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151.
The First One‐Pot Synthesis of Metal–Organic Frameworks Functionalised with Two Transition‐Metal Complexes
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Dr. Ana E. Platero‐Prats Dr. Antonio Bermejo Gómez Dr. Louise Samain Prof. Xiaodong Zou Prof. Belén Martín‐Matute 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(2):861-866
The synthesis of a metal–organic framework (UiO‐67) functionalised simultaneously with two different transition metal complexes (Ir and Pd or Rh) through a one‐pot procedure is reported for the first time. This has been achieved by an iterative modification of the synthesis parameters combined with characterisation of the resulting materials using different techniques, including X‐ray absorption spectroscopy (XAS). The method also allows the first synthesis of UiO‐67 with a very wide range of loadings (from 4 to 43 mol %) of an iridium complex ([IrCp*(bpydc)(Cl)Cl]2?; bpydc=2,2′‐bipyridine‐5,5′‐dicarboxylate, Cp*=pentamethylcyclopentadienyl) through a pre‐functionalisation methodology. 相似文献
152.
Muhammad Waqas Ali Siyuan Cheng Jianhao Si Muhammad Siddiq Xiaodong Ye 《Journal of polymer science. Part A, Polymer chemistry》2019,57(19):2030-2037
Hyperbranched poly(2‐ethyl‐2‐oxazoline) was synthesized by a combination of cationic ring‐opening polymerization and the oxidation of thiol to disulfide groups. A three‐arm star poly(2‐ethyl‐2‐oxazoline) (PEtOx) was first synthesized using 1,3,5‐tris(bromomethyl) benzene as an initiator. The star PEtOx was end‐capped with potassium ethyl xanthate. Similarly, a linear PEtOx was synthesized and end‐capped with potassium ethyl xanthate using benzyl bromide as an initiator. Hyperbranched PEtOx was then obtained by in situ cleaving and subsequent oxidation of the star PEtOx and linear PEtOx mixture with n‐butylamine as both a cleaving agent and a base in tetrahydrofuran. The linear PEtOx was used to prevent the formation of gel. The hyperbranched PEtOx can be cleaved with dithiothreitol to trithiol and monothiol polymer. The hyperbranched PEtOx shows no remaining thiols using Ellman's assay. The resulting hyperbranched PEtOx was hydrolyzed to a novel hyperbranched polyethyleneimine with degradable disulfide linkages. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 2030–2037 相似文献
153.
Dr. Tao Yang Prof. Yan Song Dr. Xiaodong Tian Prof. Huaihe Song Prof. Zhanjun Liu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(69):16514-16520
Pitch has been used to prepare electrodes by high-temperature heat treatments for supercapacitors, lithium-ion batteries, on account of its rich aromatic ring structure. Here, the toluene-soluble component of pitch is used to prepare a kind of laminated carbon. This was realized by a template-free synthesis at low temperature with the addition of pressure. The toluene-soluble component has a small molecular weight, which makes the thermal deformation ability stronger and then enhances the orientation of the carbon layer with the help of pressure. The prepared anode exhibits a splendid electrochemical performance compared with the traditional graphite anode. A high stable capacity of approximately 550 mAh g−1 at 50 mA g−1, which is much higher than graphite (372 mAh g−1), is obtained. Also, when the current density is up to 2 A g−1, the capacity is about 150 mAh g−1. Surprisingly, it also delivers a superior cycling performance. And when used as the anode/cathode electrode for lithium-ion capacitors, a high energy density can be obtained. The present work offers an opportunity to utilize the pitch source in lithium energy storage with promising cycle life, high energy/power density, and low cost. 相似文献
154.
Copper‐Catalyzed Reaction Cascade of Thiophenol Hydroxylation and S‐Arylation through Disulfide‐Directed C−H Activation
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Prof. Dr. Dawei Wang Xin Yu Wei Yao Wenkang Hu Chenyang Ge Prof. Dr. Xiaodong Shi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(16):5543-5546
Copper‐catalyzed thiophenol C?H activation is described. Through an initial attempt to conduct C‐arylation with arylboronic acid, a rather surprising sequential C?H activation and S‐arylation was discovered. Mechanistic investigation revealed the disulfide intermediate as the key component in directing C?H oxidation. The overall reaction proceeded under mild conditions with molecular oxygen as the oxidant. Discovery of disulfide as the directing group provides a potential new direction for catalytic C?H functionalization under mild conditions. 相似文献
155.
