以辉钼矿(MoS_(2))、褐铁矿和无烟煤为原料,通过碳热还原法制备了MoS_(x)@ZVI复合材料。研究了MoS_(2)用量、焙烧温度、无烟煤用量和焙烧时间对MoS_(x)@ZVI去除酸性橙G(OG)的影响,并确定了制备MoS_(x)@ZVI的较优制备条件为焙烧温度1000...以辉钼矿(MoS_(2))、褐铁矿和无烟煤为原料,通过碳热还原法制备了MoS_(x)@ZVI复合材料。研究了MoS_(2)用量、焙烧温度、无烟煤用量和焙烧时间对MoS_(x)@ZVI去除酸性橙G(OG)的影响,并确定了制备MoS_(x)@ZVI的较优制备条件为焙烧温度1000℃、MoS_(2)用量6%、焙烧时间60 min和无烟煤用量25%。通过X射线衍射、扫描电子显微镜和能谱仪对较优条件制备的MoS_(x)@ZVI进行表征,结果表明,材料中生成了大量核壳结构的硫化零价铁,内核为Fe-Mo-C合金,外壳可能由硫化钼、FeS、C、钼氧化物和铁氧化物组成。降解实验结果表明,将较优条件制备的MoS_(x)@ZVI碎磨至粒径<0.1 mm,用0.6 g MoS_(x)@ZVI处理400 mL 200 mg/L OG模拟废水,在初始pH=3.0~10.0范围处理150 min,OG的去除率均在90%以上。展开更多
The design of anode materials with a high specific capacity,high cyclic stability,and superior rate performance is required for the practical applications of sodium-ion batteries(SIBs).In this regard,we introduce in t...The design of anode materials with a high specific capacity,high cyclic stability,and superior rate performance is required for the practical applications of sodium-ion batteries(SIBs).In this regard,we introduce in this work a facile,low-cost and scalable method for the synthesis of nanocomposites of amorphous molybdenum sulfide(a-MoS_(x))and hierarchical porous carbon and have systematically investigated their performance for sodium ion storage.In the synthesis,ammonium molybdate tetrahydrate and thioacetamide are used as molybdenum and sulfur sources,respectively,with abundant corn starch as the carbon source and KOH as an activation agent.A simple pyrolysis of their mixtures leads to the formation of nanocomposites with a-MoS_(x)embedded within a hierarchical porous carbon(MoS_(x)@HPC),which are featured with a high surface area of up to 518.4 m^(2) g^(-1)and hierarchical pores ranging from micropores to macropores.It has also been shown that the annealing of MoS_(x)@HPC results in the formation of crystalline MoS_(2)nanosheets anchored in the hierarchical porous carbon matrix(MoS_(2)@HPC).The as-prepared nanocomposite MoS_(x)@HPC1 at an optimum carbon content of 32 wt%delivers a high specific sodium storage capacity of 599 mAh g^(-1)at 0.2 A g^(-1)and a high-rate performa nce with a retained capacity of 289 mAh g^(-1)at 5 A g^(-1).A comparison of the electrochemical performances of MoS_(x)@HPC and MoS_(2)@HPC demonstrates the superior specific capacity,rate performance,and charge transfer kinetics of the former,highlighting the unique advantageous role of amorphous MoS_(x)relative to crystalline MoS_(2).展开更多
Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))an...Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))and unraveling its structure−activity relationship.By leveraging transition molybdenum polysulfide clusters as functional units for multi-level ordering,we successfully designed and synthesized MoS_(x)nanowire networks derived from[Mo_(3)S_(13)]^(2−) clusters via evaporationinduced self-assembly,which exhibit enhanced HER activity attributed to a high density of active sites and dynamic evolution behavior under cathodic potentials.MoS_(x) nanowire networks electrode yields a current density of 100 mA·cm^(−2) at 142 mV in 0.5 M H_(2)SO_(4).This work provides an attractive prospect for optimizing catalysts at the sub-nano scale and offers insights into a strategy for designing catalysts in various gas evolution reactions.展开更多
Traditional bulk MoS_(2) as an effective H_(2)-evolution cocatalyst is mainly subjected to the weak hydrogen-adsorption ability of highporpotion saturated S,resulting in a slow interfacial H_(2)-evolution reaction.In ...Traditional bulk MoS_(2) as an effective H_(2)-evolution cocatalyst is mainly subjected to the weak hydrogen-adsorption ability of highporpotion saturated S,resulting in a slow interfacial H_(2)-evolution reaction.In this paper,an efficient strategy for enhancing hydrogen adsorption of saturated S by manipulating electron density through O atoms is proposed to boost photocatalytic performance of CdS.Simultaneously,amorphization of MoS_(2) can further increase the unsaturated active S sites.Herein,oxygencontained amorphous MoS_(x)(a-MoOS_(x))nanoparticles(10-30 nm)were tightly loaded on the CdS surface through a mild photoinduced deposition method by using(NH_(4))_(2)[MoO(S_(4))_(2)]solution as the precursor at room temperature.The photocatalytic H_(2)-evolution result showed that the a-MoOS_(x)/CdS performed the