A series of Co3O4-CeO2 binary oxides with various Co/(Ce+Co)molar ratios were synthesized using a citric acid method,and their catalytic properties toward the total oxidation of propane were examined.The activities of...A series of Co3O4-CeO2 binary oxides with various Co/(Ce+Co)molar ratios were synthesized using a citric acid method,and their catalytic properties toward the total oxidation of propane were examined.The activities of the catalysts decrease in the order CoCeOx-70>CoCeOx-90>Co3O4>CoCeOx-50>CoCeOx-20>CeO2.CoCeOx-70(Co/(Ce+Co)=70% molar ratio)exhibits the highest catalytic activity toward the total oxidation of propane,of which the T90 is 310℃(GHSV=120000 mL h^-1 g^-1],which is 25℃ lower than that of pure Co3 O4.The enhancement of the catalytic performance of CoCeOx-70 is attributed to the strong interaction between CeO2 and Co3O4,the improvement of the low-temperature reducibility,and the increase in the number of active oxygen species.In-situ DRIFTS and reaction kinetics measurement reveal that Ce addition does not change the reaction mechanism,but promotes the adsorption and activation of propane on the catalyst surface.The addition of water vapor and CO2 in reactant gas has a negative effect on the propane conversion,and the catalyst is more sensitive to water vapor than to CO2.In addition,CoCeOx-70 exhibits excellent stability and reusability in water vapor and CO2 atmosphere.展开更多
The Central Asian Orogenic Belt,as one of world-class gold economic belts,preserves a number of giant,large black shale-hosted gold deposits,while it is still debated for origin of sulfides and gold mainly due to lack...The Central Asian Orogenic Belt,as one of world-class gold economic belts,preserves a number of giant,large black shale-hosted gold deposits,while it is still debated for origin of sulfides and gold mainly due to lack of identification for multiple stages of sulfides.The Haoyaoerhudong gold deposit is hosted in a sequence of Mesoproterozoic carbonaceous and pyritic slate,phyllite,and schist that form a tight syncline along the north margin of the North China Craton.Detailed petrography of the host rocks and mineralization have defined five stages of pyrites.The earliest form of pyrite(Py_(1))occurs as fine-grained dispersed pyrite in black carbonaceous slate and medium-to coarse-grained disseminated pyrite in pyrite-rich layers,contains relative low gold and high arsenic content,indicating a syn-sedimentary or diagenetic in origin.Stage Ⅱ pyrite(Py_(2))occurs with garnet and quartz inclusions and Py_(3) occurs as pyrite veins,contains higher gold and lower As content,and are interpreted to have formed from the dissolution-reprecipitation of Py_(1) during the peak metamorphism or post-peak metamorphism.Stage Ⅳ pyrite(Py_(4))from the pyrite-quartz veins crosscut the metamorphic garnet,contains the highest gold concentrations and other trace elements,and is considered to have formed post-peak metamorphism.Abundant native gold,electrum,and maldonite occur as inclusions within Py_(4) and monazite and in fractures that crosscut garnet.While,Py_(5) with typical remobilized feature is thought to be a product of melting of former pyrites(Py_(1) to Py_(4))triggered by the large-scale Hercynian magmatism.The sedimentary/diagenetic Py_(1) have δ^(34)S values that range from +12.4‰to +16.2‰.Later generations of sulfides,including Py_(2) to Py_(5),and Ccp_(2) to Ccp_(3),have δ^(34)S values from +9.5‰to +12.7‰.Monazite with maldonite inclusions from quartz-pyrite veins yielded an intercept age of 341.3±6.6 Ma,while coarse grained monazite associated biotite along fractures in the reefs yielded an intercept age of 254.6±8.2 Ma.The paragenetic,textural,chemical,and isotopic data suggest three distinct gold producing episodes at Haoyaoerhudong gold deposit.Gold and arsenic were clearly initially concentrated in organic muds,and enriched along the structures of diagenetic arsenic-rich pyrite.Subsequently,accompanying metamorphism and deformation,gold was liberated from the dissolution of diagenetic pyrites to form the pyrite veins.Finally,accompanying transformation of pyrite into pyrrhotite,gold was released into the metamorphic fluids to become concentrated as native gold,electrum,and maldonite in pyrite-quart veins.Monazite with age of 341 Ma from quartz-pyrite veins suggests that the third major gold mineralizing event in Haoyaoerhudong occurred before the Hercynian magmatism,suggesting that the Haoyaoerhudong deposit is a typical orogenic gold deposit rather than intrusion-related deposit.展开更多
