Hydrogen will be at the basis of the World’s energy policy in forthcoming decades, owing to its decarbonized nature, at least when produced from renewables. For now, hydrogen is still essentially produced from fossil...Hydrogen will be at the basis of the World’s energy policy in forthcoming decades, owing to its decarbonized nature, at least when produced from renewables. For now, hydrogen is still essentially produced from fossil feedstock(and to a minor extent from biomass);in consequence the present hydrogen gas on the market is containing non-negligible amounts of impurities that prevent its immediate usage in specialty chemistry or as an energy carrier in fuel cells, e.g. in transportation applications(cars, buses, trains, boats, etc.) that gradually spread on the planet. For these purposes, hydrogen must be of sufficient purity but also sufficiently compressed(at high pressures, typically 70 MPa), rendering purification and compression steps unavoidable in the hydrogen cycle. As shown in the first part of this contribution "Electrochemical hydrogen compression and purification versus competing technologies: Part I. pros and cons", electrochemical hydrogen compressors(EHCs), which enable both hydrogen purification and compression, exhibit many theoretical(thermodynamic) and practical(kinetics) advantages over their mechanical counterparts. However, in order to be competitive, EHCs must operate in very intensive conditions(high current density and low cell voltage) that can only be reached if their core materials, e.g. the membrane and the electrodes/electrocatalysts, are optimized. This contribution will particularly focus on the properties electrocatalysts must exhibit to be used in EHCs: they shall promote(very) fast hydrogen oxidation reaction(HOR) in presence of impurities, which implies that they are(very) tolerant to poisons as well. This consists of a prerequisite for the operation of the anode of an EHC used for the purification-compression of hydrogen, and the materials developed for poison-tolerance in the vast literature on low-temperature fuel cells, may not always satisfy these two criteria, as this contribution will review.展开更多
Iodine-sulfur （IS） thermochemical water-splitting cycle is the most promising massive hydrogen production process. To avoid the undesirable side reactions between hydriodic acid（HI） and sulfuric acid （H2SO4）, it...Iodine-sulfur （IS） thermochemical water-splitting cycle is the most promising massive hydrogen production process. To avoid the undesirable side reactions between hydriodic acid（HI） and sulfuric acid （H2SO4）, it is necessary to purify the two phases formed by the Bunsen reaction. The purification process could be achieved by reverse reaction of the Bunsen reaction. In this study, the purification of the H2SO4 and HI Phases was studied. The purification proceeded in both batches and the continuous mode, the influences of operational parameters, including the reaction temperature, the flow rate of nitrogen gas, and the composition of the raw material solutions, on the purification effect, were investigated. Results showed that the purification of the H2SO4 phase was dominantly-affected by the reaction temperature, and iodine ion in the sulfuric acid phase could be removed completely when the temperature was above 130℃; although, the purification effect of the HI phase improved with increasing of both the flow rate of nitrogen gas and temperature.展开更多
The process of mechanically assisted hydriding and subsequent thermal dehydriding was proposed to produce nanocrystalline Mg and Mg alloy powders using pure Mg and Mg-5.5%Zn-0.6%Zr(mass fraction)(ZK60 Mg) alloy as the...The process of mechanically assisted hydriding and subsequent thermal dehydriding was proposed to produce nanocrystalline Mg and Mg alloy powders using pure Mg and Mg-5.5%Zn-0.6%Zr(mass fraction)(ZK60 Mg) alloy as the starting materal.The hydriding was achieved by room-temperature reaction milling in hydrogen.The dehydriding was carried out by vacuum annealing of the as-milled powders.The microstructure and morphology of both the as-milled and subsequently dehydrided powders were characterized by X-ray diffraction analysis(XRD) ,transmission electron microscopy(TEM) ,and scanning electron microscopy(SEM) ,respectively.The results show that,by reaction milling in hydrogen,both Mg and ZK60 Mg alloy can be fully hydrided to form nanocrystalline MgH2 with an average grain size of 10 nm.After subsequent thermal dehydriding at 300℃,the MgH2 can be turned into Mg again,and the newly formed Mg grains are nanocrystallines,with an average grain size of 25 nm.展开更多
