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911.
Electrochemical Synthesis of Tetrahexahedral Rhodium Nanocrystals with Extraordinarily High Surface Energy and High Electrocatalytic Activity 下载免费PDF全文
Neng‐Fei Yu Dr. Na Tian Dr. Zhi‐You Zhou Long Huang Jing Xiao Yu‐Hua Wen Prof. Shi‐Gang Sun 《Angewandte Chemie (International ed. in English)》2014,53(20):5097-5101
Noble metal nanocrystals (NCs) enclosed with high‐index facets hold a high catalytic activity thanks to the high density of low‐coordinated step atoms that they exposed on their surface. Shape‐control synthesis of the metal NCs with high‐index facets presents a big challenge owing to the high surface energy of the NCs, and the shape control for metal Rh is even more difficult because of its extraordinarily high surface energy in comparison with Pt, Pd, and Au. The successful synthesis is presented of tetrahexahedral Rh NCs (THH Rh NCs) enclosed by {830} high‐index facets through the dynamic oxygen adsorption/desorption mediated by square‐wave potential. The results demonstrate that the THH Rh NCs exhibit greatly enhanced catalytic activity over commercial Rh black catalyst for the electrooxidation of ethanol and CO. 相似文献
912.
Pumping through Porous Hydrophobic/Oleophilic Materials: An Alternative Technology for Oil Spill Remediation 下载免费PDF全文
Jin Ge Yin‐Dong Ye Hong‐Bin Yao Xi Zhu Xu Wang Liang Wu Jin‐Long Wang Prof. Hang Ding Prof. Ni Yong Prof. Ling‐Hui He Prof. Dr. Shu‐Hong Yu 《Angewandte Chemie (International ed. in English)》2014,53(14):3612-3616
Recently, porous hydrophobic/oleophilic materials (PHOMs) have been shown to be the most promising candidates for cleaning up oil spills; however, due to their limited absorption capacity, a large quantity of PHOMs would be consumed in oil spill remediation, causing serious economic problems. In addition, the complicated and time‐consuming process of oil recovery from these sorbents is also an obstacle to their practical application. To solve the above problems, we apply external pumping on PHOMs to realize the continuous collection of oil spills in situ from the water surface with high speed and efficiency. Based on this novel design, oil/water separation and oil collection can be simultaneously achieved in the remediation of oil spills, and the oil sorption capacity is no longer limited to the volume and weight of the sorption material. This novel external pumping technique may bring PHOMs a step closer to practical application in oil spill remediation. 相似文献
913.
Transition from π Radicals to σ Radicals: Substituent‐Tuned Cyclization of Hydrazonyl Radicals 下载免费PDF全文
Xiu‐Long Yang Prof. Dr. Wei Yu Prof. Dr. Bing Han 《Angewandte Chemie (International ed. in English)》2014,53(12):3158-3162
Hydrazonyl radicals are known for their π‐electronic structures; however, their σ‐electronic structures have not been reported as yet. Herein, we show that readily accessible β,γ‐ and γ,δ‐unsaturated N‐trichloroacetyl and N‐trifluoroacetyl hydrazones can be conveniently converted into hydrazonyl σ radicals, which subsequently undergo 5‐exo‐trig radical cyclization at the N1 or N2 atom to form pyrazolines and azomethine imines, respectively. 相似文献
914.
Metal‐Free Aminosulfonylation of Aryldiazonium Tetrafluoroborates with DABCO⋅(SO2)2 and Hydrazines 下载免费PDF全文
Danqing Zheng Yuanyuan An Dr. Zhenhua Li Prof. Dr. Jie Wu 《Angewandte Chemie (International ed. in English)》2014,53(9):2451-2454
The coupling of aryldiazonium tetrafluoroborates, DABCO?(SO2)2, and hydrazines under metal‐free conditions leads to the formation of aryl N‐aminosulfonamides. The reaction proceeds smoothly at room temperature and shows broad functional‐group tolerance. A radical process is proposed for this transformation. 相似文献
915.
Hexafluoroantimonic Acid Catalysis: Formal [3+2+2] Cycloaddition of Aziridines with Two Alkynes 下载免费PDF全文
Ming‐Bo Zhou Ren‐Jie Song Prof. Dr. Jin‐Heng Li 《Angewandte Chemie (International ed. in English)》2014,53(16):4196-4199
A practical method for the synthesis of azepine derivatives, a typical seven‐membered heterocyclic ring system, was developed and involves the use of hexafluoroantimonic acid to catalyze a formal [3+2+2] cycloaddition of aziridines with two alkynes. This method was applicable to two of the same or different terminal alkynes for the [3+2+2] cycloaddition with unactivated aziridines, and furnished the corresponding azepine derivatives in good yields with good levels of chemo‐ and regioselectivity. The mechanism was also discussed according to the results of the in situ HRMS and 1H NMR analysis. 相似文献
916.
