高速气体与椭圆柱云相互作用的数值研究

高速颗粒流在天文、自然灾害、工业安全、医疗工业和国防等领域有着重要应用。采用基于分层流模型的直接数值模拟方法,对平面激波与椭圆柱云的相互作用进行数值研究,重点关注椭圆柱横截面的不同长短轴之比和椭圆柱横截面长轴与来流方向所成角度对流场的影响,从气体来流方向上的速度、x轴和y轴方向上的均方根速度、动能、内能和湍动能的分布上进行分析,对能量在计算域的上游区域、椭圆柱云区域和下游区域进行定量分析。同时针对椭圆柱改进了一维体积平均模型,利用该模型拟合了由直接数值模拟得到的反射激波和透射激波位置,获得了最适配的一维体积平均模型中的人工有效阻力系数,并探讨此系数的分布规律。     

Structure-tuned membrane active Ir-complexed oligoarginine overcomes cancer cell drug resistance and triggers immune responses in mice

The development of chemotherapy, an important cancer treatment modality, is hindered by the frequently found drug-resistance phenomenon. Meanwhile, researchers have been enthused lately by the synergistic use of chemotherapy with emerging immunotherapeutic treatments. In an effort to address both of the two unmet needs, reported herein is a study on a series of membrane active iridium(iii) complexed oligoarginine peptides with a new cell death mechanism capable of overcoming drug resistance as well as stimulating immunological responses. A systematic structure–activity relationship study elucidated the interdependent effects of three structural factors, i.e., hydrophobicity, topology and cationicity, on the regulation of the cytotoxicity of the Ir(iii)-oligoarginine peptides. With the most prominent toxicities, Ir-complexed octaarginines (R8) were found to display a progressive oncotic cell death featuring cell membrane-penetration and eruptive cytoplasmic content release. Consequently, this membrane-centric death mechanism showed promising potential in overcoming multiple chemical drug-resistance of cancer cells. More interestingly, the eruptive mode of cell death proved to be immunogenic by stimulating the dendritic cell maturation and inflammatory factor accumulation in mice tumours. Taking these mechanisms together, this work demonstrates that membrane active compounds may become the next generation chemotherapeutics because of their combined advantages.

Structure optimized Ir-complexed cyclic octa-arginine shows a potential of “one-drug two-effects” for cancer treatment.     

介孔碳材料抑制锂电池负极枝晶生长

为了解决锂电池负极表面锂枝晶生长带来的性能衰退和安全问题。 以沸石咪唑酯骨架-8(ZIF-8)为前驱体制得介孔碳材料(MCM),用于金属锂负极表面改性。 X射线粉末衍射(XRD)和拉曼光谱表明,退火制得的MCM具有一定的石墨化程度,N₂气吸脱附测试(BET)证明MCM具有典型的介孔特征。 对比不同温度退火样品的XRD、拉曼光谱和BET测试结果,确定900 ℃为最佳退火温度。 优化的MCM作为表面改性剂对金属锂负极进行改性研究。 电池充放电循环后,负极样品的XRD和扫描电子显微镜(SEM)测试表明,MCM能够通过均衡锂负极表面的电荷分布抑制金属锂的取向沉积和锂枝晶的生长。 本研究为制备抑制锂电池负极枝晶生长表面改性剂提供了一种简便而有效的合成方法,有利于锂电池循环寿命的延长和安全性能的提高。     

Reversible Switching CuII/CuI Single Sites Catalyze High-rate and Selective CO2 Photoreduction

Herein, we first design a model of reversible redox-switching metal–organic framework single-unit-cell sheets, where the abundant metal single sites benefit for highly selective CO₂ reduction, while the reversible redox-switching metal sites can effectively activate CO₂ molecules. Taking the synthetic Cu-MOF single-unit-cell sheets as an example, synchrotron-radiation quasi in situ X-ray photoelectron spectra unravel the reversible switching Cu^II/Cu^I single sites initially accept photoexcited electrons and then donate them to CO₂ molecules, which favors the rate-liming activation into CO₂^δ−, verified by in situ FTIR spectra and Gibbs free energy calculations. As an outcome, Cu-MOF single-unit-cell sheets achieve near 100 % selectivity for CO₂ photoreduction to CO with a high rate of 860 μmol g⁻¹ h⁻¹ without any sacrifice reagent or photosensitizer, where both the activity and selectivity outperform previously reported photocatalysts evaluated under similar conditions.     

Enhancing Built-in Electric Fields for Efficient Photocatalytic Hydrogen Evolution by Encapsulating C60 Fullerene into Zirconium-Based Metal-Organic Frameworks

High-efficiency photocatalysts based on metal-organic frameworks (MOFs) are often limited by poor charge separation and slow charge-transfer kinetics. Herein, a novel MOF photocatalyst is successfully constructed by encapsulating C₆₀ into a nano-sized zirconium-based MOF, NU-901. By virtue of host-guest interactions and uneven charge distribution, a substantial electrostatic potential difference is set-up in C₆₀@NU-901. The direct consequence is a robust built-in electric field, which tends to be 10.7 times higher in C₆₀@NU-901 than that found in NU-901. In the catalyst, photogenerated charge carriers are efficiently separated and transported to the surface. For example, photocatalytic hydrogen evolution reaches 22.3 mmol g⁻¹ h⁻¹ for C₆₀@NU-901, which is among the highest values for MOFs. Our concept of enhancing charge separation by harnessing host-guest interactions constitutes a promising strategy to design photocatalysts for efficient solar-to-chemical energy conversion.