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991.
Controllably synthesizing well-dispersed covalent organic frameworks (COFs) with uniform both morphology and size is still a challenge. Herein, we report the template-directed synthesis of COFTTA-DHTA-based core-shell hybrids under solvothermal conditions by using amino-functionalized SiO2 microspheres as templates coupled with stepwise addition of initial monomer molecules. The modified amino groups on the surfaces of SiO2 templates play an important role in the formation of well-defined NH2-f-SiO2@COFTTA-DHTA core-shell hybrids. COFTTA-DHTA hollow spheres can be obtained by etching SiO2 cores of NH2-f-SiO2@COFTTA-DHTA. Both the NH2-f-SiO2@COFTTA-DHTA and COFTTA-DHTA hollow spheres possess the well-defined morphology, high crystallinity and porosity, excellent dispersion property and high chemical stability. The template synthesis method demonstrated in this work provides a general method for the shape-controlled synthesis of COF-based materials, which is important for the further applications in the fields such as energy storage, drug delivery and catalysis. 相似文献
992.
Yunfeng Xu Chong Zhang Pan Mu Na Mao Xue Wang Qian He Feng Wang Jia-Xing Jiang 《中国科学:化学(英文版)》2017,60(8):1075-1083
Two novel tetra-armed conjugated microporous polymers with different geometries have been designed and synthesized via Suzuki-Miyaura cross coupling polycondensation. Both polymers are stable in various organic solvents tested and are thermally stable. The pyrene-containing polymer of PrPy with the rigid pyrene unit shows a higher Brunauer-Emmet-Teller specific surface area of 1219 m2 g?1 than the tetraphenylethylene-containing polymer of PrTPE (770 m2 g?1), which leads to a high CO2 uptake ability of 3.89 mmol g?1 at 1.13 bar/273 K and a H2 uptake ability of 1.69 wt% at 1.13 bar/77 K. The photocatalytic hydrogen production experiments revealed that PrPy also shows a better photocatalytic performance than PrTPE due to the higher conjugation degree and planar structure, the broader UV-visible (UV-Vis) absorption, the lower photoluminescence lifetime, and the higher specific surface area. 相似文献
993.
Xinhui?ZhouEmail author Yali?Zhu Liang?Li Tao?Yang Jin?Wang Wei?Huang 《中国科学:化学(英文版)》2017,60(8):1130-1135
Three isostructural three-dimensional(3D) lanthanide-based metal-organic frameworks [Ln_2L(H_2L)(NMP)_2].H_2O(Ln=Sm(1), Eu(2), Gd(3); H_4L=1,1′:4′,1″-terphenyl-2′,4,4″,5′-tetracarboxylic acid; NMP=N-methyl-2-pyrrolidone) have been synthesized and structurally characterized. In 1–3, two Ln3+ ions are doubly-bridged by two oxygen atoms of two carboxylate groups to form the dinuclear Ln_2(OCOO–)_2 unit. Each Ln_2(OCOO–)_2 unit links with four H_2L~(2-) ligands and four L4. ligands to lead to the 3D framework,which can be rationalized as a new trinodal 4,4,8-connected(44.62)(45.6)(412.616) topological network by considering the dinuclear Ln_2(OCOO–)_2 units as 8-connected nodes and L~4./H_2L~(2-) ligands as planar 4-connected nodes, respectively. 1 and 3 exhibit blue emission originated from the ligand with the emission maximum at 384 nm, while 2 shows intense characteristic red emission of Eu~(3+) ions and weak ligand-centered emission. Moreover, 2 has fluorescent quenching response towards the aromatic nitro compounds, especially for the 3,4-dinitrotoluene(3,4-DNT) with the linear Stern-Volmer relationship in the concentration range of 0–1 mM and the quenching constant(Ksv) of 2.084×10~3 M~(-1). 相似文献
994.
Shujun Yu Xiangxue Wang Shitong Yang Guodong Sheng Ahmed Alsaedi Tasawar Hayat Xiangke Wang 《中国科学:化学(英文版)》2017,60(2):170-187
The X-ray absorption fine structure (XAFS) technology has exhibited a very unique application in the study of sorption mechanism, chemical species and microstructures of radionuclides at the natural solid-water interfaces. In this review, the interaction mechanism of radionuclides with clay minerals and nanomaterials under different environmental conditions are summarized from the XAFS spectroscopy analysis. The coordination number and the bond distances of radionuclides, the oxidation-reduction reactions, the influence of humic substances and microorganisms on the species and structures of radionuclides at molecule level are reviewed and compared. This review is helpful to understand the interactions of radionuclides with oxides, natural clay minerals and nanomaterials, which is also crucial to evaluate the physicochemical behaviors of radionuclides in the natural environment. 相似文献
995.