Hydrogen evolution reaction(HER),zinc corrosion,and dendrites growth on zinc metal anode are the major issues limiting the practical applications of zinc-ion batteries.Herein,an in-situ physical/chemical cross-linked ...Hydrogen evolution reaction(HER),zinc corrosion,and dendrites growth on zinc metal anode are the major issues limiting the practical applications of zinc-ion batteries.Herein,an in-situ physical/chemical cross-linked hydrogel electrolyte(carrageenan/polyacrylamide/ZnSO_(4),denoted as CPZ)has been developed to stabilize the zinc anode-electrolyte interface,which can eliminate side reactions and prevent dendrites growth.The in-situ CPZ hydrogel electrolyte improves the reversibility of zinc anode due to eliminating side reactions caused by active water molecules.Furthermore,the electrostatic interaction between the SO_(4)^(-)groups in CPZ and Zn^(2+)can encourage the preferential deposition of zinc atoms on(002)crystal plane,which achieve dendrite-free and homogeneous zinc deposition.The in-situ hydrogel electrolyte offers a streamlined approach to battery manufacturing by allowing for direct integration into the battery.Subsequently,the Zn//Zn half battery with CPZ hydrogel electrolyte can enable an ultra-long cycle over 5500 h at a current density of 0.5 mA cm^(-2),and the Zn//Cu half battery reach an average coulombic efficiency of 99.37%.The Zn//V_(2)O_5-GO full battery with CPZ hydrogel electrolyte demonstrates94.5%of capacity retention after 2100 cycles.This study is expected to open new thought for the development of commercial hydrogel electrolytes for low-cost and long-life zinc-ion batteries.展开更多
Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was pr...Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate(PMMA)as a matrix and neopentyl glycol diacrylate(NPGDA)as cross-linking agent.The cross-linked structure of the GPE was preliminarily investigated,as well as the influence of the degree of cross-linking on its phys-ical properties.The GPE exhibited a superior conductivity of 1.391 mS cm^(-1) at 25℃.Herein,the Li|GPE|LiNi_(0.8) Co_(0.1) Mn_(0.1) O_(2) cell has an excellent capacity retention rate of 80.7%after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g^(-1).The structure of the cathode ma-terial is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.展开更多
Lithium-sulfur (Li-S) batteries are considered appealing power sources due to their high theoretical energy density (2600 Wh kg-1), low cost, and environmental friendliness. However, their widespread applicability is ...Lithium-sulfur (Li-S) batteries are considered appealing power sources due to their high theoretical energy density (2600 Wh kg-1), low cost, and environmental friendliness. However, their widespread applicability is restricted by two scientific problems: sluggish sulfur reaction kinetics and severe polysulfide shuttle effects. Multifarious strategies have been developed to overcome these two obstacles and achieve high sulfur utilization and capacity retention. Among these strategies, the introduction of catalytic materials into the Li-S battery system can greatly accelerate sulfur conversion and effectively inhibit the polysulfide shuttle effects. Herein, we have comprehensively reviewed the recent progress of catalytic engineering for polysulfide conversion in high-performance lithium-sulfur batteries. First, various catalytic materials serve as sulfur hosts, functionalized separators, and electrolyte additives;the mechanisms by which these materials promote the conversion of polysulfides in Li-S batteries have been systematically summarized. The relationship of structure, preparation, property, advantages, and limitations of these catalytic materials are comprehensively presented. Subsequently, the advanced characterization techniques of these catalytic processes are discussed, shedding light on the fundamental understanding of catalytic effects for improved electrochemical performance. Furthermore, future design tactics for high-performance Li-S batteries are discussed.展开更多
Porphyrinoid metal-organic frameworks(MOFs)with dual effective uranium uptake sites were synthesized through combined insitu and post-synthetic method.The MOF10@5 demonstrates the uptake amount of uranium reaches 1476...Porphyrinoid metal-organic frameworks(MOFs)with dual effective uranium uptake sites were synthesized through combined insitu and post-synthetic method.The MOF10@5 demonstrates the uptake amount of uranium reaches 1476 mg/g under visiblelight irradiation.The PN-MOF10@5 with dual uranyl uptake sites yields the amount of extracting uranyl of 1590 mg/g under visible-light irradiation.The density functional theory(DFT)calculations reveal strong interaction between uranyl and dual uranyl effective active sites.These MOFs demonstrate a powerful synthesis strategy for uranium extraction materials with dual effective active sites.展开更多
基金supported by the National Key R&D Program of China(2016YFB0600305)~~
文摘A series of Co3O4-CeO2 binary oxides with various Co/(Ce+Co)molar ratios were synthesized using a citric acid method,and their catalytic properties toward the total oxidation of propane were examined.The activities of the catalysts decrease in the order CoCeOx-70>CoCeOx-90>Co3O4>CoCeOx-50>CoCeOx-20>CeO2.CoCeOx-70(Co/(Ce+Co)=70% molar ratio)exhibits the highest catalytic activity toward the total oxidation of propane,of which the T90 is 310℃(GHSV=120000 mL h^-1 g^-1],which is 25℃ lower than that of pure Co3 O4.The enhancement of the catalytic performance of CoCeOx-70 is attributed to the strong interaction between CeO2 and Co3O4,the improvement of the low-temperature reducibility,and the increase in the number of active oxygen species.In-situ DRIFTS and reaction kinetics measurement reveal that Ce addition does not change the reaction mechanism,but promotes the adsorption and activation of propane on the catalyst surface.The addition of water vapor and CO2 in reactant gas has a negative effect on the propane conversion,and the catalyst is more sensitive to water vapor than to CO2.In addition,CoCeOx-70 exhibits excellent stability and reusability in water vapor and CO2 atmosphere.