Photocatalytic hydrogen(H_(2))production via water splitting in the absence of sacrificial agents is a promising strategy for producing clean and sustainable hydrogen energy from solar energy.However,the realization o...Photocatalytic hydrogen(H_(2))production via water splitting in the absence of sacrificial agents is a promising strategy for producing clean and sustainable hydrogen energy from solar energy.However,the realization of a photocatalytic pure water splitting system with desirable efficiency is still a huge challenge.Herein,visible light photocatalytic H_(2) production from pure water splitting was successfully achieved using a g-C_(3)N_(4)/CoTiO_(3) S-scheme heterojunction photocatalyst in the absence of sacrificial agents.An optimum hydrogen evolution rate of 118μmol∙h^(−1)∙g^(−1) was reached with the addition of 1.5 wt%CoTiO_(3).The remarkably promoted hydrogen evolution rate was attributed to the intensified light absorption coupled with the synergistic effect of visible light responsive CoTiO_(3),the promoted efficiency in charge separation,and the reserved strong redox capacity induced by the S-scheme charge transfer mechanism.This work provides an alternative to visible light-responding oxidation photocatalysts for the construction of S-scheme heterojunctions and high-efficiency photocatalytic systems for pure water splitting.展开更多
In the hydrogen network with the minimum hydrogen utility flow rate,the pinch appears at the point with zero hydrogen surplus,while the hydrogen surpluses of all the other points are positive.In the hydrogen purity pr...In the hydrogen network with the minimum hydrogen utility flow rate,the pinch appears at the point with zero hydrogen surplus,while the hydrogen surpluses of all the other points are positive.In the hydrogen purity profiles,the pinch can only lie at the sink-tie-line intersecting the source purity profile.According to the alternative distribution of the negative and positive regions,the effect of the purification to the hydrogen surplus is analyzed.The results show that when the purification is applied,the pinch point will appear neither above the purification feed nor between the initial pinch point and the purification feed,no matter the purification feed lies above or below the initial pinch point.This is validated by two case studies.展开更多
The analysis of the interaction of hydrogen, nitrogen （and their isotopes） with tungsten is important, since this material is a strong candidate to form the first wall of fusion reactors for both magnetic and inerti...The analysis of the interaction of hydrogen, nitrogen （and their isotopes） with tungsten is important, since this material is a strong candidate to form the first wall of fusion reactors for both magnetic and inertial confinement, and these atoms have a very sensitive （desired and unwanted） interaction with it. For this purpose, we study the effects and electronic state densities of atomic hydrogen and nitrogen in pure tungsten, in order to analyze some important properties such as the density of states of the system. Focusing on this application, this work is a preliminary study of the behavior of atoms of hydrogen and nitrogen, on a surface of tungsten on the three sites of the cell： top, hollow and bridge. We use a program simulation based on the DFT （density functional theory） implemented in the Open-Source Code Quantum Espresso, in order to obtain the adsorption energy and the density of states of the systems.展开更多
基金The authors thank the Auvergne Rhone-Alpes region for the funding of the PhD thesis of Marine TregaroPart of the work has been performed within the framework of the Centre of Excellence of Multifunctional Architectured Materials“CEMAM”no.ANR-10-LABX-44-01Both MT and MR make their PhD in the frame of the Eco-Sesa project,funded by IDEX Universite Grenoble Alpes.
文摘Hydrogen will be at the basis of the World’s energy policy in forthcoming decades, owing to its decarbonized nature, at least when produced from renewables. For now, hydrogen is still essentially produced from fossil feedstock(and to a minor extent from biomass);in consequence the present hydrogen gas on the market is containing non-negligible amounts of impurities that prevent its immediate usage in specialty chemistry or as an energy carrier in fuel cells, e.g. in transportation applications(cars, buses, trains, boats, etc.) that gradually spread on the planet. For these purposes, hydrogen must be of sufficient purity but also sufficiently compressed(at high pressures, typically 70 MPa), rendering purification and compression steps unavoidable in the hydrogen cycle. As shown in the first part of this contribution "Electrochemical hydrogen compression and purification versus competing technologies: Part I. pros and cons", electrochemical hydrogen compressors(EHCs), which enable both hydrogen purification and compression, exhibit many theoretical(thermodynamic) and practical(kinetics) advantages over their mechanical counterparts. However, in order to be competitive, EHCs must operate in very intensive conditions(high current density and low cell voltage) that can only be reached if their core materials, e.g. the membrane and the electrodes/electrocatalysts, are optimized. This contribution will particularly focus on the properties electrocatalysts must exhibit to be used in EHCs: they shall promote(very) fast hydrogen oxidation reaction(HOR) in presence of impurities, which implies that they are(very) tolerant to poisons as well. This consists of a prerequisite for the operation of the anode of an EHC used for the purification-compression of hydrogen, and the materials developed for poison-tolerance in the vast literature on low-temperature fuel cells, may not always satisfy these two criteria, as this contribution will review.
