The performance of proton exchange membrane fuel cells is heavily dependent on the microstructure of electrode catalyst especially at low catalyst loadings.This work shows a hybrid electrocatalyst consisting of PtNi-W...The performance of proton exchange membrane fuel cells is heavily dependent on the microstructure of electrode catalyst especially at low catalyst loadings.This work shows a hybrid electrocatalyst consisting of PtNi-W alloy nanocrystals loaded on carbon surface with atomically dispersed W sites by a two-step straightforward method.Single-atomic W can be found on the carbon surface,which can form protonic acid sites and establish an extended proton transport network at the catalyst surface.When implemented in membrane electrode assembly as cathode at ultra-low loading of 0.05 mgPt cm^(−2),the peak power density of the cell is enhanced by 64.4%compared to that with the commercial Pt/C catalyst.The theoretical calculation suggests that the single-atomic W possesses a favorable energetics toward the formation of*OOH whereby the intermediates can be efficiently converted and further reduced to water,revealing a interfacial cascade catalysis facilitated by the single-atomic W.This work highlights a novel functional hybrid electrocatalyst design from the atomic level that enables to solve the bottle-neck issues at device level.展开更多
Voluminous platinum-group mineral （PGM） inclusions including erlichmanite （Os,Ru）S2, laurite （Ru,Os）S2, and irarsite （Ir, Os,Ru,Rh）AsS, as well as native osmium Os（Ir） and inclusions of base metal sulphides ...Voluminous platinum-group mineral （PGM） inclusions including erlichmanite （Os,Ru）S2, laurite （Ru,Os）S2, and irarsite （Ir, Os,Ru,Rh）AsS, as well as native osmium Os（Ir） and inclusions of base metal sulphides （BMS）, including millerite （NiS）, heazlewoodite （NiaS2）, covellite （CuS） and digenite （Cu3S2）, accompanied by native iron, have been identified in chromitites of the Zedang ophiolite, Tibet. The PGMs occur as both inclusions in magnesiochromite grains and as small interstitial granules between them; most are less than 10 ~m in size and vary in shape from euhedral to anhedral. They occur either as single or composite （biphase or polyphase） grains composed solely of PGM, or PGM associated with silicate grains. Os-, Ir-, and Ru-rich PGMs are the common species and Pt-, Pd-, and Rh-rich varieties have not been identified. Sulfur fugacity and temperature appear to be the main factors that controlled the PGE mineralogy during crystallization of the host chromitite in the upper mantle. If the activity of chalcogenides （such as S, and As） is low, PGE clusters will remain suspended in the silicate melt until they can coalesce to form alloys. Under appropriate conditions of fS2 and fO2, PGE alloys might react with the melt to form sulfides-sulfarsenides. Thus, we suggest that the Os, Ir and Ru metallic clusters and alloys in the Zedang chromitites crystallized first under high temperature and low fS2, followed by crystallization of sulphides of the laurite-erlichmanite, solid-solution series as the magma cooled and fS2 increased. The abundance of primary BMS in the chromitites suggests that fS2 reached relatively high values during the final stages of magnesiochromite crystallization. The diversity of the PGE minerals, in combination with differences in the petrological characteristics of the magnesiochromites, suggest different degrees of partial melting, perhaps at different depths in the mantle. The estimated parental magma composition suggests formation in a suprasubdu展开更多
Today more and more cars are produced every year. All of them have to be equipped with catalytic converters, the main role of which is to obtain substances harmless to the environment instead of exhausted gases. Catal...Today more and more cars are produced every year. All of them have to be equipped with catalytic converters, the main role of which is to obtain substances harmless to the environment instead of exhausted gases. Catalytic converters contain platinum group metals （PGM） especially platinum, palladium and rhodium. The price of these metals and their increasing demand are the reasons why today it is necessary to recycle used auto catalytic converters. There are many available methods of recovering PGM metals from them, especially platinum. These methods used mainly hydrometallurgical processes; however pyrometallurgical ones become more and more popular. The article presents results of the research mainly concerning pyrometallurgical processes. Two groups of research were carried out. In the first one different metals such as lead, magnesium and copper were used as a metal collector. During the tests, platinum went to those metals forming an alloy. In other research metal vapours were blown through catalytic converter carrier （grinded or whole）. In the tests metals such as calcium, magnesium, cadmium and zinc were applied. As a result white or grey powder （metal plus platinum） was obtained. The tables present results of the research. Processing parameters and conclusions are also shown. To compare efficiency of pyrometallurgical and hydrometallurgical methods catalytic converter carrier and samples of copper with platinum obtained from pyrometallurgical method were solved in aqua regia, mixture of aqua regia and fluoric acid.展开更多
基金Y.Li acknowledges the financial support from the National Natural Science Foundation of China(No.52171199)X.Ke acknowledges the financial support from the National Natural Science Foundation of China(No.12074017).