A Rhodium Catalyst Superior to Iridium Congeners for Enantioselective Radical Amination Activated by Visible Light
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Xiaodong Shen Dr. Klaus Harms Michael Marsch Prof. Dr. Eric Meggers 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(27):9102-9105
A bis‐cyclometalated rhodium(III) complex catalyzes a visible‐light‐activated enantioselective α‐amination of 2‐acyl imidazoles with up to 99 % yield and 98 % ee. The rhodium catalyst is ascribed a dual function as a chiral Lewis acid and, simultaneously, as a light‐activated smart initiator of a radical‐chain process through intermediate aminyl radicals. Notably, related iridium‐based photoredox catalysts reported before were unsuccessful in this enantioselective radical C?N bond formation. The surprising preference for rhodium over iridium is attributed to much faster ligand‐exchange kinetics of the rhodium complexes involved in the catalytic cycle, which is crucial to keep pace with the highly reactive and thus short‐lived nitrogen‐centered radical intermediate. 相似文献
156.
Generation of Oxazolidine‐2,4‐diones Bearing Sulfur‐Substituted Quaternary Carbon Atoms by Oxothiolation/Cyclization of Ynamides
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Hai Huang Junzhen Fan Dr. Guangke He Zhimin Yang Xiaodong Jin Qi Liu Prof. Dr. Hongjun Zhu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(7):2532-2538
A novel method for metal‐free oxothiolation of ynamides to construct oxazolidine‐2,4‐diones bearing sulfur‐substituted quaternary carbon atoms has been developed. It represents a rare C?O bond cleavage of ynamides, as well as a facile and tandem approach for the formation of C?O, C?S, and C?Cl bonds. This redox‐neutral protocol can be applied to the synthesis of multisubstituted oxazolidine‐2,4‐diones with good chemoselectivity and good yields of isolated products under mild conditions. 相似文献
157.
通过连续3年的模拟增温实验,探讨了东北松嫩草甸草原单优种羊草的有性生殖策略对大气温度增加的响应.结果表明:增温使羊草物候期从抽穗期开始比对照提前,尤其是从第一花粉囊外露之后到果实成熟期,物候期均比对照明显提前5~7d.增温降低了单位面积的生殖枝数量,但使生殖枝单株重量、每穗小花数、结实粒数、籽粒重量都显著增加.种群水平上,用于有性生殖的总能量减少,但单株水平上,用于籽粒发育的能量增加.羊草这一多年生根茎型禾草在大气温度升高的条件下会采取减少生殖枝数量而增加生殖枝结实能力的繁殖策略,说明类似于羊草的多年生根茎型禾草在温度变化的条件下生殖策略会发生较大改变,多年的持续增温可能导致种子产量的持续降低. 相似文献
158.
记录采自河北大学校园的中国刺足蛛科1新纪录属:唇蛛属Labialithus Kamura, 2021,其模式种为唇形唇蛛Labialithus labialis(Paik,1991).此前该属只记载分布于日本、韩国和俄罗斯(远东地区). 相似文献
159.
160.
Yuping Liu Hongxing Wang Fengru Liu Jialing Kang Dr. Feng Qiu Prof. Changchun Ke Dr. Yu Huang Prof. Sheng Han Prof. Fan Zhang Prof. Xiaodong Zhuang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(6):2155-2164
Transition metal-based nanoparticle-embedded carbon materials have received increasing attention for constructing next-generation electrochemical catalysts for energy storage and conversion. However, designing hybrid carbon materials with controllable hierarchical micro/mesoporous structures, excellent dispersion of metal nanoparticles, and multiple heteroatom-doping remains challenging. Here, a novel pyridinium-containing ionic hypercrosslinked micellar frameworks (IHMFs) prepared from the core–shell unimicelle of s-poly(tert-butyl acrylate)-b-poly(4-bromomethyl) styrene (s-PtBA-b-PBMS) and linear poly(4-vinylpyridine) were used as self-sacrificial templates for confined growth of molybdenum disulfide (MoS2) inside cationic IHMFs through electrostatic interaction. After pyrolysis, MoS2-anchored nitrogen-doped porous carbons possessing tunable hierarchical micro/mesoporous structures and favorable distributions of MoS2 nanoparticles exhibited excellent electrocatalytic activity for hydrogen evolution reaction as well as small Tafel slope of 66.7 mV dec−1, low onset potential, and excellent cycling stability under acidic condition. Crucially, hierarchical micro/mesoporous structure and high surface area could boost their catalytic hydrogen evolution performance. This approach provides a novel route for preparation of micro/mesoporous hybrid carbon materials with confined transition metal nanoparticles for electrochemical energy conversion. 相似文献