基金the National Natural Science Foundation of China(Nos.41402042,41002064)Natural Sciences and Engineering Research Council of Canada Discovery Grant+1 种基金Fundamental Research Funds for the Central Universities(310827172006,300102278402)Geological Investigation Work Project of China Geological Survey(12120115069701).
文摘The Central Asian Orogenic Belt,as one of world-class gold economic belts,preserves a number of giant,large black shale-hosted gold deposits,while it is still debated for origin of sulfides and gold mainly due to lack of identification for multiple stages of sulfides.The Haoyaoerhudong gold deposit is hosted in a sequence of Mesoproterozoic carbonaceous and pyritic slate,phyllite,and schist that form a tight syncline along the north margin of the North China Craton.Detailed petrography of the host rocks and mineralization have defined five stages of pyrites.The earliest form of pyrite(Py_(1))occurs as fine-grained dispersed pyrite in black carbonaceous slate and medium-to coarse-grained disseminated pyrite in pyrite-rich layers,contains relative low gold and high arsenic content,indicating a syn-sedimentary or diagenetic in origin.Stage Ⅱ pyrite(Py_(2))occurs with garnet and quartz inclusions and Py_(3) occurs as pyrite veins,contains higher gold and lower As content,and are interpreted to have formed from the dissolution-reprecipitation of Py_(1) during the peak metamorphism or post-peak metamorphism.Stage Ⅳ pyrite(Py_(4))from the pyrite-quartz veins crosscut the metamorphic garnet,contains the highest gold concentrations and other trace elements,and is considered to have formed post-peak metamorphism.Abundant native gold,electrum,and maldonite occur as inclusions within Py_(4) and monazite and in fractures that crosscut garnet.While,Py_(5) with typical remobilized feature is thought to be a product of melting of former pyrites(Py_(1) to Py_(4))triggered by the large-scale Hercynian magmatism.The sedimentary/diagenetic Py_(1) have δ^(34)S values that range from +12.4‰to +16.2‰.Later generations of sulfides,including Py_(2) to Py_(5),and Ccp_(2) to Ccp_(3),have δ^(34)S values from +9.5‰to +12.7‰.Monazite with maldonite inclusions from quartz-pyrite veins yielded an intercept age of 341.3±6.6 Ma,while coarse grained monazite associated biotite along fractures in the reefs yielded an intercept age of 254.6±8.2 Ma.The paragenetic,textural,chemical,and isotopic data suggest three distinct gold producing episodes at Haoyaoerhudong gold deposit.Gold and arsenic were clearly initially concentrated in organic muds,and enriched along the structures of diagenetic arsenic-rich pyrite.Subsequently,accompanying metamorphism and deformation,gold was liberated from the dissolution of diagenetic pyrites to form the pyrite veins.Finally,accompanying transformation of pyrite into pyrrhotite,gold was released into the metamorphic fluids to become concentrated as native gold,electrum,and maldonite in pyrite-quart veins.Monazite with age of 341 Ma from quartz-pyrite veins suggests that the third major gold mineralizing event in Haoyaoerhudong occurred before the Hercynian magmatism,suggesting that the Haoyaoerhudong deposit is a typical orogenic gold deposit rather than intrusion-related deposit.