文摘The performance of proton exchange membrane fuel cells is heavily dependent on the microstructure of electrode catalyst especially at low catalyst loadings.This work shows a hybrid electrocatalyst consisting of PtNi-W alloy nanocrystals loaded on carbon surface with atomically dispersed W sites by a two-step straightforward method.Single-atomic W can be found on the carbon surface,which can form protonic acid sites and establish an extended proton transport network at the catalyst surface.When implemented in membrane electrode assembly as cathode at ultra-low loading of 0.05 mgPt cm^(−2),the peak power density of the cell is enhanced by 64.4%compared to that with the commercial Pt/C catalyst.The theoretical calculation suggests that the single-atomic W possesses a favorable energetics toward the formation of*OOH whereby the intermediates can be efficiently converted and further reduced to water,revealing a interfacial cascade catalysis facilitated by the single-atomic W.This work highlights a novel functional hybrid electrocatalyst design from the atomic level that enables to solve the bottle-neck issues at device level.
基金financially supported by the National Natural Science Foundation of China (Grant No.41262002,40930313,41302052,41502062)National Industry Special Projects (Sino Probe-05-02)+2 种基金China Bureau of Geological Survey Projects (DD20160023-01)IGCP-649Institute of Geology, Chinese Academy of Geological Science (J1526)
文摘Voluminous platinum-group mineral （PGM） inclusions including erlichmanite （Os,Ru）S2, laurite （Ru,Os）S2, and irarsite （Ir, Os,Ru,Rh）AsS, as well as native osmium Os（Ir） and inclusions of base metal sulphides （BMS）, including millerite （NiS）, heazlewoodite （NiaS2）, covellite （CuS） and digenite （Cu3S2）, accompanied by native iron, have been identified in chromitites of the Zedang ophiolite, Tibet. The PGMs occur as both inclusions in magnesiochromite grains and as small interstitial granules between them; most are less than 10 ~m in size and vary in shape from euhedral to anhedral. They occur either as single or composite （biphase or polyphase） grains composed solely of PGM, or PGM associated with silicate grains. Os-, Ir-, and Ru-rich PGMs are the common species and Pt-, Pd-, and Rh-rich varieties have not been identified. Sulfur fugacity and temperature appear to be the main factors that controlled the PGE mineralogy during crystallization of the host chromitite in the upper mantle. If the activity of chalcogenides （such as S, and As） is low, PGE clusters will remain suspended in the silicate melt until they can coalesce to form alloys. Under appropriate conditions of fS2 and fO2, PGE alloys might react with the melt to form sulfides-sulfarsenides. Thus, we suggest that the Os, Ir and Ru metallic clusters and alloys in the Zedang chromitites crystallized first under high temperature and low fS2, followed by crystallization of sulphides of the laurite-erlichmanite, solid-solution series as the magma cooled and fS2 increased. The abundance of primary BMS in the chromitites suggests that fS2 reached relatively high values during the final stages of magnesiochromite crystallization. The diversity of the PGE minerals, in combination with differences in the petrological characteristics of the magnesiochromites, suggest different degrees of partial melting, perhaps at different depths in the mantle. The estimated parental magma composition suggests formation in a suprasubdu
基金financially supported by Polish Ministry of Science and Higher Education (Contract No.NN508 381133 and No.NN508 625540)
文摘Today more and more cars are produced every year. All of them have to be equipped with catalytic converters, the main role of which is to obtain substances harmless to the environment instead of exhausted gases. Catalytic converters contain platinum group metals （PGM） especially platinum, palladium and rhodium. The price of these metals and their increasing demand are the reasons why today it is necessary to recycle used auto catalytic converters. There are many available methods of recovering PGM metals from them, especially platinum. These methods used mainly hydrometallurgical processes; however pyrometallurgical ones become more and more popular. The article presents results of the research mainly concerning pyrometallurgical processes. Two groups of research were carried out. In the first one different metals such as lead, magnesium and copper were used as a metal collector. During the tests, platinum went to those metals forming an alloy. In other research metal vapours were blown through catalytic converter carrier （grinded or whole）. In the tests metals such as calcium, magnesium, cadmium and zinc were applied. As a result white or grey powder （metal plus platinum） was obtained. The tables present results of the research. Processing parameters and conclusions are also shown. To compare efficiency of pyrometallurgical and hydrometallurgical methods catalytic converter carrier and samples of copper with platinum obtained from pyrometallurgical method were solved in aqua regia, mixture of aqua regia and fluoric acid.