Metalloproteins have inspired chemists for many years to synthesize artificial catalysts that mimic native enzymes.As a complementary approach to studying native enzymes or making synthetic models,biosynthetic approach using small and stable proteins to model native enzymes has offered advantages of incorporating non-covalent secondary sphere interactions under physiological conditions.However,most biosynthetic models are restricted to natural amino acids.To overcome this limitation,incorporating unnatural amino acids into the biosynthetic models has shown promises.In this review,we summarize first synthetic,semisynthetic and biological methods of incorporates unnatural amino acids(UAAs)into proteins,followed by progress made in incorporating UAAs into both native metalloproteins and their biosynthetic models to fine-tune functional properties beyond native enzymes or their variants containing natural amino acids,such as reduction potentials of azurin,O_2 reduction rates and percentages of product formation of HCO models in Mb,the rate of radical transport in ribonucleotide reductase(RNR)and the proton and electron transfer pathways in photosystemⅡ(PSⅡ).We also discuss how this endeavour has allowed systematic investigations of precise roles of conserved residues in metalloproteins,such as Metl21 in azurin,Tyr244 that is cross-linked to one of the three His ligands to CuB in HCO,Tyr122,356,730 and 731 in RNR and TyrZ in PSⅡ.These examples have demonstrated that incorporating UAAs has provided a new dimension in our efforts to mimic native enzymes and in providing deeper insights into structural features responsible high enzymatic activity and reaction mechanisms,making it possible to design highly efficient artificial catalysts with similar or even higher activity than native enzymes. 相似文献
996.
Polymer electron acceptors are the key materials in all-polymer solar cells(all-PSCs).In this review,we focused on introducing the principle of boron-nitrogen coordination bond(B←N),and summarizing our recent research on polymer electron acceptors containing B←N unit for efficient all-PSC devices.Two approaches have been reported to design polymer electron acceptors using B←N unit.One is to replace a C-C unit by a B←N unit in conjugated polymers to transform a polymer electron donor to a polymer electron acceptor.The other approach is to construct novel electron-deficient building block based on B←N unit for polymer electron acceptors.The polymer electron acceptors containing B←N unit showed tunable lowest unoccupied molecular orbital(LUMO) energy levels and exhibited excellent all-PSC device performance with power conversion efficiency of exceeding6%.These results indicate that organic boron chemistry is a new toolbox to develop functional polymer materials for optoelectronic device applications. 相似文献
997.
Dunfeng Gao Fan Cai Guoxiong Wang Xinhe Bao 《Current Opinion in Green and Sustainable Chemistry》2017
Electrochemical reduction of CO2 provides a sustainable solution to address the intermittent renewable electricity storage while recycling CO2 to produce fuels and chemicals. Highly efficient catalytic materials and reaction systems are required to drive this process economically. This Review highlights the new trends in advancing the electrochemical reduction of CO2 by developing and designing nanostructured heterogeneous catalysts. The activity, selectivity and reaction mechanism are significantly affected by the nano effects in nanostructured heterogeneous catalysts. In the future, energy efficiency and current density in electrochemical reduction of CO2 need to be further improved to meet the requirements for practical applications. 相似文献
998.
999.
1000.
Jingwei Wang Qianqian Luo Chunhua Luo Hechun Lin Ruijuan Qi Ni Zhong Hui Peng 《Journal of Solid State Electrochemistry》2017,21(7):2071-2077
In this study, MoS2 nanosheets were first prepared by exfoliating its bulk material in HCl/LiNO3 solution with a yield of 45%, and then a facile strategy was developed to synthesize polyaniline/MoS2 (PANI/MoS2) nanocomposite via in situ polymerization. Structural and morphological characterizations of MoS2 nanosheets and the nanocomposite were investigated by scanning electron microscope (SEM), transmission electron microscope (TEM), and X-ray powder diffraction. The results of SEM illustrated that orderly sawtooth polyaniline (PANI) nanoarrays were formed on the surface of MoS2 nanosheets. The nanocomposite displayed good electrochemical performance as a supercapacitor electrode material. The specific capacitance reached 560 F/g at a current density of 1.0 A g?1 in 1.0 M H2SO4 solution. Such good performance is because that the MoS2 nanosheets provided a highly electrolytic accessible surface area for redox-active PANI and a direct path for electrons. 相似文献