Hydrogen Incorporation in Crystalline Jadeite: Insight from First Principles Calculations     

ZHANG Xiaoling  FAN Xiaoyu  MENG Dawei  WU Xiuling  LIU Weiping 《《地质学报》英文版》2016,90(3):939-945

Hydrogen incorporation is critical for explaining defect energies, structure parameters and other physical characteristics of minerals and understanding mantle dynamics. This work analyzed the hydrogen complex defects in jadeite by the plane-wave pseudo-potential method based on density functional theory, and optimized the atomic positions and lattice constants in all configurations(different defective systems). Incorporation mechanisms considered for hydrogen(H) in jadeite include:(1) hydrogen incorporating with the O2 site oxygen and coexisting with M2 vacancy;(2) one H atom combined with an Al atom replacing Si in tetrahedron;(3) 4H atoms directly replacing Si in tetrahedron and(4) 3H atoms replacing Al on the M1 site. The four incorporation mechanisms mentioned above form the corresponding V_(Na)-H_i, Al_(Si)-H_i, V_(Si)-4H_i and V_(Al)-3H_i point defects. The molecular dynamics simulation to the ideal, V_(Na)-H_i, Al_(Si)-H_i, V_(Si)-4H_i and V_(Al)-3H_i point defects under the P-T conditions of 900 K, 2 GPa, the V_(Na)-H_i and Al_(Si)-H_i point defects under different pressures at T = 900 K, and Al_(Si)-H_i point defects under different temperatures at P = 3 GPa was performed to examine the preferential mode of hydrogen incorporation in jadeite by means of first-principles calculations. The calculations show that the averaged O–H bond-length in the hydrogen point defects system decreased in the order of Al_(Si)-H_i, V_(Na)-H_i, V_(Si)-4H_i and V_(Al)-3H_i. V_(Na)-H_i complex defects result in a contraction of the jadeite volume and the presence of Al_(Si)-H_i, V_(Si)-4H_i and V_(Al)-3H_i defects could increase the supercell volume, which is the most obvious in the V_(Al)-3H_i defects. The energy of formation of Al_(Si)-H_i and V_(Al)-3H_i complex defects was much lower than that of other defect systems. The V_(Al)-3H_i defects system has the lowest energy and the shortest O–H bond-length, suggesting that this system is the most favorable. The analytical results of vacancy formation energy, O–H bondlength, and the stability of the hydrogen defects in jadeite have suggested that the preferred hydration incorporation mode in jadeite is V_(Al)-3H_i complex defect.  相似文献   

Simultaneous Measurement of Hydrogen Peroxide and Fe Species (Fe(II) and Fe<Subscript>(tot)</Subscript>) in Okinawa Island Seawater: Impacts of Red Soil Pollution     

Takemitsu?ArakakiEmail author  Hiroyuki?Fujimura  Asha?Mansour?Hamdun  Kouichirou?Okada  Hiroaki?Kondo  Tamotsu?Oomori  Akira?Tanahara  Hatsuo?Taira 《Journal of Oceanography》2005,61(3):561-568

The northern part of Okinawa Island suffers from red soil pollution—runoff of red soil into coastal seawater—which damages coastal ecosystems and scenery. To elucidate the impacts of red soil pollution on the oxidizing power of seawater, hydrogen peroxide (HOOH) and iron species including Fe(II) and total iron (Fe_(tot), defined as the sum of Fe(II) and Fe(III)) were measured simultaneously in seawater from Taira Bay (red-soil-polluted sea) and Sesoko Island (unpolluted sea), off the northern part of Okinawa Island, Japan. We performed simultaneous measurements of HOOH and Fe(II) because the reaction between HOOH and Fe(II) forms hydroxyl radical (•OH), the most potent environmental oxidant. Gas-phase HOOH concentrations were also measured to better understand the sources of HOOH in seawater. Both HOOH and Fe(II) in seawater showed a clear diurnal variation, i.e. higher in the daytime and lower at night, while Fe_(tot) concentrations were relatively constant throughout the sampling period. Fe(II) and Fe_(tot) concentrations were approximately 58% and 19% higher in red-soil-polluted seawater than in unpolluted seawater. Gas-phase HOOH and seawater HOOH concentrations were comparable at both sampling sites, ranging from 1.4 to 5.4 ppbv in air and 30 to 160 nM in seawater. Since Fe(II) concentrations were higher in red-soil-polluted seawater while concentrations of HOOH were similar, •OH would form faster in red-soil-polluted seawater than in unpolluted seawater. Since the major scavenger of •OH, Br⁻, is expected to have similar concentrations at both sites, red-soil-polluted seawater is expected to have higher steady-state •OH concentrations.  相似文献   

