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991.
[Cu2(UO2)4(suc)4(pac)4] (1), [(Cu(H2O)2)(4,4′-bipy)2][(UO2)2(H2O)2(Hca)2]·3H2O (2), and [(Cu(H2O)2)(UO2)(bta)]·4H2O (3) were synthesized by the reaction of succinic acid and 3-pyridinecarboxylic acid, citric acid and 4,4′-bipyridine, or 1,2,4,5-benzenetetracarboxylic acid ligands with Cu(NO3)2·3H2O and UO2(CH3COO)2·2H2O. The complexes were characterized by IR and UV–vis spectroscopy, powder X-ray diffraction, single-crystal X-ray diffraction, and photoluminescence spectroscopy. Photocatalytic activities of the complexes were also investigated.  相似文献   
992.
Two novel phosphonate compounds (H2L)·Hphen (1) and [Ca(HL)(H2O)]n·3.5nH2O (2) (L = N(CH2PO3H)33?) were synthesized under hydrothermal conditions. Compound 1 features a chain structure in the ac plane, where HL2? anions are interconnected through sharing hydrogen ions to form a 1D zigzag type. Compound 2 features a layered structure in the ab plane, which has inorganic calcium cores with the organic part of the phosphonate anions being encircling the cores through coordination actions. The free water molecules can form hydrogen bonds with the coordinated water molecules and phosphonate oxygen atoms, which are able to link the adjacent layers to generate a 3D network structure. In addition, the thermal stability and photoluminescence properties were also studied.  相似文献   
993.
The efficiency of impregnation methods for making Cu-based solid oxide fuel cells (SOFCs) is qualitatively characterized for the first time through a conformal coating model. It is found that the low-efficiency results from the uneven distribution of Cu instead of the small loading. Most of the Cu deposits form isolated islands, e.g., in a 20.4 vol.% Cu-loaded anode, 81% Cu is isolated from each other. In order to address the limited impregnation efficiency, two different procedures are adopted to fabricate the practical Cu/CeO2 anodes, namely, simultaneous and sequential impregnation procedures. It is found that CeO2 works as a solid dispersant, improving the Cu distribution drastically. Compared to the Cu-only anode, more than a threefold improvement of impregnation efficiency is achieved by both methods. The anode made by the sequential impregnation yields the best performance in CH4 at 700 °C, 170 mW cm?2, which represents an 18% enhancement over that of the simultaneous impregnation, or 340% over the Cu-only anode. These findings demonstrate that it is of importance to optimize the Cu impregnation to yield a highly active anode, and the sequential impregnation method is a promising procedure to break the efficiency-limiting factor and produce a high-performance anode with minimized fabrication effort.  相似文献   
994.
二甲四氯钠(MCPA-Na)是一种广泛用于牧场和果园的除草剂,但由于其生物降解性极低,已成为地下水和浅水中的主要污染物.研究发现,半导体可以有效地辅助降解转化危险化学品.ZnO纳米管因其中空结构和较大的比表面积,而在光催化降解有机物方面备受关注.但是,ZnO只能吸收紫外光,如果将其与窄带隙半导体进行复合,可以有效降低带隙,增强其在可见光区域的光吸收,表现出更好的光催化性能.WO3是一种具有稳定物理化学性质及耐光腐蚀窄带隙半导体.采用WO3修饰ZnO纳米管,能扩展ZnO吸收光的范围以及提高ZnO纳米管的耐光腐蚀性能.本文首先通过电化学合成的方法制备了ZnO纳米管,然后按照不同的W/Zn摩尔比将(NH4)6H2W12O40·XH2O滴加在纳米管表面,并在450 ℃下退火2 h制得ZnO-WO3纳米管阵列.研究了不同WO3含量的ZnO-WO3纳米管光催化降解MCPA-Na性能,并且通过X射线光电子能谱(XPS)、傅里叶红外光谱仪(FTIR)、紫外可见光谱(UV-Vis)和光致发光光谱(PL)等手段研究了复合WO3纳米颗粒后ZnO纳米管半导体光催化性能提高的原因.XPS结果表明,W元素在ZnO-WO3纳米管阵列中以W6+的形式存在.FTIR结果表明,复合WO3后的ZnO-WO3复合半导体上比纯ZnO纳米管表面具有更多的OH-基团.由于OH-可以捕获光生空穴,并转化为具有反应活性的●OH自由基,因此复合WO3能在一定程度上提高ZnO纳米管的光催化活性.UV-Vis结果表明,WO3的复合使得光谱发生明显红移,但随着WO3含量的增加,ZnO-WO3的吸光度明显增加.另外,PL结果表明,适当的复合WO3可以抑制光生电子-空穴的复合.这是因为W6+和晶格氧的相互作用产生了较高不饱和键和表面缺陷,而表面缺陷可以作为光生载流子的陷阱,促进了光生电子和空穴的分离,因而光催化性能提高.在模拟太阳光下研究了不同WO3含量的ZnO纳米管对光催化降解MCPA-Na溶液的性能.发现W/Zn摩尔比为3%的ZnO-WO3样品表现出最好的光催化活性,200 min内其降解率为98.5%.与纯ZnO纳米管相比,其光催化循环性能也有所提高.利用Mott-Schottky测试方法并结合UV-vis结果,我们计算得到不同WO3含量的ZnO-WO3复合半导体导带价带位置.由于WO3导带位置和价带位置都比ZnO的更高,WO3上产生的光生电子会向ZnO的导带移动,而ZnO光生空穴向WO3的价带移动,从而促使光生电子和空穴的分离,提高了光催化性能.但是如果WO3复合的量太大,则在ZnO纳米管上分散性不好,反而成为光生空穴和电子复合中心,导致其光催化活性降低.  相似文献   
995.
