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Development of Zr/ZrO_2 high temperature and high pressure sensors for in-situ measuring chemical parameters of deep-sea water

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Science China(Technological Sciences) 2009年第8期52卷 2466-2473页

作者： ZHANG XueTong, ZHANG RongHua, HU ShuMin & WANG Yong open research laboratory of geochemical kinetics, Institute of Mineral Resources, Chinese Academy of Geological Sciences, Beijing 100037, China open research laboratory of geochemical kinetics Institute of Mineral Resources Chinese Academy of Geological Sciences Beijing China

In order to in situ measure chemical parameters of deep-sea water and hydrothermal fluids at midocean ridge(MOR), it is necessary to use high temperature and high pressure chemical *** new sensors is essential to measure in-situ pH and other chemical parameters(dissolved H2, dissolved H2S) of deep-sea water and hydrothermal fluids in a wide temperature range(2℃―400℃) at MOR *** YSZ(Yttria Stabilized Zirconia, 9%Y2O3) ceramic-based(HgO/Hg) chemical sensors possess excellent electrochemical properties at high temperatures, which have been used to measure chemical parameters of hydrothermal fluids above 200℃.A novel Zr/ZrO2 oxidation/reduction electrode was constructed by oxidation of Zr wire in Na2CO3 *** Zr/ZrO2 electrode has good chemical stability while measuring pH of high-temperature aqueous solutions, combined with a Ag/AgCl reference *** of the Zr/ZrO2 sensor in association with a Ag/AgCl reference electrode vary linearly with pH over a wide pH range, as tested by various NaCl-HCl-H2O solutions(NaOH-NaCl-H2O for basic solutions), at temperatures in the range of 20℃―200℃.Thus, the Zr/ZrO2 sensors can be utilized in monitoring the fluids over the temperature range of 2℃―200℃.The Zr/ZrO2 electrode combined with Ag/AgCl, Ag/Ag2S, and Au electrodes has been used to measure pH and other chemical parameters(dissolved H2, dissolved H2S) of aqueous fluids from low to high temperatures and high pressures in the laboratory and to monitor those parameters of deep-sea water in South China Sea.

关键词： Zr/ZrO2 sensor melt oxidation method high temperature and high pressure chemical parameters investigation in the deep ocean

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Mineral Surface after Reaction with Aqueous Solution at High Temperatures and Pressures

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Acta Geologica Sinica(English Edition) 2000年第2期74卷 406-411页

作者： ZHANG Xuetong ZHANG Ronghua HU Shumin YU Wenbin open research laboratory of geochemical kinetics Chinese Academy of GeologicalSciences26 Baiwanzhuang RoadBeijing 100037

This work presents new experimental results on surface chemistry of reacting minerals and interface kinetics between mineral and aqueous solutions. These experiments were carried out using a flow reactor (packed bed reactor) of an open system as well as a continuous stirred tank reactor, CSTR. The authors measured reaction rates of such minerals as zeolite, albite and carbonate (rhodochrosite, dolomite) in various solutions, and tested corresponding mineral surface by using SEM, XPS, SIMS, etc. This paper mainly presents the experimental results of zeolite dissolution in water and in low pH solutions at room temperature, and dolomite dissolution at elevated temperatures. The results show that the release rates of Si, Al and Na of zeolite are different in most cases. The incongruent dissolution of zeolite is related to surface chemical modifications. The Na, Al and Si release rates for dissolution of albite and zeolite in water and various solutions were measured as a function of temperature, flow velocity, pH and solution composition in the reaction system. In most cases, dissolutions of both albite and zeolite are incongruent. Dissolution of dolomite is also incongruent in most cases and varied with T, pH, and nature of aqueous solutions. For dolomite dissolution, the release rates of Mg are less than those of Ca at high temperatures as T increases from 25 to 300°C. SIMS study indicates that the contents of Al, Na and Si in the leached layer of zeolite or albite surface, change with the distance from the surface, exhibiting a non-linear behaviour within a thickness range of 1000%. The distributions of Ca, Mg, Mn, H and Cl in the leached surface layer of carbonate have a non-linear behaviour too.

