空心结构在能量转化和储存等重要应用方面,展现出了巨大的潜力.为了进一步提高性能,根据物质的组成和结构,合理设计出更复杂的空心结构材料是非常必要的,但目前仍然存在相当大的挑战.本文报导了一种以硅小球作为模板的高效方法,合成了...空心结构在能量转化和储存等重要应用方面,展现出了巨大的潜力.为了进一步提高性能,根据物质的组成和结构,合理设计出更复杂的空心结构材料是非常必要的,但目前仍然存在相当大的挑战.本文报导了一种以硅小球作为模板的高效方法,合成了新型的NiO@Co_3O_4空心多孔小球,其比表面积可达219.68 m2·g-1.NiO@Co_3O_4空心多孔小球的高比表面积有利于增强离子的扩散和提高活性物质的利用效率,并可防止纳米颗粒团聚.测试结果表明,在5 m V·s-1的扫描速度下,所制备的NiO@Co_3O_4空心多孔小球的比电容值达1140.9 F·g-1,同时具有良好的循环稳定性,显示出该材料在超级电容器领域有较好的应用前景.展开更多
Supported gold catalysts show high activity toward CO oxidation, and the nature of the support significantly affects the catalytic activity. Herein, serial Ni doping of thin porous Al2 O3 nanosheets was performed via ...Supported gold catalysts show high activity toward CO oxidation, and the nature of the support significantly affects the catalytic activity. Herein, serial Ni doping of thin porous Al2 O3 nanosheets was performed via a precipitation-hydrothermal method by varying the amount of Ni during the precipitation step. The prepared nanosheets were subsequently used as supports for the deposition of Au nanoparticles(NPs). The obtained Au/Nix Al catalysts were studied in the context of CO oxidation to determine the effect of Ni doping on the supports. Enhanced catalytic performances were obtained for the Au/Nix Al catalysts compared with those of the Au supported on bare Al2 O3. The Ni content and pretreatment atmosphere were both shown to influence the catalytic activity. Pretreatment under a reducing atmosphere was beneficial for improving catalytic activity. The highest activity was observed for the catalysts with a Ni/Al molar ratio of 0.05, achieving complete CO conversion at 20 °C with a gold loading of 1 wt%. The in-situ FTIR results showed that the introduction of Ni strengthened CO adsorption on the Au NPs. The H2-TPR and O2-TPD results indicated that the introduction of Ni produced new oxygen vacancies and allowed the oxygen molecules to be adsorbed and activated more easily. The improved catalytic performance after doping Ni was attributed to the smaller size of the Au NPs and more active oxygen species.展开更多
CO methanation on Ni/CeO2 has recently received increasing attention.However,the low-temperature activity and carbon resistance of Ni/CeO2 still need to be improved.In this study,plasma decomposition of nickel nitrate...CO methanation on Ni/CeO2 has recently received increasing attention.However,the low-temperature activity and carbon resistance of Ni/CeO2 still need to be improved.In this study,plasma decomposition of nickel nitrate was performed at ca.150℃ and atmospheric pressure.This was followed by hydrogen reduction at 500 ℃ in the absence of plasma,and a highly dispersed Ni/CeO2 catalyst was obtained with improved CO adsorption and enhanced metal-support interaction.The plasma-decomposed catalyst showed significantly improved low-temperature activity with high methane selectivity(up to 100%)and enhanced carbon resistance for CO methanation.For example,at 250 ℃,the plasma-decomposed catalyst showed a CO conversion of 96.8% with high methane selectivity(almost 100%),whereas the CO conversion was only 14.7% for a thermally decomposed catalyst.展开更多
Quasi-one-dimensional NiO with a hierarchically porous structure was synthesized through a facile coordination−precipitation method with the coupling effect of ammonia and a post-calcination treatment.The electrocatal...Quasi-one-dimensional NiO with a hierarchically porous structure was synthesized through a facile coordination−precipitation method with the coupling effect of ammonia and a post-calcination treatment.The electrocatalytic properties of NiO fibers for the oxidation of ethanol were compared with those of NiO spheres.The results show that the fibrous NiO possesses a larger specific surface area of 140.153 m2/g and a lower electrical resistivity of 4.5×105Ω·m,leading to an impressively superior electrocatalytic activity to spherical NiO for ethanol oxidation in alkaline media.The current decay on fibrous NiO at 0.6 V in 100−900 s was 0.00003%,which is much lower than that of spherical NiO,indicating its better stability.The unique morphology and hierarchically porous structure give the fibrous NiO great potential to be used as an anodic electrocatalyst for direct ethanol fuel cells.展开更多