superior H_(2)-production activity(382μmol·h^(-1),apparent quantum efficiencies(AQE)=11.83%)with a lot of visual H_(2)bubbles,which was 54.6,2.5,and 5.1 times as high as that of CdS,MoS_(x)/CdS,and annealed a-MoOS_(x)/CdS,respectively.Characterizations and density functional theory(DFT)calculations revealed the mechanism of improved H_(2)-evolution activity is that the O heteroatom in amorphous MoOS_(x) can enhance the atomic H-adsorption ability by manipulating the electron density to form electron-deficient S^((2-δ)-)sites.This study provides a new idea to improve the efficiency and number of H_(2)-evolution active sites for developing efficient cocatalysts in the field of photocatalytic hydrogen evolution.展开更多
Aqueous zinc-ion batteries(ZIBs)have attracted increasing attention due to their low cost and high safety.MoS_(2) is a promising cathode material for aqueous ZIBs due to its favorable Zn^(2+)accommodation ability.Howe...Aqueous zinc-ion batteries(ZIBs)have attracted increasing attention due to their low cost and high safety.MoS_(2) is a promising cathode material for aqueous ZIBs due to its favorable Zn^(2+)accommodation ability.However,the structural strain and large volume changes during intercalation/deintercalation lead to exfoliation of active materials from substrate and cause irreversible capacity fading.In this work,a highly stable cathode was developed by designing a hierarchical carbon nanosheet-confined defective MoS_(x)material(CNS@MoS_(x)).This cathode material exhibits an excellent cycling stability with high capacity retention of 88.3%and~100%Coulombic efficiency after 400 cycles at 1.2 A·g^(-1),much superior compared to bare MoS_(2).Density functional theory(DFT)calculations combined with experiments illustrate that the promising electrochemical properties of CNS@MoS_(x)are due to the unique porous conductive structure of CNS with abundant active sites to anchor MoS_(x)via strong chemical bonding,enabling MoS_(x)to be firmly confined on the substrate.Moreover,this unique hierarchical complex structure ensures the fast migration of Zn^(2+)within MoS_(x)interlayer.展开更多
文摘以辉钼矿(MoS_(2))、褐铁矿和无烟煤为原料,通过碳热还原法制备了MoS_(x)@ZVI复合材料。研究了MoS_(2)用量、焙烧温度、无烟煤用量和焙烧时间对MoS_(x)@ZVI去除酸性橙G(OG)的影响,并确定了制备MoS_(x)@ZVI的较优制备条件为焙烧温度1000℃、MoS_(2)用量6%、焙烧时间60 min和无烟煤用量25%。通过X射线衍射、扫描电子显微镜和能谱仪对较优条件制备的MoS_(x)@ZVI进行表征,结果表明,材料中生成了大量核壳结构的硫化零价铁,内核为Fe-Mo-C合金,外壳可能由硫化钼、FeS、C、钼氧化物和铁氧化物组成。降解实验结果表明,将较优条件制备的MoS_(x)@ZVI碎磨至粒径<0.1 mm,用0.6 g MoS_(x)@ZVI处理400 mL 200 mg/L OG模拟废水,在初始pH=3.0~10.0范围处理150 min,OG的去除率均在90%以上。
基金financially supported by grants from the Natural Science and Engineering Research Council of Canada(Grant#RGPIN-2020-05546)。
文摘The design of anode materials with a high specific capacity,high cyclic stability,and superior rate performance is required for the practical applications of sodium-ion batteries(SIBs).In this regard,we introduce in this work a facile,low-cost and scalable method for the synthesis of nanocomposites of amorphous molybdenum sulfide(a-MoS_(x))and hierarchical porous carbon and have systematically investigated their performance for sodium ion storage.In the synthesis,ammonium molybdate tetrahydrate and thioacetamide are used as molybdenum and sulfur sources,respectively,with abundant corn starch as the carbon source and KOH as an activation agent.A simple pyrolysis of their mixtures leads to the formation of nanocomposites with a-MoS_(x)embedded within a hierarchical porous carbon(MoS_(x)@HPC),which are featured with a high surface area of up to 518.4 m^(2) g^(-1)and hierarchical pores ranging from micropores to macropores.It has also been shown that the annealing of MoS_(x)@HPC results in the formation of crystalline MoS_(2)nanosheets anchored in the hierarchical porous carbon matrix(MoS_(2)@HPC).The as-prepared nanocomposite MoS_(x)@HPC1 at an optimum carbon content of 32 wt%delivers a high specific sodium storage capacity of 599 mAh g^(-1)at 0.2 A g^(-1)and a high-rate performa nce with a retained capacity of 289 mAh g^(-1)at 5 A g^(-1).A comparison of the electrochemical performances of MoS_(x)@HPC and MoS_(2)@HPC demonstrates the superior specific capacity,rate performance,and charge transfer kinetics of the former,highlighting the unique advantageous role of amorphous MoS_(x)relative to crystalline MoS_(2).
