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101.
负载型金属纳米催化剂由于其优异的光催化性能,被广泛应用于光催化产氢协同胺类氧化偶联合成高附加值亚胺体系。但在反应过程中,金属表面对H原子和亚胺表现出较强的吸附能力,导致了亚胺易于发生自氢化反应而生成仲胺,显著降低了亚胺的选择性。在本文中,我们证实了在Pd/Ti O2表面构建超薄碳层(Pd/Ti O2@C)是一种解决上述问题的有效策略。在Pd/Ti O2表面构筑的超薄碳层可以有效调控H原子和亚胺在其表面的吸附行为,避免了光催化氧化偶联过程中亚胺的自氢化。因此,Pd/Ti O2@C光催化剂在光催化产氢协同胺类选择性氧化合成亚胺体系中展现出优异的亚胺选择性。本研究提供了一种便捷有效的策略推动负载型金属纳米催化剂在光催化产氢协同合成高附加值产物体系中的应用。 相似文献
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Dengrong Sun Dr. Yanghe Fu Wenjun Liu Lin Ye Dengke Wang Lin Yang Prof. Dr. Xianzhi Fu Prof. Dr. Zhaohui Li 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(42):14279-14285
Metal–organic framework (MOF) NH2‐Uio‐66(Zr) exhibits photocatalytic activity for CO2 reduction in the presence of triethanolamine as sacrificial agent under visible‐light irradiation. Photoinduced electron transfer from the excited 2‐aminoterephthalate (ATA) to Zr oxo clusters in NH2‐Uio‐66(Zr) was for the first time revealed by photoluminescence studies. Generation of ZrIII and its involvement in photocatalytic CO2 reduction was confirmed by ESR analysis. Moreover, NH2‐Uio‐66(Zr) with mixed ATA and 2,5‐diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO2 reduction due to its enhanced light adsorption and increased adsorption of CO2. This study provides a better understanding of photocatalytic CO2 reduction over MOF‐based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO2 reduction. 相似文献
104.
Caiming Tang Caixing Tang Wei Zhan Juan Du Zhifang Wang Xianzhi Peng 《Journal of separation science》2013,36(16):2584-2592
LC‐MS/MS is currently the most selective and efficient tool for the quantitative analysis of drugs and metabolites in the pharmaceutical industry and in clinical assays. However, phase II metabolites sometimes negatively affect the selectivity and efficiency of the LC‐MS/MS method, especially for the metabolites that possess similar physicochemical characteristics and generate the same precursor ions as their parent compounds due to the in‐source collision‐induced dissociation during the ionization process. This paper proposes some strategies for examining co‐eluting metabolites existing in real samples, and further assuring whether these metabolites could affect the selectivity and accuracy of the analytical methods. Strategies using precursor‐ion scans and product‐ion scans were applied in this study. An example drug, namely, caffeic acid phenethyl ester, which can generate many endogenous phase II metabolites, was selected to conduct this work. These metabolites, generated during the in vivo metabolic processes, can be in‐source‐dissociated to the precursor ions of their parent compounds. If these metabolites are not separated from their parent compounds, the quantification of the target analytes (parent compounds) would be influenced. Some metabolites were eluted closely to caffeic acid phenethyl ester on LC columns, although long columns and relatively long elution programs were used. The strategies can be utilized in quantitative methodologies that apply LC‐MS/MS to assure the performance of selectivity, thus enhancing the reliability of the experimental data. 相似文献
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Junyi Li Baiyi Zu Ying Zhang Xianzhi Guo Huiqi Zhang 《Journal of polymer science. Part A, Polymer chemistry》2010,48(15):3217-3228
This article describes for the first time the development of a new polymerization technique by introducing iniferter‐induced “living” radical polymerization mechanism into precipitation polymerization and its application in the molecular imprinting field. The resulting iniferter‐induced “living” radical precipitation polymerization (ILRPP) has proven to be an effective approach for generating not only narrow disperse poly(ethylene glycol dimethacrylate) microspheres but also molecularly imprinted polymer (MIP) microspheres with obvious molecular imprinting effects towards the template (a herbicide 2,4‐dichlorophenoxyacetic acid (2,4‐D)), rather fast template rebinding kinetics, and appreciable selectivity over structurally related compounds. The binding association constant Ka and apparent maximum number Nmax for the high‐affinity sites of the 2,4‐D imprinted polymer were determined by Scatchard analysis and found to be 1.18 × 104 M?1 and 4.37 μmol/g, respectively. In addition, the general applicability of ILRPP in molecular imprinting was also confirmed by the successful preparation of MIP microspheres with another template (2‐chloromandelic acid). In particular, the living nature of ILRPP makes it highly useful for the facile one‐pot synthesis of functional polymer/MIP microspheres with surface‐bound iniferter groups, which allows their direct controlled surface modification via surface‐initiated iniferter polymerization and is thus of great potential in preparing advanced polymer/MIP materials. © 2010 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 48: 3217–3228, 2010 相似文献
108.