Formation of volatile nickel carbonyls with CO in catalytic reaction is one of the mechanisms of catalyst deactivation. CO is one of the most popular probe molecules to study the surface properties in model catalysis....Formation of volatile nickel carbonyls with CO in catalytic reaction is one of the mechanisms of catalyst deactivation. CO is one of the most popular probe molecules to study the surface properties in model catalysis. Under ultra-high vacuum (UHV) conditions, the problem of nickel carbonyl impurity almost does not exist in the case that a high purity of CO is used directly. While in the near ambient pressure (NAP) range, nickel carbonyl is easily found on the surface by passing through the Ni containing tubes. Here, the NAP techniques such as NAP-X-ray photoelectron spectroscopy and NAP-scanning tunneling microscopy are used to study the adsorption of nickel carbonyl contaminated CO gas on Cu(111) surface in UHV and NAP conditions. By controlling the pressure of contaminated CO, the Ni-Cu bimetallic catalyst can form on Cu(111) surface. Furthermore, we investigate the process of CO adsorption and dissociation on the formed Ni-Cu bi-metal surface, and several high-pressure phases of CO structures are reported. This work contributes to understanding the interaction of nickel carbonyl with Cu(111) at room temperature, and reminds the consideration of CO molecules contaminated by nickel carbonyl especially in the NAP range study.展开更多
Direct N2O decomposition has been investigated over bare NiO and a series of its alkali-promoted catalysts. These catalysts were characterized by X-ray diffractometry, X-ray photoelectron spectroscopy (XPS) and fiel...Direct N2O decomposition has been investigated over bare NiO and a series of its alkali-promoted catalysts. These catalysts were characterized by X-ray diffractometry, X-ray photoelectron spectroscopy (XPS) and field emission scanning electron microscopy. XPS analysis revealed that surface nickel is present in three forms: metal particles, NiO and Ni(OH)2. It is suggested that nickel(0) valent atoms are essential for the interaction with N2O molecules at the catalyst surfaces. Bare NiO exhibited a very low N2O decomposition reactivity. However, the alkali-containing catalysts exhibited a marked activity enhancement.展开更多
Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) in alkaline medium are of significance f...Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) in alkaline medium are of significance for producing clean fuel to relieve energy and environment crisis.Here,a novel Ni/NiO monolithic electrode was developed by a facile and cost-effective acid promoted activation of Ni foam.After the treatment,this obtained monolithic electrode with a layer of NiO on its surface demonstrates rough and sheet-like morphology,which not only possesses larger accessible surface area but also provides more reactive active sites. Compared with powder catalysts,this monolithic electrode can achieve intimate contact between the electrocatalyst and the current collector,which will alleviate the problem of pulverization and enable the stable function of the electrode. It can be served as an efficient bi-functional electrocatalyst with an overpotential of 160 mV for HER and 290 mV for OER to produce current densities of 10 mA cm^(-2) in the alkaline medium. And it maintains benign stability after 5,000 cycles,which rivals many recent reported noble-metal free catalysts in 1.0mol L^(-1) KOH solution. Attributed to the easy,scalable methodology and high catalytic efficiency,this work not only offers a promising monolithic catalyst but also inspires us to exploit other inexpensive,highly efficient and self-standing noble metalfree electrocatalysts for scale-up electrochemical water-splitting technology.展开更多
基金supported by National Natural Science Foundation of China(No.51173212)National Basic Research Program of China(No.2015CB932304)+2 种基金Natural Science Foundation of Guangdong Province(No.S2013020012833)Project of High Level Talents in Higher School of Guangdong ProvinceScience and Technology Planning Project of Guangdong Province(No.2013B010403011)
文摘空心结构在能量转化和储存等重要应用方面,展现出了巨大的潜力.为了进一步提高性能,根据物质的组成和结构,合理设计出更复杂的空心结构材料是非常必要的,但目前仍然存在相当大的挑战.本文报导了一种以硅小球作为模板的高效方法,合成了新型的NiO@Co_3O_4空心多孔小球,其比表面积可达219.68 m2·g-1.NiO@Co_3O_4空心多孔小球的高比表面积有利于增强离子的扩散和提高活性物质的利用效率,并可防止纳米颗粒团聚.测试结果表明,在5 m V·s-1的扫描速度下,所制备的NiO@Co_3O_4空心多孔小球的比电容值达1140.9 F·g-1,同时具有良好的循环稳定性,显示出该材料在超级电容器领域有较好的应用前景.