关键词： mineral surface kinetics liquid/solid interface reaction

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Experimental Study of the Distribution of Au and Cu in Aqueous Vapor Phase at High Temperatures and Its Role on Ore-forming Transportation

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Acta Geologica Sinica(English Edition) 2008年第4期82卷 875-883页

作者： ZHANG Ronghua HU Shumin ZHANG Xuetong open research laboratory of geochemical kinetics Institute of Mineral Resources Chinese Academy of Geological Sciences Beijing 100037

This study focuses on experiments of Au and Cu dissolved in vapor phase in hydrothermal fluids. Experiments prove that Au and Cu can re-distribute in vapor phase and liquid phase during separation of Au- and Cu-bearing supercritical fluids to vapor and liquid phases. These experimental results can illustrate some ore geneses, where boiling phenomena of ore fluids were found. Au- and Cubearing NaHCO3-HCl solutions were heated up to more than 350℃ in the main vessel, and then passed through a phase separator in a temperature range from 250℃ to 300℃, separated into vapor and liquid phases. We collected and analyzed the liquid and vapor samples separately, and found that Au and Cu dissolved and distributed in vapor phase. In some cases, the concentrations of Au and Cu in vapor are higher than those in liquid phase. Those experiments are used to interpret field observations of fluid inclusion data of some Au and Cu deposits, and demonstrate that some Au and Cu ore deposits are derived from metals transportation in vapor phase.

关键词： Au and Cu in vapor phase ore genesis boiling phenomena liquid and vapor phase separation metal transportation in gases

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kinetics of Hydrothermal Reactions of Minerals in Near-critical and Supercritical Water

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Acta Geologica Sinica(English Edition) 2000年第2期74卷 400-405页

作者： ZHANG Ronghua HU Shumin ZHANG Xuetong open research laboratory of geochemical kinetics Chinese Academyof Geological Sciences26 Baiwanzhuang RoadBeijing 100037

This work presents new experimental results on the kinetics of mineral dissolution in near-critical and supercritical water in a temperature range (T) from 25 to 400°C and a constant pressure of 23 MPa. Kinetic experiments were carried out by using a flow reactor (packed bed reactor) of an open system. The dissolution rates of albite and magnetite were measured under these experimental conditions. Na, Al and Si release rates for albite dissolution in water were measured as a function of the temperature and flow velocity in the reaction system. The maximum release rates of Na, Al and Si of albite dissolution in the hydrothermal flow systems under different flow velocities were always obtained at 300°C, that is to say, the maximum albite dissolution rates in the flow systems, regardless of different flow rates, were repeatedly measured at 300°C. Results indicate a wide fluctuation in albite dissolution rates occurring close to the critical point of water. The dissolution rates increased when the temperatures increased from 25 to 300°C and decreased when the temperatures increase from 300 to 400°C. At some flow velocities, the dissolution rates rose as the temperature surpassed 374°C. Albite dissolution was incongruent in water at most temperatures. It was only at 300°C that albite dissolution was congruent. The albite dissolution from 25 to 300°C (at 23 MPa) will change from incongruent to congruent, whereas from subcritical 300 to 400°C (at 23 MPa), the dissolution will change from congruent to incongruent. The release ratio of Al/Si (or Na/Si) is positive at T300°C. The dissolution rates of magnetite in water increased with increasing T until T at the critical point of water or around it. The authors believe that this is caused by the wide fluctuations in water properties under the conditions from the near-critical to supercritical state.

关键词： kinetics hydrothermal reaction critical state

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Hydrothermal Alteration Zoning and Kinetic Process of Mineral-Water Interactions

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Acta Geologica Sinica(English Edition) 2002年第3期76卷 351-366页

作者：张荣华胡书敏苏艳丰 open research laboratory of geochemical kinetics Institute of Mineral ResourcesChinese Academy of Geological Sciences 26 Baiwanzhuang Road Beijing 100037 China

