussed from different perspectives, including Zn²⁺ concentrations, oxygen vacancies, photocatalytic activities and the DNA structural characteristics of different bacterial species.     

Copper‐Catalyzed Difunctionalization of Activated Alkynes by Radical Oxidation–Tandem Cyclization/Dearomatization to Synthesize 3‐Trifluoromethyl Spiro[4.5]trienones

A copper‐catalyzed difunctionalizing trifluoromethylation of activated alkynes with the cheap reagent sodium trifluoromethanesulfinate (NaSO₂CF₃ or Langlois’ reagent) has been developed incorporating a tandem cyclization/dearomatization process. This strategy affords a straightforward route to synthesis of 3‐(trifluoromethyl)‐spiro[4.5]trienones, and presents an example of difunctionalization of alkynes for simultaneous formation of two carbon–carbon single bonds and one carbon–oxygen double bond.     

航空导管弯曲试验的疲劳裂纹萌生寿命

飞行器液压导管受接头和卡箍等约束，在使用的振动环境中，会因弯曲应力而导致破裂，影响到飞行安全．本文对飞行器液压系统通用的不锈钢导管的裂纹萌生寿命进行了试验研究．首先在对8 mm、12 mm 无缺陷导管和含U 型缺口8 mm 导管的疲劳试验和有限元分析的基础上，得到了导管的最大拉应变-裂纹萌生寿命数据．然后采用基于强度极限和弹性模量估算法的Manson-Coffin 公式来预测导管裂纹萌生寿命．最后引入加载类型修正系数、表面质量修正系数、试样尺寸修正系数、应力集中敏感系数和有效应力集中系数，使修正后的公式对三种类型的导管均有较好的裂纹萌生寿命预测精度．     

Metal-Mediated Directional Capping of Rod-Packing Metal–Organic Frameworks

Two new rod-packing metal–organic frameworks (RPMOF) are constructed by regulating the in situ formation of the capping agent. In CPM-s7, carboxylate linkers extend 1D manganese-oxide chains in four additional directions, forming 3D RPMOF. The substitution of Mn²⁺ with a stronger Lewis acidic Co²⁺, leads to an acceleration of the hydrolysis-prone sulfonate linker, resulting in presence of sulfate ions to reduce two out of the four carboxylate-extending directions, and thus forming a new 2D rod-packing CPM-s8. Density functional theory calculations and magnetization measurements reveal ferrimagnetic ordering of CPM-s8, signifying the potential of exploring 2D RPMOF for effective low-dimensional magnetic materials.     

The Spin Modulation Stimulated Efficient Electrocatalytic Oxygen Evolution Reaction over LaCoO3 Perovskite

Perovskite is a promising non-noble catalyst and has been widely investigated for the electrochemical oxygen evolution reaction (OER). However, there is still serious lack of valid approaches to further enhance their catalytic performance. Herein, we propose a spin state modulation strategy to improve the OER electrocatalytic activity of typical perovskite material of LaCoO₃. Specifically, the electronic configuration transition was realized by a simple high temperature thermal reduction process. M-H hysteresis loop results reveal that the reduction treatment can produce more unpaired electrons in 3d orbit by promoting the electron transitions of Co from low spin state to high spin state, and thus lead to the increase of the spin polarization. Electrochemical measurements show that the catalytic performance of LaCoO₃ is strongly dependent on its electronic configuration. With the optimized reduction treatment, the overpotential for the OER process in 0.5 M KOH electrolyte solution at 10 mA cm⁻² current density was 396 mV, significantly lower than that of the original state. Furthermore, it can mediate efficient OER with an overpotential of 383 mV under an external magnetic field, which is attributed to the appropriate electron filling. Our results show that electron spin state regulation is a new way to boost the OER electrocatalytic activity.     

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.