The relationship between seagrass (Posidonia oceanica) decline and sulfide porewater concentration in carbonate sediments   总被引：2，自引：0，他引：2  

Maria Ll. Calleja  Núria Marb  Carlos M. Duarte 《Estuarine, Coastal and Shelf Science》2007,73(3-4):583-588

In this study we test the hypothesized negative relationship between seagrass status and porewater hydrogen sulfide (H₂S) levels, through a comparative analysis within a range of seven Posidonia oceanica meadows growing over carbonate sediments in the NW Mediterranean Sea around Mallorca Island. The studied meadows range from meadows growing on sediments with very low sulfide porewater concentrations (4.6 μM) to those growing over higher sulfide conditions (33.5 μM). Organic matter content, sulfate reduction rates and sulfide porewater concentrations in the sediments were determined concurrently with the assessment of demographic plant dynamics (specific mortality and net population growth rates). Sulfide porewater concentration increased with increasing organic matter content in the sediment, while net population growth decreased significantly with low increases of sulfide concentrations. Our results confirm the previously suspected vulnerability of seagrass meadows growing on carbonate sediments to increased sulfide levels. An excess of 10 μmols H₂S L⁻¹ porewater is identified to already conduce P. oceanica meadows to decline, which this study identifies, particularly, as strongly sensitive to sulfides. The results reported here suggest that even moderate increases in organic carbon inputs may lead to enhancement of dissolved sulfides and may be an important factor for seagrass status in these iron-depleted carbonate sediments from the Mediterranean Sea.  相似文献   

Mats of Beggiatoa bacteria reveal that organic pollution from lumber mills inhibits growth of Zostera marina     

Joel K. Elliott  Erin Spear  & Sandy Wyllie-Echeverria 《Marine Ecology》2006,27(4):372-380

The objectives of this study were to determine the distribution and abundance of Zostera marina (eelgrass) in relation to the distribution of the mat forming bacteria Beggiatoa spp., and the levels of sulfide and organic material (wood waste) in the sediment. Underwater videography and intertidal surveys were used to map the distribution and abundance of Z. marina beds and Beggiatoa in the nearshore area of Commencement Bay, WA (USA), a location that has a long history of sawmill activity. Zostera marina occurred from the intertidal to ?6 m mean lower low water (MLLW) on sandy substrates in areas with low levels of sulfide (<50 μm ) and organic material (<5 % total volatile solids). Areas with high sulfide levels (>200 μm ) occurred where there were significant amounts of organic material in the sediments, which was found to be wood waste that had been discarded from sawmills. Zostera marina was absent from the intertidal and occurred at lower densities in areas with high sulfide levels. In contrast, mats of Beggiatoa were only found in areas where the sulfide levels were >1000 μm and there were significant deposits of wood. Thus, the negative correlation between the distribution and abundance of Z. marina and Beggiatoa suggests that the presence of Beggiatoa mats could be used as a biological indicator of inhibiting levels of hydrogen sulfide in the marine environment.  相似文献   

Discharge Control on Boundary of Tidal Models and Measuring Techniques of Low Current Velocity     

Li Guochen Xu Jinhuan Associate Prof.  Dept. of Navigation  Ocean Eng.  Hohai University  Nanjing Lecturer  Dept. of Navigation  Ocean Eng.  Hohai University  Nanjing 《中国海洋工程》1992,(3)

