Mantle-derived gaseous components in ore-forming fluids of the Xiangshan uranium

The Xiangshan U deposit, the largest hydrothermal U deposit in China, is hosted in late Jurassic felsic volcanic rocks although the U mineralization post dates the volcanics by at least 20 Ma. The mineralization coincides with intrusion of local mantle-derived mafic dykes formed during Cretaceous crustal extension in South China. Ore-forming fluids are rich in CO2, and U in the fluid is thought to have been dissolved in the form of UO2 (CO3)22− and UO2 (CO3) 34− complexes. This paper provides He and Ar isotope data of fluid inclusions in pyrites and C isotope data of calcites associated with U mineralization (pitchblende) in the Xiangshan U deposit. He isotopic compositions range between 0.1 and 2.0Ra (where Ra is the 3He/4He ratio of air=1.39×10−6) and correlates with 40Ar/36Ar; although there is potential for significant 3He production via 6Li(n,α)3H(β)3He reactions in a U deposit (due to abundant neutrons), nucleogenic production cannot account for either the 3He concentration in these fluids, nor the correlations between He and Ar isotopic compositions. It is more likely that the high 3He/4He ratios represent trapped mantle-derived gases. A mantle origin for the volatiles of Xiangshan is consistent with the δ13C values of calcites, which vary from −3.5‰ to −7.7‰, overlapping the range of mantle CO2. The He, Ar and CO2 characteristics of the ore-forming fluids responsible for the deposit are consistent with mixing between 3He- and CO2-rich mantle-derived fluids and CO2-poor meteoric fluids. These fluids were likely produced during Cretaceous extension and dyke intrusion which permitted mantle-derived CO2 to migrate upward and remobilize U from the acid volcanic source rocks, resulting in the formation of the U deposit. Subsequent decay of U within the fluid inclusions has reduced the 3He/4He ratio, and variations in U/3He result in the range in 3He/4He observed with U/3He ratios in the range 5–17×103 likely corresponding to U concentrations in the fluids b0.2 ppm.

Graphitic nanofilaments as novel support of Ru-Ba catalysts for ammonia synthesis

A novel graphitic-nanofilament-(GNF-) supported Ru-Ba catalyst is prepared and used in ammonia synthesis reaction. The Ru-Ba/GNFs catalyst shows remarkably high activity and stability for ammonia synthesis, which can be attributed to high purity and graphitization of GNFs with unique structure. TEM micrographs of the Ru-Ba/GNFs catalysts show that Ru metal particles uniformly disperse on the outer wall of GNFs, and the particles become bigger than that before ammonia synthesis reaction after 50 h of operation at 500degreesC and 7.0 MPa, probably due to the Ru crystals covered by promoter and support materials and/or sintering of Ru crystals. (C) 2002 Elsevier Science (USA).

Ammonia synthesis over Ru/C catalysts with different carbon supports promoted by barium and potassium compounds

Ammonia synthesis over ruthenium catalysts supported on different carbon materials using Ba or K compounds as promoters has been investigated. Ba(NO3)(2), KOH, and KNO3 are used as the promoter or promoter precursor, and activated carbon (AC), activated carbon fiber (ACF). and carbon molecular sieve (CMS) are used as the support. The activity measurement for ammonia synthesis was carried out in a flow micro-reactor under mild conditions: 350-450 degreesC and 3.0 MPa. Results show that KOH promoter was more effective than KNO3. and that Ba(NO3)(2) was the most effective promoter among the three. The roles of promoters can be divided into the electronic modification of ruthenium, the neutralization of surface functional groups on the carbon support and the ruthenium precursor. The catalyst with AC as the support gave the highest ammonia concentration in the effluent among the supports used, while the catalyst with ACF as the support showed the highest turnover-frequency (TOF) value. It seems that the larger particles of Ru on the carbon supports are more active for ammonia synthesis in terms of TOF value. (C) 2001 Elsevier Science B.V. All rights reserved.

The ion-molecule reaction after multiphoton ionization in the binary cluster of ammonia and methanol

The binary cluster (CH3OH)(n)(NH3)(m) was studied by using a multiphoton ionization time-of-flight mass spectrometer (MPI-TOFMS). The measured two series of protonated cluster ions: (CH3OH)(n)H+ and (CH3OH)(n)NH4+ (1 less than or equal to n less than or equal to 14) were attributed to the ion-molecule reaction in the binary cluster ions. The mixed cluster of CH3OD with ammonia was also studied. The results implied that the proton transfer probability from the OD group was larger than that from CH3 group. The ab initio calculation of the binary cluster was carried out at the HF/STO-3G and MP2/6-31G** levels of theory, and indicated that the latter process of the proton transfer must overcome a barrier of similar to 29 kcal/mol. (C) 1999 Elsevier Science B.V. All rights reserved.

Photoelectron spectroscopy of ammonia via a fast predissociative state

We report a study on resonance enhanced multiphoton ionization photoelectron spectroscopy (REMPI-PES) involving the fast predissociative (A) over tilde state of ammonia, using nano- and femtosecond lasers. The multiphoton scheme involves (1 + 1), (2 + 2), (2 + 2) + 1 and (2 + 2) + 2 photon processes. We have found a progression of stretching vibrations nu(1) in the PE spectrum when pumping NH3 (A) over tilde upsilon(2) = 0, 1 and 3 as intermediate states. The stretching vibration intensity distributions in the photoelectron spectrum are calculated by using the Chebychev method of the wavepacket propagation. The femtosecond spectrum shows a similar feature to the nanosecond spectrum. However, high laser power also causes band broadening and shifting effect as well as above threshold multiphoton ionization.

Covariance analysis of the Coulomb explosion of ammonia induced by intense nanosecond laser at 532 nm

The Coulomb explosion of ammonia clusters induced by nanosecond laser at 532 not with an intensity of similar to 10(12) Wcm(-2) has been studied by time of flight mass spectrometry. The dominant multiply charged ions are N3+ and N2+ with kinetic energies of 110 and 50 eV respectively. The electrons generated from the multiphoton ionization are heated through inverse bremsstrahlung by the laser field when colliding with neutral or ionic particles. When their energies surpass the corresponding ionization potentials of the molecules or ions, the subsequent electron impact ionization may take place thus resulting in multi-charged nitrogen ions. Covariance analysis is made to study the possible pathways of the Coulomb explosion.

爆轰波在楔面上反射数值分析

应用基元反应模型和频散可控耗散格式(DCD)对氢氧爆轰波在楔面反射进行了数值模拟.计算中氢氧混合物的化学反应采用了8种组分20个反应方程式.在处理化学反应引起的刚性问题时采用了时间算子分裂的方法.模拟了爆轰波在楔面反射由马赫反射向规则反射转变的过程,得到了反射转变临界角,同时考虑了初始压力和组分的影响,并和实验及理论分析结果进行了比较,结果是令人满意的.