碳青霉烯类β-内酰胺抗生素的化学合成及构效关系研究进展

碳青霉烯是一类新型β-内酰胺抗生素,它具有广谱、耐酶等特点,已用于临床抗重症感染的治疗。骨架和侧链的化学合成是碳青霉烯类药物研究和开发的重点和热点方向。近年来,采用有机金属催化合成骨架、四氢吡咯烷与疏水基团相连接合成侧链,取得了一定的进展。未来合成研究所面临的最大挑战是提高碳青霉烯类β-内酰胺抗生素的生物活性,其策略是寻找有效的骨架合成途径,同时增加药物的脂溶性和稳定性。

Synthesis and structures of cdq‑topological quaternary and(4,4,8)‑c topological quinary Zn‑MOFs with both oxalic acid and triazole ligands

Different solvothermal reactions of ZnC2O_(4)with oxalic acid(H_(2)ox)and 1,2,4-triazole(Htrz)successfully gave a new quaternary(NJTU-Bai83,NJTU-Bai=Nanjing Tech University Bai's group)and a new quinary(NJTU-Bai84)anionic metal-organic frameworks(MOFs),where NJTU-Bai83=(Me_(2)NH_(2))2[Zn_(3)(trz)_(2)(ox)_(3)]·2H_(2)O and NJTU-Bai84=(Me_(2)NH_(2))[Zn_(3)(trz)_(3)(ox)_(2)]·H_(2)O,respectively.With the[Zn_(2)(ox)4(trz)_(2)]secondary building unit(SBU)in NJTU-Bai83 replaced by the[Zn_(3)(ox)_(2)(trz)_(6)]and planar[Zn(ox)_(2)(trz)_(2)]ones in NJTU-Bai84,2D supramolecular building layers(SBLs)are changed from the A-layer and B-layer to another A-layer,while pillars are transformed from the tetrahedral[Zn(ox)_(2)(trz)_(2)]SBU to the irregular tetrahedral[Zn(ox)_(2)(trz)_(2)]and planar[Zn(ox)_(2)(trz)_(2)]SBUs.Thus,cdq-topological quaternary NJTU-Bai83 is tuned to(4,4,8)-c new topological quinary NJTU-Bai84.Two MOFs were well characterized by powder X-ray diffraction,thermogravimetric analysis,elemental analysis,etc.CCDC:2351819,NJTU-Bai83;2351820,NJTU-Bai84.

Amine-grafted on lanthanide metal-organic frameworks:Three solid base catalysts for Knoevenagel condensation reaction

A post-synthetic modification strategy has been used to prepare three solid base catalysts, including Er（btc）（ED）075（H2O）0.25 （2, btc = 1,3,5-benzenetricarboxylates, ED = 1,2-ethanediamine）, Er（btc）（PP）0.55（H20）0.45 （3, PP = piperazine）, and Er（btc）（DABCO）0.15（H2O）0.85 （4, DABCO = 1,4- diazabicyclo[2.2.2]octane）, by grafting three different diamines onto the coordinatively unsaturated Er（III） ions into the channels of the desolvated lanthanide metal-organic framework （Er（otc））. The resulting metal-organic frameworks were characterized by elemental analysis, thermogravimetric analysis, powder X-ray diffraction, and N2 adsorption. Based on its higher loading ratio of the diamine, as well as its greater stability and porosity, catalyst 2 exhibited higher catalytic activity and reusability than catalysts 3 and 4- for the Knoevenagel condensation reaction. The catalytic mechanism of 2 has also been investigated using size-selective catalysis tests.

基于视频的现实人物运动创作

提出一种根据用户指定的人体运动和观察视角生成真实感视频的方法.首先采集演员进行少数基本运动时的多视角视频数据库,并使用无标记运动捕捉的方法获得任意时刻人体对应的骨骼和3D模型.其次,用户对人体骨架指定运动并设定视角,以此定义目标视频.实验结果验证了文中方法能够利用有限的数据库合成演员在用户指定运动和视角下的真实感视频.

Al_(x)/HKUST-1 prepared by synthetic exchange as catalyst for reduction of NO by CO at low temperature

Al_(x)/HKUST-1(x=1/24,1/12,1/6,1/3),one of the bimetallic copper-based organic framework materials,was successfully prepared by the synthetic exchange method and characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),specific surface area(BET),thermogravimetric analysis(TG),infrared spectra(IR),X-ray photoelectron spectroscopy(XPS),and H_(2)-temperature programmed reduction(H_(2)-TPR).The findings indicated that Al_(x)/HKUST-1 maintained the octahedral morphology of its precursor(HKUST-1).The thermal stability and catalytic reduction ability of HKUST-1 skeleton were improved by doping aluminum(Al^(3+)).Al_(1/12)/HKUST-1 showed the best performance among all samples,with a nitric oxide(NO)conversion rate of 100%at 210℃(50℃lower than that of HKUST-1).The valence kind of Al,Cu,and O in Al_(1/12)/HKUST-1 did not change after the catalytic reaction,but the contents of Al,Cu,and O in different forms changed significantly.The catalytic process of the Al_(x)/HKUST-1 followed a Langmuir-Hinshelwood mechanism.

Tuning the growth of Cu-MOFs for efficient catalytic hydrolysis of carbonyl sulfide

Development of the high activity,promoter‐free catalysts for carbonyl sulfide(COS)hydrolysis is important for the efficient utilization of various feedstocks.In this study,the Cu‐based metal‐organic framework HKUST‐1is synthesized by a simple and mild anodic‐dissolution electrochemical method.The physical and chemical properties of the samples are characterized by several techniques,including scanning electron microscopy,X‐ray diffraction,Brunauer‐Emmett‐Teller analysis and X‐ray photoelectron spectroscopy.The results reveal that the synthesis voltage plays a crucial role in controlling the morphology of the resulting HKUST‐1.The obtained samples function as novel catalysts for the hydrolysis of COS.A high efficiency,approaching100%,can be achieved for the conversion of COS at150oC over the optimal HKUST‐1synthesized at25V.This is significantly higher than that of the sample prepared by the traditional hydrothermal method.Additionally,the effects of the water temperature and the flow velocity on the hydrolysis of COS are also investigated in detail.Finally,a possible reaction pathway of COS hydrolysis over HKUST‐1is also proposed.This work represents the first example of MOFs applied to the catalytic hydrolysis of COS.The results presented in this study can be anticipated to give a feasible impetus to design novel catalysts for removing the sulfur‐containing compounds.

Synthesis, structure, and magnetism of three manganese-organic framework with PtS topology

Three 3D manganese-organic frameworks, Mn2(BPTC)(DMF)2(H2O)·DMF·3H2O(1), Mn2(BPTC)(bipy)(DMF)·DMF·H2O(2), and Mn2(BPTC)(phen)(DMF)·EtOH(3), have been solvothermally synthesized using 3,3′,5,5′-biphenyltetracarboxylic acid(H4BPTC). All complexes are characterized by PXRD, EA, IR and TG. The results show that they all bear the PtS topology with(42.84)(42.84) for the vertex symbols of the planar and tetrahedral nodes, in which the BPTC ligand is considered as a square-planar 4-connected linker, and every binuclear SBU connected to the four BPTC ligands is simplified into tetrahedral 4-connected nodes. Because the three coordination sites of one metal center of SBU are occupied by the coordinated solvent molecules, complex 1 exhibits low stability. After substituting 2,2′-bipy or 1,10-phen for two coordinated solvent molecules, complexes 2 and 3 display evidently higher structure stability. The magnetism property of complex 2 is also discussed in detail.