基金supported by Innovation Support Programme(Soft Science Research)Project Achievements of Jiangsu Province(No.BK20231514)the National College Student Innovation and Entrepreneurship Training Program(NO.202310293173K).
文摘Precise design and synthesis of sub-nano scale catalysts with controllable electronic and geometric structures are pivotal for enhancing the hydrogen evolution reaction(HER)performance of molybdenum sulfide(MoS_(2))and unraveling its structure−activity relationship.By leveraging transition molybdenum polysulfide clusters as functional units for multi-level ordering,we successfully designed and synthesized MoS_(x)nanowire networks derived from[Mo_(3)S_(13)]^(2−) clusters via evaporationinduced self-assembly,which exhibit enhanced HER activity attributed to a high density of active sites and dynamic evolution behavior under cathodic potentials.MoS_(x) nanowire networks electrode yields a current density of 100 mA·cm^(−2) at 142 mV in 0.5 M H_(2)SO_(4).This work provides an attractive prospect for optimizing catalysts at the sub-nano scale and offers insights into a strategy for designing catalysts in various gas evolution reactions.
基金This work was supported by the National Natural Science Foundation of China(No.22178275)the Natural Science Foundation of Hubei Province of China(No.2022CFA001).
文摘Traditional bulk MoS_(2) as an effective H_(2)-evolution cocatalyst is mainly subjected to the weak hydrogen-adsorption ability of highporpotion saturated S,resulting in a slow interfacial H_(2)-evolution reaction.In this paper,an efficient strategy for enhancing hydrogen adsorption of saturated S by manipulating electron density through O atoms is proposed to boost photocatalytic performance of CdS.Simultaneously,amorphization of MoS_(2) can further increase the unsaturated active S sites.Herein,oxygencontained amorphous MoS_(x)(a-MoOS_(x))nanoparticles(10-30 nm)were tightly loaded on the CdS surface through a mild photoinduced deposition method by using(NH_(4))_(2)[MoO(S_(4))_(2)]solution as the precursor at room temperature.The photocatalytic H_(2)-evolution result showed that the a-MoOS_(x)/CdS performed the superior H_(2)-production activity(382μmol·h^(-1),apparent quantum efficiencies(AQE)=11.83%)with a lot of visual H_(2)bubbles,which was 54.6,2.5,and 5.1 times as high as that of CdS,MoS_(x)/CdS,and annealed a-MoOS_(x)/CdS,respectively.Characterizations and density functional theory(DFT)calculations revealed the mechanism of improved H_(2)-evolution activity is that the O heteroatom in amorphous MoOS_(x) can enhance the atomic H-adsorption ability by manipulating the electron density to form electron-deficient S^((2-δ)-)sites.This study provides a new idea to improve the efficiency and number of H_(2)-evolution active sites for developing efficient cocatalysts in the field of photocatalytic hydrogen evolution.
基金The authors acknowledge the financial support by the National Natural Science Foundation of China(Nos.21922501,21625102,and 21471018)the China National Petroleum Corporation Research Fund Program,and the Research Institute of Petroleum Exploration and Development Research Fund Program.
文摘Aqueous zinc-ion batteries(ZIBs)have attracted increasing attention due to their low cost and high safety.MoS_(2) is a promising cathode material for aqueous ZIBs due to its favorable Zn^(2+)accommodation ability.However,the structural strain and large volume changes during intercalation/deintercalation lead to exfoliation of active materials from substrate and cause irreversible capacity fading.In this work,a highly stable cathode was developed by designing a hierarchical carbon nanosheet-confined defective MoS_(x)material(CNS@MoS_(x)).This cathode material exhibits an excellent cycling stability with high capacity retention of 88.3%and~100%Coulombic efficiency after 400 cycles at 1.2 A·g^(-1),much superior compared to bare MoS_(2).Density functional theory(DFT)calculations combined with experiments illustrate that the promising electrochemical properties of CNS@MoS_(x)are due to the unique porous conductive structure of CNS with abundant active sites to anchor MoS_(x)via strong chemical bonding,enabling MoS_(x)to be firmly confined on the substrate.Moreover,this unique hierarchical complex structure ensures the fast migration of Zn^(2+)within MoS_(x)interlayer.