This study reports the kinetic experimental results of albite in water and inKCl solution at 22 MPa in the temperature range of 25 to 400 deg C. Kinetic experiments have beencarried out in an open flow-through reaction system (packed bed reactor). Albite dissolution isalways incongruent in water at most temperatures, but becomes congruent at 300 deg C (close to thecritical point 374 deg C). At temperatures from 25 to 300 deg C, the incongruent dissolution ofalbite is reflected by the fact that sodium and aluminum are easily dissolved into water; from 300to 400 deg C it is reflected by silicon being more easily dissolved in water than Al and Na. Maximumalbite dissolution rates in the flow hydrothermal systems have been repeatedly observed at 300 degC, independent of flow rates. The kinetic experiments of albite dissolution in a KCl aqueoussolution (0.1 mol KCl) indicate that the dissolution rate of albite increases with increasingtemperature. Maximum silicon release rates of albite have been observed at 400 deg C, while maximumaluminum release rates of albite at 374 deg C. The reaction rates of albite also depend on thepotassium concentration in the aqueous solution. These results can be used to interpret themechanism for forming hydrothermal alteration. The kinetic experiments of mineral-aqueous solutionsinteractions in the hydrothermal system from 25 to 400 deg C and at 22 MPa indicate that theformation of the feldspar-mica-kaolinite zoning occurring in some ore deposits may depend not onlyon the mineral stability but also on the kinetics of feldspar hydration, which is affected by thewater property variation when crossing the critical point.

关键词： albite dissolution reaction rate incongruent dissolution criticalpoint

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Deep xenoliths in alkalic porphyry,liuhe,Yunnan,and implications to petrogenesis of alkalic porphyry and associated mineralizations

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Science China Earth Sciences 1999年第6期42卷 627-635页

作者：刘显凡战新志高振敏刘家军李朝阳苏文超 open laboratory of geochemical research Institute of Geochemistry Chinese Academy of Sciences

Na-rich microlite-glass is first discovered in deep-source xenoliths in alkali-rich porphyry, Liuhe village, Heqing County, Yunnan Province. It is shown that the ultramafic xenoliths originated from partial melting of primary mantle and the glass resulted from metasomatism between the xenoliths and mantle fluid derived from mantle degassing. Mantle metasomatism not only resulted in the enrichment of alkaline, large-ion elements, ore metals and volatiles but also created a favorable condition for the generation of alkaline magmas. The mantle xenoliths and their characteristics of mantle metasomatism provide important evidence for a better understanding of the petrogenesis and mineralization of the Cenozoic alkali-rich porphyry in western Yunnan.

关键词： deep xenoliths mantle metasomatism alkali-rich porphyry petrogenesis and mineralization.

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A Study of Near-and Super-Critical Fluids Using Diamond Anvil Cell and in-Situ FT-IR Spectroscopy

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Acta Geologica Sinica(English Edition) 2000年第2期74卷 412-417页

作者： HU Shumin ZHANG Ronghua ZHANG Xuetong open research Lab.of geochemical kinetics Chinese Academy of Geological Sciences26 Baiwanzhuang RoadBeijing100037

The phase relation and solution structure of water and NaCl aqueous solution have been observed and examined by using the hydrothermal diamond anvil cell (HDAC) at elevated temperatures and pressures and the in situ FT-IR spectroscopy. The temperature of observations ranges from 25 to 850°C and the pressure up to 10 or 30 kb. At first, we observed the phase transition process from halite+liquid+vapour (H+L+V) to L+H, then to L (or supercritical fluid, SCF), and another path: H+L+V→L+V→L (or SCF) in heating process. By means of the visual microscope, the authors found that in the L+V immiscibility field L+V exhibits an ordered structure, i.e. a large visual cluster of solvent around ions. The liquid phase is manifested by vapour bubbles. When phase transitions are observed, the authors examined their infrared spectra by using the FT-IR microscopy simultaneously. In the case of the phase transition from liquid (L) to liquid + vapor (L+V) immisciblity field of NaCl solutions, a sudden change (strong frequency shift) of infrared spectra of the aqueous solution is observed near the critical temperature of water as the temperature is raised from 25 to 650°C. The frequency of the maximum intensity of OH symmetric and asymmetric vibration varies with respect to temperature. The sharp peak of the OH stretching vibration of the maximum intensity appears in an interval from 300 to 400°C. It is indicated that the hydrogen bonding network is weakened and broken at last near the critical point of water, which causes the aqueous solution to become more associated. Besides, a pressure indicator (a mineral or compound) was introduced to the HDAC.