A thermo- and pH- dual responsive luminescent hydrogel was successfully constructed by coupling dysprosium-containing polyoxometalates Na9DyW10O36 (DyW10) with the ABA triblock copolymer, where the B block is PEO and the A block is the thermosensitive poly(methoxydi(ethylene glycol) methacrylate-co-N,N-dimethylaminoethyl methacrylate). The complex hybrid underwent a sol-gel phase transition above the lower critical solution temperature (LCST) of the A block. DyW10 was electrostatically encapsulated into the hydrophobic domain of the A block with enhanced photoluminescence. When temperature cooled down, the luminescence could be restored. By addition of acids to protonate the A block, and emission of DyW10 was simultaneously enhanced. Sensitivity of poly(N,N-dimethy laminoethyl methacrylate) (PDMAEMA) to pH also enabled the emission of DyW10/copolymer hydrogel to be reversibly switched by alternating acid/base treatments.  相似文献   
996.
Three fluorescent BINOL-Si complexes (FS1, FS2 and FS3) were rationally designed and synthesized to detect diethyl chlorophosphate (DCP), a mimic of lethal nerve agents. These three fluorescent probes showed green, yellow and orange fluorescence, respectively. Moreover, the series of fluorescent probes has the characteristics of fast response time (≤4 s), low detection limit (0.0097 μmol/L), high sensitivity and naked eye detection. More important, a fiber optic sensor capable of detecting DCP vapor in real time was also prepared for the first time, the lowest detection limits (down to 4.4 ppb) were all lower than that of the IDLH (immediately dangerous to life or health) concentration of Sarin (7.0 ppb).  相似文献   
997.
雷琦锋  王畅  戴卫理  武光军  关乃佳  Michael Hunger  李兰冬 《催化学报》2021,42(7):1176-1184,中插46-中插49
1,2-二醇主要由环氧化合物水合产生、广泛用于防冻剂,聚酯树脂和医药等化学品中间体的生产.研究表明,具有Lewis酸性的含锡沸石分子筛在环氧化物的水合反应中表现出优异的催化性能.环氧化合物是众所周知的碳亲电体之一,主要由烯烃环氧化生成.含Ti(IV)沸石,如Ti-Beta和TS-1,是烯烃环氧化反应的高效催化剂.串联催...  相似文献   
998.
本文基于密度泛函(DFT)结合非平衡格林函数(NEGF)的方法,以具有氧化还原中心的紫罗碱衍生物(N,N'-bis(4-thioalkyl)-4,4'-bipyridinium,HS-4V4-SH)功能分子构造Au(111)/S-4V4-S/Au(111)分子结,详细分析了分子在三种价态V、V+和V2+下的电学性质与分...  相似文献   
999.
Reduced graphene oxide hollow microspheres (rGO HMS) were encapsulated with gold nanoparticles (AuNPs) by spray drying. Scanning electron microscopy, transmission electron microscopy, X-ray diffraction and Raman spectroscopy were used to characterize the AuNP/rGO HMS. When placed on a glassy carbon electrode (GCE), it exhibits excellent electrochemical catalytic properties towards the oxidation of nitrite. The electrocatalytic properties were studied using various electrochemical techniques. Compared to AuNP-decorated graphene sheet based electrodes documented in the literature, the one presented here provides a larger surface area. This enhances the catalytic activity towards nitrite. The electrode, typically operated at a working potential of 0.82 V (vs. SCE), has a linear response in the 5.0 μM to 2.6 mM nitrate concentration range, and a detection limit as low as 0.5 μM (at an S/N ratio of 3).
Graphical abstract Schematic presentation of the synthesis of graphene hollow microspheres encapsulated with of gold nanoparticles (AuNP/rGO HMS) through a spray drying technique. The material was applied to the electrochemical determination of nitrite.
  相似文献   
1000.
The Rose Bengal sensitized intermolecular [2 + 2]-cycloaddition of 3-ylideneoxindoles for the synthesis of spirocyclic oxindoles was developed successfully under visible light irradiation conditions. The cycloaddition products were obtained in good yields (up to 93%) with excellent diastereoselectivity and regioselectivity by using a low loading of Rose Bengal (0.125 mol%) as a triplet sensitizer. This work demonstrates the potential benefits of Rose Bengal in visible light catalysis.  相似文献   
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