Porphyrin distortion during affinity maturation of a ferrochelatase antibody, monitored by Resonance Raman spectroscopy

Resonance Raman (RR) spectra are reported for mesoporphyrin IX bound to the Fab fragment of the ferrochelatase antibody 7G12. Binding induces activation of a Raman band at 680 cm(-1), which is assigned to an out-of-plane porphyrin vibration, gamma15. This is exactly the predicted effect of distorting mesoporphyrin to the geometry of N-methylmesoporphyrin IX, the 7G12 hapten, based on DFT/CIS modeling of the RR spectrum. The modeling also shows that the pyrrole ring that is tilted out of the porphyrin plane bears a nitrogen lone pair, which is therefore available for coordination by an incoming metal ion. The 680 cm(-1) band intensity is approximately 3 times higher for the affinity-matured antibody than for the germline precursor antibody, while intermediate values are found for variants in which germline residues are mutated to mature residues or vice versa. Thus, RR spectroscopy reveals an evolution from weak substrate distortion in the germline antibody to strong substrate distortion in the affinity-matured antibody, and supports the view that catalysis involves a substrate strain mechanism.     

静止化学反应界面：理论和验证

在静止中和反应界面的基础上，提出了静止化学反应界面的概念，导出了一些静止化学反应界面方程。这些方程显示：为了建立稳定的静止化学反应界面，正、负反应离子（比如氢离子和氢氧根离子）的迁移数必须相等。分析表明，方程的理论预测与下列事实定量吻合：（１）已建立的静止中和反应界面的实验，（２）基于Ｋｏｈｌｒａｕｓｃｈ′ｓ调整函数的计算机模拟。     

Two new C18-norditerpenoid alkaloids from Aconitum delavayi

Further phytochemical investigation of the unique C18-norditerpenoid alkaloids from the roots of Aconitum delavayi Franch ledto the isolation of two new norditerpenoid alkaloids,delavaconitine F 1 and delavaconitine G 2.Their structures were determinedfrom spectroscopic evidence.     

Zeolite NaY-mediated oxidation of dyes with H2O2: unique heterogeneous non-transition metal center cleavage of H2O2 under visible light irradiation

This study investigated the visible-light catalysis mediated by zeolite NaY on the oxidation of dyes with H₂O₂. The results demonstrated that zeolite NaY acts as a sink for the electron from the photo-excited dye in the heterogeneous catalysis. Furthermore, the electron can effectively activate H₂O₂ to produce ^·OH radical that is a powerful oxidant for the oxidation of dye at room temperature. The effects of the framework topology, Si/Al ratio, and exchangeable cation of the zeolite on the oxidation of various dyes were also shown.     

Theoretical studies on the band structures of superconducting solid compounds: Nb3X (X=Si, Ge, Sn, Pb)

The band structures of several analogous superconducting A-15 type solid compounds, Nb3X (X=Si, Ge, Sn, Pb), have been calculated by use of the tight-binding method within the Extended Huckel approximation (EHT). By analysis of their energy bands, densities of states and crystal orbital overlap populations, the dependence of the superconducting transition temperatures (Tc) on the electronic structures and bondings is qualitatively elucidated.     

FABRICATION OF SELF-ASSEMBLY DNA-C_(60) MULTILAYER FILMS

Electrostatic layer-by-layer self-assembly multilayer films were successfully fabricated from C_(60)-ethylenediamineadduct (C_(60)-EDA) and DNA. Under visible light irradiation, DNA is ready to be cleaved and the films are destroyed.     

高比表面积介孔网状氧化镁的制备、表征及对废水中Pb(Ⅱ)的吸附性能和机理

以天然水菱镁矿为原料，通过"煅烧-水化-煅烧"的简单方法制备了高比表面积介孔网状MgO，且实验过程中无须加入任何试剂。系统性研究了氧化镁用量、吸附时间、吸附温度及pH对氧化镁吸附模拟废水中铅离子吸附性能的影响，揭示了吸附机理，并考察了氧化镁对多种离子的吸附效果。结果表明：该氧化镁吸附剂具有188 m²·g^-1的高比表面积和0.85 cm³·g^-1的高孔体积，平均孔径为12.33 nm，其吸附动力学和等温线数据与伪二级模型和Langmuir模型高度吻合，表明重金属离子在氧化镁上为单层化学吸附。MgO介孔网状结构表现出对Pb（Ⅱ）的高吸附性能，最大吸附量为7 431.5 mg·g^-1，该数值远高于其他报道的基于MgO吸附剂的数值，铅去除率高达99.8%以上。介孔网状MgO的吸附机理主要是羟基官能团以及Mg（Ⅱ）与MgO表面重金属离子之间的离子交换所致。另外，该氧化镁可同时吸附多种离子，对Cd、Cr、Ni、As、Co、P、Se、Be、Bi、Cu、Fe、Mn、V、Zn、Al离子均具有优异的吸附性能。     

Flexible all-biomass gas sensor based on doped carbon quantum dots/nonwoven cotton with discriminative function

Carbon quantum dots (CQDs) co-doped with N, P and S derived from expired milk was prepared by a simple hydrothermal method. By dipping pure cotton face towel (PCFT) into CQDs ink, a flexible all-biomass CQDs/PCFT sensor was prepared for the first time. Due to the heteroatom doping, extremely small particle size of CQDs and excellent permeability of CQDs/PCFT film, the flexible CQDs/PCFT sensor showed the high sensitivity and bending stability. In the range of 0–60° bending states, the responses of CQDs/PCFT sensor to four target analytes changed by less 5.0%. After 3000 bending of 60°, the maximum change of the response to the target analytes was only 6.4%. Interestingly, due to the abundant functional groups and defects of CQDs, the flexible CQDs/PCFT sensor displayed sensing curves of different shapes for different target analytes. In this way, by establishing a database of sensing curves of target analytes, multiple analytes can be detected discriminatively by relying only on single sensor with the help of image recognition. This work provided a reference for the development of cotton fiber based all biomass flexible gas sensor.

Graphical abstract

     

Synthesis and Catalytic Application of Homo-bimetallic Metallocene Complexes as Ethylene Polymerization Catalysts

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Clean Aerobic Liquid Oxidation of Aldehydes with Solid Catalyst

Clean liquid oxidation of aldehydes can be accomplished using solid catalyst in the presence of molecular oxygen at room temperature, which is a valuable alternative to traditional counterparts.