The grafting reaction of SnMe4 on the surface of Pt/NaY zeolite was investigated in a 1.6 × 104 Pa hydrogen atmosphere. The chemical compositions, structure and properties of the resulting solid were characterized by in situ FTIR, ICP, XRD, XPS, temperature programmed decomposition and nitrogen adsorption. The results show that Pt atoms of Pt/NaY zeolite react with tetramethyltin to form a bimetallic Me3Sn? Pt surface species in the presence of hydrogen at 353 K. The reaction does not destroy the zeolite framework, while its surface properties are changed. The BET surface area and the pore volume of the zeolite decrease significantly. The CO chemisorption results and the XPS results show that the electronic properties of the modified Pt atoms on the surface of NaY zeolite are altered remarkably by the inductive effect of electron between Pt and methyl groups. The grafted product has excellent selective hydrogenation of furfural to furfuryl alcohol. Copyright © 2007 John Wiley & Sons, Ltd. 相似文献
109.
稀土镍磷非晶合金的PAS和DSC研究 总被引:1,自引:0,他引:1
文中报导了在Ni-P非晶合金中掺入稀土元素钇(Y)的诱导共沉积方法;并通过正电子湮没寿命谱和示差扫描量热计研究了Ni-P-Y非晶合金的缺陷态及热稳定性;还从不同角度讨论了稀土元素对该合金热稳定性的贡献。 相似文献
110.
Baiyi Zu Ying Zhang Xianzhi Guo Huiqi Zhang 《Journal of polymer science. Part A, Polymer chemistry》2010,48(3):532-541
The first application of atom transfer radical “bulk” polymerization (ATRBP) in molecular imprinting is described, which provides molecularly imprinted polymers (MIPs) with obvious imprinting effects towards the template, very fast binding kinetics, and an appreciable selectivity over structurally related compounds. In comparison with the MIP prepared via the normally used traditional “bulk” free radical polymerization (BFRP), the MIPs obtained via ATRBP showed somewhat lower binding capacities and apparent maximum numbers Nmax for high‐affinity sites as well as quite similar binding association constants Ka for high‐affinity sites and high‐affinity site densities, in contrast with the previous reports (e.g., nitroxide/iniferter‐mediated “bulk” polymerization provided MIPs with improved properties). This is tentatively ascribed to the occurrence of rather fast gelation process in ATRBP, which greatly restricted the mobility of the chemical species, leading to a heavily interrupted equilibrium between dormant species and active radicals and heterogeneous polymer networks. In addition, the general applicability of ATRBP was also confirmed by preparing MIPs for different templates. This work clearly demonstrates that applying controlled radical polymerizations (CRPs) in molecular imprinting not always benefits the binding properties of the resultant MIPs, which is of significant importance for the rational use of CRPs in generating MIPs with improved properties. © 2009 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 48: 532–541, 2010 相似文献