文摘Supported gold catalysts show high activity toward CO oxidation, and the nature of the support significantly affects the catalytic activity. Herein, serial Ni doping of thin porous Al2 O3 nanosheets was performed via a precipitation-hydrothermal method by varying the amount of Ni during the precipitation step. The prepared nanosheets were subsequently used as supports for the deposition of Au nanoparticles(NPs). The obtained Au/Nix Al catalysts were studied in the context of CO oxidation to determine the effect of Ni doping on the supports. Enhanced catalytic performances were obtained for the Au/Nix Al catalysts compared with those of the Au supported on bare Al2 O3. The Ni content and pretreatment atmosphere were both shown to influence the catalytic activity. Pretreatment under a reducing atmosphere was beneficial for improving catalytic activity. The highest activity was observed for the catalysts with a Ni/Al molar ratio of 0.05, achieving complete CO conversion at 20 °C with a gold loading of 1 wt%. The in-situ FTIR results showed that the introduction of Ni strengthened CO adsorption on the Au NPs. The H2-TPR and O2-TPD results indicated that the introduction of Ni produced new oxygen vacancies and allowed the oxygen molecules to be adsorbed and activated more easily. The improved catalytic performance after doping Ni was attributed to the smaller size of the Au NPs and more active oxygen species.
基金This work was supported by the National Natural Science Foundation of China(21476157,21536008 and 21621004)the National Key R&D Program of China(2016YFB0600902)~~
文摘CO methanation on Ni/CeO2 has recently received increasing attention.However,the low-temperature activity and carbon resistance of Ni/CeO2 still need to be improved.In this study,plasma decomposition of nickel nitrate was performed at ca.150℃ and atmospheric pressure.This was followed by hydrogen reduction at 500 ℃ in the absence of plasma,and a highly dispersed Ni/CeO2 catalyst was obtained with improved CO adsorption and enhanced metal-support interaction.The plasma-decomposed catalyst showed significantly improved low-temperature activity with high methane selectivity(up to 100%)and enhanced carbon resistance for CO methanation.For example,at 250 ℃,the plasma-decomposed catalyst showed a CO conversion of 96.8% with high methane selectivity(almost 100%),whereas the CO conversion was only 14.7% for a thermally decomposed catalyst.
基金Project(51404306)supported by the National Natural Science Foundation of ChinaProject(JNJJ201613)supported by Jiana Foundation of Central South University,ChinaProject(2017YFC0210401)supported by the National Key Research and Development Program of China。
文摘Quasi-one-dimensional NiO with a hierarchically porous structure was synthesized through a facile coordination−precipitation method with the coupling effect of ammonia and a post-calcination treatment.The electrocatalytic properties of NiO fibers for the oxidation of ethanol were compared with those of NiO spheres.The results show that the fibrous NiO possesses a larger specific surface area of 140.153 m2/g and a lower electrical resistivity of 4.5×105Ω·m,leading to an impressively superior electrocatalytic activity to spherical NiO for ethanol oxidation in alkaline media.The current decay on fibrous NiO at 0.6 V in 100−900 s was 0.00003%,which is much lower than that of spherical NiO,indicating its better stability.The unique morphology and hierarchically porous structure give the fibrous NiO great potential to be used as an anodic electrocatalyst for direct ethanol fuel cells.
