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排序方式: 共有129条查询结果,搜索用时 31 毫秒
51.
Hao Zhang Aleksei Bolshakov Raghavendra Meena Gustavo A. Garcia A. Iulian Dugulan Alexander Parastaev Guanna Li Emiel J. M. Hensen Nikolay Kosinov 《Angewandte Chemie (International ed. in English)》2023,62(32):e202306196
Non-oxidative coupling of methane is a promising route to obtain ethylene directly from natural gas. We synthesized siliceous [Fe]zeolites with MFI and CHA topologies and found that they display high selectivity (>90 % for MFI and >99 % for CHA) to ethylene and ethane among gas-phase products. Deactivated [Fe]zeolites can be regenerated by burning coke in air. In situ X-ray absorption spectroscopy demonstrates that the isolated Fe3+ centers in zeolite framework of fresh catalysts are reduced during the reaction to the active sites, including Fe2+ species and Fe (oxy)carbides dispersed in zeolite pores. Photoelectron photoion coincidence spectroscopy results show that methyl radicals are the reaction intermediates formed upon methane activation. Ethane is formed by methyl radical coupling, followed by its dehydrogenation to ethylene. Based on the observation of intermediates including allene, vinylacetylene, 1,3-butadiene, 2-butyne, and cyclopentadiene over [Fe]MFI, a reaction network is proposed leading to polyaromatic species. Such reaction intermediates are not observed over the small-pore [Fe]CHA, where ethylene and ethane are the only gas-phase products. 相似文献
52.
Dr. Tiancheng Pu Jiaqi Ding Fanxing Zhang Dr. Ke Wang Ning Cao Prof. Emiel J. M. Hensen Prof. Pengfei Xie 《Angewandte Chemie (International ed. in English)》2023,62(40):e202305964
The pursuit of high metal utilization in heterogeneous catalysis has triggered the burgeoning interest of various atomically dispersed catalysts. Our aim in this review is to assess key recent findings in the synthesis, characterization, structure-property relationship and computational studies of dual-atom catalysts (DACs), which cover the full spectrum of applications in thermocatalysis, electrocatalysis and photocatalysis. In particular, combination of qualitative and quantitative characterization with cooperation with DFT insights, synergies and superiorities of DACs compare to counterparts, high-throughput catalyst exploration and screening with machine-learning algorithms are highlighted. Undoubtably, it would be wise to expect more fascinating developments in the field of DACs as tunable catalysts. 相似文献
53.
Selective Coke Combustion by Oxygen Pulsing During Mo/ZSM‐5‐Catalyzed Methane Dehydroaromatization
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Dr. Nikolay Kosinov Ferdy J. A. G. Coumans Evgeny Uslamin Prof. Freek Kapteijn Prof. Emiel J. M. Hensen 《Angewandte Chemie (International ed. in English)》2016,55(48):15086-15090
Non‐oxidative methane dehydroaromatization is a promising reaction to directly convert natural gas into aromatic hydrocarbons and hydrogen. Commercialization of this technology is hampered by rapid catalyst deactivation because of coking. A novel approach is presented involving selective oxidation of coke during methane dehydroaromatization at 700 °C. Periodic pulsing of oxygen into the methane feed results in substantially higher cumulative product yield with synthesis gas; a H2/CO ratio close to two is the main side‐product of coke combustion. Using 13C isotope labeling of methane it is demonstrated that oxygen predominantly reacts with molybdenum carbide species. The resulting molybdenum oxides catalyze coke oxidation. Less than one‐fifth of the available oxygen reacts with gaseous methane. Combined with periodic regeneration at 550 °C, this strategy is a significant step forward, towards a process for converting methane into liquid hydrocarbons. 相似文献
54.
55.
负载型纳米金催化剂由于其独特的化学性质在一系列氧化反应中受到广泛关注.其中,一氧化碳氧化不仅在实际应用领域(如汽车尾气处理)发挥重要作用,而且作为一种理想的模型反应用以深入研究和理解催化剂的构效关系.为了获得高效的纳米金催化剂,我们需要把金负载到载体上,载体不仅为金的分散提供必要的表面,而且还会和金产生相互作用,这种金... 相似文献
56.