基金supported by the Key Program of Natural Science Foundation of Gansu Province (23JRRA789)the Major Science and Technology Project of Gansu Province (22ZD6GA008)。
文摘Hydrogen evolution reaction(HER),zinc corrosion,and dendrites growth on zinc metal anode are the major issues limiting the practical applications of zinc-ion batteries.Herein,an in-situ physical/chemical cross-linked hydrogel electrolyte(carrageenan/polyacrylamide/ZnSO_(4),denoted as CPZ)has been developed to stabilize the zinc anode-electrolyte interface,which can eliminate side reactions and prevent dendrites growth.The in-situ CPZ hydrogel electrolyte improves the reversibility of zinc anode due to eliminating side reactions caused by active water molecules.Furthermore,the electrostatic interaction between the SO_(4)^(-)groups in CPZ and Zn^(2+)can encourage the preferential deposition of zinc atoms on(002)crystal plane,which achieve dendrite-free and homogeneous zinc deposition.The in-situ hydrogel electrolyte offers a streamlined approach to battery manufacturing by allowing for direct integration into the battery.Subsequently,the Zn//Zn half battery with CPZ hydrogel electrolyte can enable an ultra-long cycle over 5500 h at a current density of 0.5 mA cm^(-2),and the Zn//Cu half battery reach an average coulombic efficiency of 99.37%.The Zn//V_(2)O_5-GO full battery with CPZ hydrogel electrolyte demonstrates94.5%of capacity retention after 2100 cycles.This study is expected to open new thought for the development of commercial hydrogel electrolytes for low-cost and long-life zinc-ion batteries.
基金supported by the National Natural Science Foundation of China(No.U22A20420)the Science and Technology Plan Project of Changzhou(No.CJ20235017)In addi-tion,the authors thank Jiangsu Development&Reform Commis-sion for their support.
文摘Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate(PMMA)as a matrix and neopentyl glycol diacrylate(NPGDA)as cross-linking agent.The cross-linked structure of the GPE was preliminarily investigated,as well as the influence of the degree of cross-linking on its phys-ical properties.The GPE exhibited a superior conductivity of 1.391 mS cm^(-1) at 25℃.Herein,the Li|GPE|LiNi_(0.8) Co_(0.1) Mn_(0.1) O_(2) cell has an excellent capacity retention rate of 80.7%after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g^(-1).The structure of the cathode ma-terial is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.
基金financially supported by National Natural Science Foundation of China(Nos.52164030 and 22179055)Natural Science Foundation of Jiangxi Province(Nos.20202ACBL204007 and 20224BAB204004)Program of Qingjiang Excellent Young Talents of Jiangxi University of Science and Technology(No.JXUSTQJYX2019010).
文摘Lithium-sulfur (Li-S) batteries are considered appealing power sources due to their high theoretical energy density (2600 Wh kg-1), low cost, and environmental friendliness. However, their widespread applicability is restricted by two scientific problems: sluggish sulfur reaction kinetics and severe polysulfide shuttle effects. Multifarious strategies have been developed to overcome these two obstacles and achieve high sulfur utilization and capacity retention. Among these strategies, the introduction of catalytic materials into the Li-S battery system can greatly accelerate sulfur conversion and effectively inhibit the polysulfide shuttle effects. Herein, we have comprehensively reviewed the recent progress of catalytic engineering for polysulfide conversion in high-performance lithium-sulfur batteries. First, various catalytic materials serve as sulfur hosts, functionalized separators, and electrolyte additives;the mechanisms by which these materials promote the conversion of polysulfides in Li-S batteries have been systematically summarized. The relationship of structure, preparation, property, advantages, and limitations of these catalytic materials are comprehensively presented. Subsequently, the advanced characterization techniques of these catalytic processes are discussed, shedding light on the fundamental understanding of catalytic effects for improved electrochemical performance. Furthermore, future design tactics for high-performance Li-S batteries are discussed.
基金supported by the National Natural Science Foundation of China(No.22301108)the Project Startup Foundation for Distinguished Scholars of Jiangsu University(No.4111310026).
文摘Porphyrinoid metal-organic frameworks(MOFs)with dual effective uranium uptake sites were synthesized through combined insitu and post-synthetic method.The MOF10@5 demonstrates the uptake amount of uranium reaches 1476 mg/g under visiblelight irradiation.The PN-MOF10@5 with dual uranyl uptake sites yields the amount of extracting uranyl of 1590 mg/g under visible-light irradiation.The density functional theory(DFT)calculations reveal strong interaction between uranyl and dual uranyl effective active sites.These MOFs demonstrate a powerful synthesis strategy for uranium extraction materials with dual effective active sites.