基金Supported by the National Defense Fundamental Research Fund (A1420080145)
文摘Iodine-sulfur （IS） thermochemical water-splitting cycle is the most promising massive hydrogen production process. To avoid the undesirable side reactions between hydriodic acid（HI） and sulfuric acid （H2SO4）, it is necessary to purify the two phases formed by the Bunsen reaction. The purification process could be achieved by reverse reaction of the Bunsen reaction. In this study, the purification of the H2SO4 and HI Phases was studied. The purification proceeded in both batches and the continuous mode, the influences of operational parameters, including the reaction temperature, the flow rate of nitrogen gas, and the composition of the raw material solutions, on the purification effect, were investigated. Results showed that the purification of the H2SO4 phase was dominantly-affected by the reaction temperature, and iodine ion in the sulfuric acid phase could be removed completely when the temperature was above 130℃; although, the purification effect of the HI phase improved with increasing of both the flow rate of nitrogen gas and temperature.
基金Project(50574034)supported by the National Natural Science Foundation of ChinaProject(20060213016)supported by Doctoral Education Fund of Ministry of Education of China
文摘The process of mechanically assisted hydriding and subsequent thermal dehydriding was proposed to produce nanocrystalline Mg and Mg alloy powders using pure Mg and Mg-5.5%Zn-0.6%Zr(mass fraction)(ZK60 Mg) alloy as the starting materal.The hydriding was achieved by room-temperature reaction milling in hydrogen.The dehydriding was carried out by vacuum annealing of the as-milled powders.The microstructure and morphology of both the as-milled and subsequently dehydrided powders were characterized by X-ray diffraction analysis(XRD) ,transmission electron microscopy(TEM) ,and scanning electron microscopy(SEM) ,respectively.The results show that,by reaction milling in hydrogen,both Mg and ZK60 Mg alloy can be fully hydrided to form nanocrystalline MgH2 with an average grain size of 10 nm.After subsequent thermal dehydriding at 300℃,the MgH2 can be turned into Mg again,and the newly formed Mg grains are nanocrystallines,with an average grain size of 25 nm.
文摘Photocatalytic hydrogen(H_(2))production via water splitting in the absence of sacrificial agents is a promising strategy for producing clean and sustainable hydrogen energy from solar energy.However,the realization of a photocatalytic pure water splitting system with desirable efficiency is still a huge challenge.Herein,visible light photocatalytic H_(2) production from pure water splitting was successfully achieved using a g-C_(3)N_(4)/CoTiO_(3) S-scheme heterojunction photocatalyst in the absence of sacrificial agents.An optimum hydrogen evolution rate of 118μmol∙h^(−1)∙g^(−1) was reached with the addition of 1.5 wt%CoTiO_(3).The remarkably promoted hydrogen evolution rate was attributed to the intensified light absorption coupled with the synergistic effect of visible light responsive CoTiO_(3),the promoted efficiency in charge separation,and the reserved strong redox capacity induced by the S-scheme charge transfer mechanism.This work provides an alternative to visible light-responding oxidation photocatalysts for the construction of S-scheme heterojunctions and high-efficiency photocatalytic systems for pure water splitting.
基金Supported by the State Key Development Program for Basic Research of China（2012CB720500） the National Natural Science Foundation of China（21276205,20936004） the State Key Laboratory of Heavy Oil Processing
文摘In the hydrogen network with the minimum hydrogen utility flow rate,the pinch appears at the point with zero hydrogen surplus,while the hydrogen surpluses of all the other points are positive.In the hydrogen purity profiles,the pinch can only lie at the sink-tie-line intersecting the source purity profile.According to the alternative distribution of the negative and positive regions,the effect of the purification to the hydrogen surplus is analyzed.The results show that when the purification is applied,the pinch point will appear neither above the purification feed nor between the initial pinch point and the purification feed,no matter the purification feed lies above or below the initial pinch point.This is validated by two case studies.
文摘The analysis of the interaction of hydrogen, nitrogen （and their isotopes） with tungsten is important, since this material is a strong candidate to form the first wall of fusion reactors for both magnetic and inertial confinement, and these atoms have a very sensitive （desired and unwanted） interaction with it. For this purpose, we study the effects and electronic state densities of atomic hydrogen and nitrogen in pure tungsten, in order to analyze some important properties such as the density of states of the system. Focusing on this application, this work is a preliminary study of the behavior of atoms of hydrogen and nitrogen, on a surface of tungsten on the three sites of the cell： top, hollow and bridge. We use a program simulation based on the DFT （density functional theory） implemented in the Open-Source Code Quantum Espresso, in order to obtain the adsorption energy and the density of states of the systems.