Crystal Structure of N,N′-Bis(trimethylsilyl)-imidazoliumiodide [(Me3Si)2(C3H3N2)]+I? Me3SiI forms with N-Trimethylsiylimidazole (NTMSI) a 1:1 compound which is stable at room temperature. Single crystals can be isolated from a solution of chloroform. The X-ray crystal structure investigation proves an ionic structure. 相似文献
57.
Synthesis and Crystal Structure Determination of Hexachloro-μ-dichloro-bis[N-(trimethylsilyl)imidazol]dititanium Chloroform (1/2) Hexachloro-μ-dichloro-bis[N-(trimethylsilyl)-imidazol]dititanium chloroform (1/2) 1 has been prepared by the reaction of titanium tetrachloride with N-trimethylsilylimidazole (NTMSI) in chloroform solution as orange crystals. The structure consists of two distorted TiCl5N octahedrons, which are connected by two chlorine atoms via common edges to a centrosymmetric dimer [Ti2Cl8(NTMSI)2] · 2 CHCl3. The N-trimethylsilylimidazole ligands each are located at one axial position of each octahedron, whereas the equatorial positions are occupied by the chloro ligands. The results presented are discussed assuming a gradual formation of an 1 : 1 and 1 : 2 adduct. 相似文献
58.
Using a statistical shell-model, the equilibrium internuclear distances and total molecular energies have been computed for Li 2 + , Li2, Na 2 + and Na2. The results are in good agreement with experimental data. 相似文献
59.
Crystal- and Molecular Structures of Chlorotrispyridinium-bis-(tetrachloroaluminate(III)) and a New Modification of Pyridinium Chloride The compounds PyHCl and ((PyH)3Cl)(AlCl4)2 are formed by hydrolysis during the synthesis of adducts in the system AlCl3/pyridine. The second room temperature modification of PyHCl crystallizes in the space group P21/c with the lattice constants a = 847.9(3), b = 1770.2(3), c = 801.9(3) pm, β = 95.23(3)°, Z = 8. The atomic parameters were refined from 4471 measured intensities to R(F) = 6,9%. The N? Cl distances are 306.8(7) and 311.0(8) pm. The unit cell of ((PyH)3Cl)(AlCl4)2 is orthorhombic (space group Pbca) and has the lattice constants a = 1306.3(4), b = 1589.4(4), c = 2708.6(7) pm, Z = 8. The crystal structure was refined from 7226 measured intensities to R(F) = 6.7%. The cation shows three pyridinium ions to have NH…?Cl hydrogen bonds to a central positioned chloride ion with N? Cl distances of 301.4(7), 305(1) and 306(1) pm. 相似文献
60.
Ionic Structures of 4- and 5-coordinated Silicon. Novel Ionic Crystal Structures of 4- and 5-coordinated Silicon: [Me3Si(NMI)]+ Cl?, [Me2HSi(NMI)2]+ Cl?, [Me2Si(NMI)3]2+ 2 Cl?. NMI Me3SiCl forms with N-Methylimidazole (NMI) a crystalline 1:1-compound which is stable at room temperature. The X-ray single crystal investigation proves the ionic structure [Me3Si(NMI)]+Cl? 1 which is the result of the cleavage of the Si? Cl bond and the addition of an NMI-ring. The reaction of Me2HSiCl with NMI (in the molar ratio of 1:2), under cleavage of the Si? Cl bond and co-ordination of two NMI rings, yields the compound [Me2HSi(NMI)2]+Cl? 2 . The analogous reaction of Me2SiCl2 with NMI (molar ratio 2:1) leads to a compound which consists of Me2SiCl2 and NMI in the molar ratio of 1:2. During the sublimation single crystals of the compound [Me2Si(NMI)3]2+ 2 Cl?. NMI 3 are formed. 相似文献