This paper describes the discharge control technique on boundary used in two models, one is the model of hot water drainning in Dayawan Nyclear Power Plant, Guangdong, and the other is the model for trainhing the sand bar at the Guanhe Estuary, Jiangsu. Many years of application shows that this technique has the advantages of good reliability, repeatability and validity. The speedometer of hydrogen bubble is also introduced in this paper. The device can display and store tracing lines in a computer, and help operators to obtain the value and direction of transient velocity of a nonsteady current, thus, the problem of measurment of low current velocity in tidal model tests is solved and the automation of the measurement of current velocity is realized.  相似文献   

非晶态Ni-S合金在碱液中析氢反应(HER)机理的研究   总被引：1，自引：0，他引：1  

杜敏  高荣杰 《中国海洋大学学报(自然科学版)》2003,33(6):961-968

本文研究了非晶态 Ni- S合金的析氢反应机理。用稳态极化曲线研究非晶态 Ni- S合金的极化行为 ,得到其反应的动力学参数塔菲尔斜率和表观反应活化能。用断电流法和循环伏安法研究氢原子的吸附和中间态粒子。考察电极表面粗糙度、活性粒子表面吸附浓度等因素 ,综合分析得出 Ni- S合金电极具有高催化活性的原因及其 HER电催化机理  相似文献   

Flux of Reduced Sulfur Gases Along a Salinity Gradient in Louisiana Coastal Marshes   总被引：3，自引：0，他引：3  

R. D. Delaune  I. Devai  C. W. Lindau 《Estuarine, Coastal and Shelf Science》2002,54(6):1003

Seasonal and diurnal reduced sulfur gas emissions were measured along a salinity gradient in Louisiana Gulf Coast salt, brackish and freshwater marshes. Reduced sulfur gas emission was strongly associated with habitat and salinity gradient. The dominant emission component was dimethyl sulfide (average: 57·3 μg S m⁻² h⁻¹) in saltmarsh with considerable seasonal (max: 144·03 μg S m⁻² h⁻¹; min: 1·47 μg S m⁻² h⁻¹) and diurnal (max: 83·58 μg S m⁻² h⁻¹; min: 69·59 μg S m⁻² h⁻¹) changes in flux rates. Hydrogen sulfide was dominant (average: 21·2 μg S m⁻² h⁻¹, max: 79·2 μg S m⁻² h⁻¹; min: 5·29 μg S m⁻² h⁻¹) form in brackishmarsh and carbonyl sulfide (average: 1·09 μg S m⁻² h⁻¹; max: 3·42 μg S m⁻² h⁻¹; min: 0·32 μg S m⁻² h⁻¹) was dominant form in freshwater marsh. A greater amount of H₂S was evolved from brackishmarsh (21·22 μg S m⁻² h⁻¹) as compared to the saltmarsh (2·46 μg S m⁻² h⁻¹) and freshwater marsh (0·30 μg S m⁻² h⁻¹). Emission of total reduced sulfur gases decreased with decrease in salinity and distance inland from the coast. Emission of total reduced sulfur gases over the study averaged 73·3 μg S m⁻² h⁻¹ for the saltmarsh, 32·1 μg S m⁻² h⁻¹ for brackishmarsh and 2·76 μg S m⁻² h⁻¹ for the freshwater marsh.  相似文献   