Dr. Jie Liang Dr. Jie Su Prof. Yingxia Wang Yanping Chen Prof. Xiaodong Zou Fuhui Liao Prof. Jianhua Lin Prof. Junliang Sun 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(49):16097-16101
A germanate zeolite, PKU‐14, with a three‐ dimensional large‐pore channel system was structurally characterized by a combination of high‐resolution powder X‐ray diffraction, rotation electron diffraction, NMR, and IR spectroscopy. Ordered Ge4O4 vacancies inside the [46.612] cages has been found in PKU‐14, in which a unique (H2O)2 dimer was located at the vacancies and played a structure‐directing role. It is the first time that water clusters are found to be templates for ordered framework vacancies. 相似文献
917.
Photochemically Engineering the Metal–Semiconductor Interface for Room‐Temperature Transfer Hydrogenation of Nitroarenes with Formic Acid 下载免费PDF全文
Dr. Xin‐Hao Li Yi‐Yu Cai Ling‐Hong Gong Dr. Wei Fu Dr. Kai‐Xue Wang Dr. Hong‐Liang Bao Dr. Xiao Wei Dr. Jie‐Sheng Chen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(50):16732-16737
A mild photochemical approach was applied to construct highly coupled metal–semiconductor dyads, which were found to efficiently facilitate the hydrogenation of nitrobenzene. Aniline was produced in excellent yield (>99 %, TOF: 1183) using formic acid as hydrogen source and water as solvent at room temperature. This general and green catalytic process is applicable to a wide range of nitroarenes without the involvement of high‐pressure gases or sacrificial additives. 相似文献
918.
Coverage‐ and Temperature‐Dependent Metalation and Dehydrogenation of Tetraphenylporphyrin on Cu(111) 下载免费PDF全文
Michael Röckert Matthias Franke Quratulain Tariq Stefanie Ditze Michael Stark Patrick Uffinger Daniel Wechsler Upendra Singh Dr. Jie Xiao Dr. Hubertus Marbach Prof. Dr. Hans‐Peter Steinrück Dr. Ole Lytken 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(29):8948-8953
Using temperature‐programmed desorption, supported by X‐ray photoelectron spectroscopy and scanning tunneling microscopy, a comprehensive overview of the main reactions of 5,10,15,20‐tetraphenyl‐21H,23H‐porphyrin (2HTPP) on Cu(111) as a function of coverage and temperature is obtained. Three reactions were identified: metalation with Cu substrate atoms, stepwise partial dehydrogenation, and finally complete dehydrogenation. At low coverage the reactions are independent of coverage, but at higher coverage metalation becomes faster and partial dehydrogenation slower. This behavior is explained by a weaker interaction between the iminic nitrogen atoms and the Cu(111) surface in the high‐coverage checkerboard structure, leading to faster metalation, and the stabilizing effect of T‐type interactions in the CuTPP islands formed at high coverage after metalation, leading to slower dehydrogenation. Based on the amount of hydrogen released and the appearance in STM, a structure of the partially dehydrogenated molecule is suggested. 相似文献
919.
Calcite Microneedle Arrays Produced by Inorganic Ion‐Assisted Anisotropic Dissolution of Bulk Calcite Crystal 下载免费PDF全文
Xia Long Ruijie Meng Weike Wu Prof. Yurong Ma Prof. Dong Yang Prof. Limin Qi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(15):4264-4272
Besides studies on the mineralization process, research on the demineralization of minerals provides another way to understand the crystallization mechanism of biominerals and fabricate crystals with complicated morphologies. The formation of ordered arrays of c‐axis‐oriented calcite microneedles with a tri‐symmetric structure and lengths of more than 20 μm was realized on a large scale for the first time through anisotropic dissolution of calcite substrates in undersaturated aqueous solution in the presence of ammonium salts. The lengths and the aspect ratios of the calcite microneedles can be tuned by simply changing the concentrations of the ammonium salts and the dissolution time. The shape of the transverse cross sections of the calcite microneedles obtained in the presence of NH4Cl and NH4Ac is almost regularly triangular. The tri‐symmetric transverse cross‐section geometry of the calcite microneedles could be attributed to the tri‐symmetric feature of rhombohedral calcite atomic structures, the synergetic interactions between electrostatic interaction of ammonium ions and dangling surface carbonate groups, and the ion incorporation of halide ions. 相似文献
920.
Changduo Pan Ablimit Abdukader Jie Han Prof. Dr. Yixiang Cheng Prof. Dr. Chengjian Zhu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(13):3606-3609
A ruthenium‐catalyzed direct C7 amidation of indoline C?H bonds with sulfonyl azides was developed. This procedure allows the synthesis of a variety of 7‐amino‐substituted indolines, which are useful in pharmaceutical. The good functional tolerances, as well as the mild conditions, are prominent feature of this method. 相似文献