关键词： diamond anvil cell critical state in situ IR microscopy

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kinetics of ore-forming fluids in epithermal systems

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Chinese Science Bulletin 1999年第S2期44卷 5-6页

作者： ZHANG Ronghua, ZHANG Xuetong and HU Shumin open research laboratory of geochemical kinetics, Institute of Mineral Deposits, Chinese Academy of Geological Sciences, Beijing 100037, China open research laboratory of geochemical kinetics Institute of Mineral Deposits Chinese Academy of Geological Sciences Beijing 100037 China

As verified by the data of fluid inclusions in minerals in some paleo-hydrothermal systems, a lowering intemperature of the ore-forming fluids and a decrease in salinity occurred simultaneously from the centralzone （deep part） of the deposit profile to its outer zone （shallow part）. The usual situation shown byexperimental data is that solubility rises with an increase in temperature, as shown by quartz and manyore minerals. However, the solubility of some minerals increases as the temperature decreases within acertain temperature range. Therefore, continuous deposition cannot be achieved as the temperature of thesystem decreases, as in the cases of calcite, fluorite, and anhydrite. In water and NaCl-H2O systems,the solubility of calcite （or anhydrite） decreases with a rise in temperature at < 300℃ (or < 450℃

关键词： kinetics ore-forming fluids epithermal systems.

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Boosting bidirectional sulfur conversion enabled by introducing boron-doped atoms and phosphorus vacancies in Ni2P for lithium-sulfur batteries

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Journal of Energy Chemistry 2025年第1期100卷 760-769页

作者： Lin Peng Yu Bai Hang Li Meixiu Qu Zhenhua Wang Kening Sun Advanced research Institute of Multidisciplinary Science Beijing Institute of Technology Beijing Key laboratory of Chemical Power Source and Green Catalysis School of Chemistry and Chemical Engineering Beijing Institute of Technology

Lithium-sulfur （Li-S） batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox ***,we supply a strategy to optimize the electron structure of Ni2P by concurrently introducing B-doped atoms and P vacancies in Ni2P （Vp-B-Ni2P）,thereby enhancing the bidirectional sulfur *** study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni2P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides （LiPSs） as well as expediting the bidirectional conversion kinetics of sulfur ***,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni2P selectively promotes Li2S dissolution and nucleation ***,the Li-S batteries with Vp-B-Ni2P-separators present outstanding rate ability of 777 m A h g-1at 5 C and high areal capacity of 8.03 mA h cm-2under E/S of 5μL mg-1and sulfur loading of 7.20 mg *** work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.

关键词： Lithium sulfur batteries

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A surface engineering strategy for the stabilization of zinc metal anodes with montmorillonite layers toward long-life rechargeable aqueous zinc ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 94-105页

作者： Wenbo Wang Ruifeng Xu Xu Zhang Peiyu Wang Bao Yang Bingjun Yang Juan Yang Kailimai Su Pengjun Ma Yanan Deng Xianfeng Fan Wanjun Chen Key laboratory for Electronic Materials College of Electrical Engineering Northwest Minzu University Resource Chemistry and Energy Materials research Center State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Institute for Materials and Processes School of Engineering University of Edinburgh

Rechargeable aqueous zinc-ion batteries （AZIBs） exhibit appreciable potential in the domain of electrochemical energy ***,there are serious challenges for AZIBs,for instance zinc dendrite growth,hydrogen evolution reaction （HER）,and corrosion side ***,we propose a surface engineering modification strategy for coating the montmorillonite （MMT） layer onto the surface of the Zn anode to tackle these issues,thereby achieving high cycling stability for rechargeable *** results reveal that the MMT layer on the surface of the Zn anode is able to provide ordered zincophilic channels for zinc ions migration,facilitating the reaction kinetics of zinc *** functional theory（DFT） calculations and water contact angle （CA） tests prove that MMT@Zn anode exhibits superior adsorption capacity for Zn2+and better hydrophobicity than the bare Zn anode,thereby achieving excellent cycling ***,the MMT@Zn||MMT@Zn symmetric cell holds the stable cycling over 5600 h at 0.5 mA cm-2and 0.125 m A h cm-2,even exceeding 1800 h long cycling under harsh conditions of 5 m A cm-2and 1.25 m A h *** MMT@Zn||V2O5full cell reaches over 3000 cycles at 2 A g-1with excellent rate ***,this surface engineering modification strategy for enhancing the electrochemical performance of AZIBs represents a promising application.

关键词： Hydrogen evolution reaction

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