甘肃敦煌小独山西钨矿床成矿流体特征及来源分析     

张鸣远  刘战庆  崔丰智  李瑞霜  席昊  陈玉峰  陶超群  岑炬标 《矿床地质》2022,41(3):611-622

甘肃敦煌小独山西石英脉型钨矿床位于北山成矿带柳园-俞井子裂谷带西段,经过详查和勘探工作,发现其资源量已达大型钨矿床规模。文章在野外详细观测和系统采样的基础上,对不同成矿阶段的样品使用岩相学、激光拉曼光谱、显微测温和碳、氢-氧同位素测试等方法,对矿脉中流体包裹体进行了综合研究。结果显示,该矿床矿脉中主要发育有气-液两相（Ⅰ型）和含液相CO₂三相（Ⅱ型） 2类包裹体。其中,Ⅰ阶段流体呈中高温、中盐度特征,主成矿（Ⅱ）阶段呈中高温、中低盐度特征,Ⅲ阶段呈低温,低盐度特征,均一温度与盐度呈现出正相关关系。包裹体的δD和δ¹⁸O值范围分别为-98.3‰~-76.4‰和0.8‰~5.4‰,呈岩浆水与大气降水相混合的特征;方解石中流体的δ¹³C值为-0.26‰~-0.73‰,δ¹⁸O值为-1.26‰~-3.73‰,显示C可能来源于海相碳酸盐岩,在后期演化过程中与大气降水发生了氧同位素交换作用。成矿早期与主成矿期均受到了大气降水的影响,该矿床发生了明显的流体混合作用是该地区成矿的主要因素。  相似文献   

“双碳”背景下石油地质学的理论创新与迈向能源发展多元化新时代     

李德生  李伯华 《地学前缘》2022,29(6):1-9

“双碳目标”已成为我国能源发展基本国策。如何开展这一大背景下的石油地质研究及如何推动能源多元化发展,是石油科技工作者面前的现实问题。本文对2000—2020年我国二氧化碳排放、油气能源消费、油气储量、产量等进行分析研究后认为,在“碳达峰”与“碳中和”应对全球气候变化的大背景之下,21世纪内石油和天然气仍将担任能源家族中的重要角色。我国石油工业要立足于理论和实践的自主创新,实现“万米级的超深层常规油气革命和纳米级超致密储层的非常规页岩油气革命”,实现超常规发展和低碳绿色转型发展。油田注水开发是我国提高采收率的核心技术,今后应大力推广注二氧化碳驱油技术,以达到增油与减排的双重目的,创新二氧化碳捕集与埋存技术以发展石油工业的减碳产业。21世纪为能源发展的多元化时代,水电、风能和太阳能等3类可再生能源开发利用是实现双碳目标的基本保障,地热能、生物质能和海洋能是重要推手;22世纪人类将建成一个由可再生能源和新能源保障的经济社会,氢能源将是未来最具发展潜力的新能源。  相似文献   

Characteristics of Hydrogen and Oxygen Isotopes and Noble Gas Isotopes in the Groundwater of Weishan, Wudalianchi, Northeast China     

WANG Shuai  HUANG Xuelian  QI Shihu  HAN Yongjie  KUANG Jian  WANG Siqi  WANG He  XIAO Zhicai 《《地质学报》英文版》2022,96(5):1729-1741

According to the hydrochemical characteristics, hydrogen and oxygen isotope characteristics and the ratio of noble gas isotopes of the sandstone aquifer and basalt aquifer, this study calculated the recharge temperature and residence time of groundwater in the Weishan area of Wudalianchi, also calculating the contribution of noble gas components from different sources to the samples. Based on the characteristics of hydrogen and oxygen isotopes and noble gases Xe and Ne, the recharge altitude and recharge temperature of the two aquifers were estimated, and the recharge temperature fitting with the NGT model as verified, the results showing that the main recharge altitude of groundwater in the region was 500–600 m, the recharge temperature being 2–7°C. Heeq and Heea of the samples have been simulated using the OD model, the content of radioactive 4He in the crust being obtained, the groundwater ages under the two conditions (closed condition and open condition) both being simulated. The results show that groundwater from the sandstone layer water is older than groundwater from the basalt layer. Hydrochemical characteristics and noble gas isotope ratios indicate that in the basalt aquifer and sandstone aquifer in the Weishan area, in addition to atmospheric and crustal helium, there is also an input of mantle-derived helium. The fault constitutes the uplift channel for groundwater containings mantle components, which results in the mantle source composition in water samples near the fault being much higher than those form non-fault areas.  相似文献