基金supported by the National Natural Science Foundation of China(No.91845109)Key Laboratory of Surface Physics and Chemistry Discipline Development Fund(XKFZ201711)
文摘Formation of volatile nickel carbonyls with CO in catalytic reaction is one of the mechanisms of catalyst deactivation. CO is one of the most popular probe molecules to study the surface properties in model catalysis. Under ultra-high vacuum (UHV) conditions, the problem of nickel carbonyl impurity almost does not exist in the case that a high purity of CO is used directly. While in the near ambient pressure (NAP) range, nickel carbonyl is easily found on the surface by passing through the Ni containing tubes. Here, the NAP techniques such as NAP-X-ray photoelectron spectroscopy and NAP-scanning tunneling microscopy are used to study the adsorption of nickel carbonyl contaminated CO gas on Cu(111) surface in UHV and NAP conditions. By controlling the pressure of contaminated CO, the Ni-Cu bimetallic catalyst can form on Cu(111) surface. Furthermore, we investigate the process of CO adsorption and dissociation on the formed Ni-Cu bi-metal surface, and several high-pressure phases of CO structures are reported. This work contributes to understanding the interaction of nickel carbonyl with Cu(111) at room temperature, and reminds the consideration of CO molecules contaminated by nickel carbonyl especially in the NAP range study.
文摘Direct N2O decomposition has been investigated over bare NiO and a series of its alkali-promoted catalysts. These catalysts were characterized by X-ray diffractometry, X-ray photoelectron spectroscopy (XPS) and field emission scanning electron microscopy. XPS analysis revealed that surface nickel is present in three forms: metal particles, NiO and Ni(OH)2. It is suggested that nickel(0) valent atoms are essential for the interaction with N2O molecules at the catalyst surfaces. Bare NiO exhibited a very low N2O decomposition reactivity. However, the alkali-containing catalysts exhibited a marked activity enhancement.
基金supported by the National Natural Science Foundation of China (21571073 and 21673090)the National Basic Research Program of China (2015CB932600)+2 种基金Hubei Provincial Natural Science Foundation of China (2016CFA031)the Program for HUST Interdisciplinary Innovation Team (2015ZDTD038)the Fundamental Research Funds for the Central Universities
文摘Exploring and designing bi-functional catalysts with earth-abundant elements that can work well for both hydrogen evolution reaction(HER) and oxygen evolution reaction(OER) in alkaline medium are of significance for producing clean fuel to relieve energy and environment crisis.Here,a novel Ni/NiO monolithic electrode was developed by a facile and cost-effective acid promoted activation of Ni foam.After the treatment,this obtained monolithic electrode with a layer of NiO on its surface demonstrates rough and sheet-like morphology,which not only possesses larger accessible surface area but also provides more reactive active sites. Compared with powder catalysts,this monolithic electrode can achieve intimate contact between the electrocatalyst and the current collector,which will alleviate the problem of pulverization and enable the stable function of the electrode. It can be served as an efficient bi-functional electrocatalyst with an overpotential of 160 mV for HER and 290 mV for OER to produce current densities of 10 mA cm^(-2) in the alkaline medium. And it maintains benign stability after 5,000 cycles,which rivals many recent reported noble-metal free catalysts in 1.0mol L^(-1) KOH solution. Attributed to the easy,scalable methodology and high catalytic efficiency,this work not only offers a promising monolithic catalyst but also inspires us to exploit other inexpensive,highly efficient and self-standing noble metalfree electrocatalysts for scale-up electrochemical water-splitting technology.