The solvent‐free oxidation of benzyl alcohol was studied using supported Pd‐Ni bimetallic nanoparticles.Compared with monometallic Pd,the addition of Ni to Pd was found to be effective in suppressing the nondesired ...The solvent‐free oxidation of benzyl alcohol was studied using supported Pd‐Ni bimetallic nanoparticles.Compared with monometallic Pd,the addition of Ni to Pd was found to be effective in suppressing the nondesired product toluene,thereby enhancing the selectivity towards benzaldehyde.This result was attributed to a dual effect of Ni addition:the weakening of dissociative adsorption of benzyl alcohol and the promotion of oxygen species involved in the oxidation pathway.展开更多
The development of cost-effective oxygen reduction reaction （ORR） catalysts with a high methanol tolerance and enhanced durability is highly desirable for direct methanol fuel cells. This work focuses on the convers...The development of cost-effective oxygen reduction reaction （ORR） catalysts with a high methanol tolerance and enhanced durability is highly desirable for direct methanol fuel cells. This work focuses on the conversion of PtNi nanoparticles from a disordered solid solution to an ordered intermetallic compound. Here the effect of this conversion on ORR activity, durability, and methanol tolerance are characterized. X-ray diffraction and transmission electron microscopy results confirm the formation of ordered PtNi intermetallic nanoparticles with high dispersion and a mean particle size of about 7.6 nm. The PtNi intermetallic nanoparticles exhibited enhanced mass and specific activities toward the methanol-tolerant ORR in pure and methanol-containing electrolytes. The specific activity of the ORR at 0.85 V on the PtNi intermetallic nanoparticles is almost 6 times greater than on commercial Pt/C and 3 times greater than on disordered PtNi alloy. Durability tests indicated a minimal loss of ORR activity for PtNi intermetallic nanoparticles after 5,000 potential cycles, whereas the ORR activity decreased by 28% for disordered PtNi alloy. The enhanced methanoltolerant ORR activity and durability may be attributed to the structural and compositional stabilities of the ordered PtNi intermetallic nanoparticles compared relative to the stabilities of the disordered PtNi alloy, strongly suggesting that the PtNi intermetallic nanoparticles may serve as highly active and durable methanol-tolerant ORR electrocatalysts for practical applications.展开更多
Ni@Pd core-shell nanoparticles with a mean particle size of 8–9 nm were prepared by solvothermal reduction of bivalent nickel and palladium in oleylamine and trioctylphosphine.Subsequently,the first-ever deposition o...Ni@Pd core-shell nanoparticles with a mean particle size of 8–9 nm were prepared by solvothermal reduction of bivalent nickel and palladium in oleylamine and trioctylphosphine.Subsequently,the first-ever deposition of Ni@Pd core-shell nanoparticles having different compositions on a metal-organic framework（MIL-101）was accomplished by wet impregnation in n-hexane.The Ni@Pd/MIL-101 materials were characterized by powder X-ray diffraction,Fourier transform infrared spectroscopy,transmission electron microscopy,and energy-dispersive X-ray spectroscopy and also investigated as catalysts for the hydrogenation of nitrobenzene under mild reaction conditions.At 30 °C and 0.1 MPa of H2 pressure,the Ni@Pd/MIL-101 gives a TOF as high as 375 h–1 for the hydrogenation of nitrobenzene and is applicable to a wide range of substituted nitroarenes.The exceptional performance of this catalyst is believed to result from the significant Ni-Pd interaction in the core-shell structure,together with promotion of the conversions of aromatics by uncoordinated Lewis acidic Cr sites on the MIL-101 support.展开更多
电催化二氧化碳(CO_(2))还原被认为是将CO_(2)转化为可再生能源产品的一种有前途的方法。开发性能优异的电催化剂高效完成这一重要反应是关键。镍基催化剂广泛应用于电催化CO_(2)还原研究,但是,镍纳米颗粒经常表现较差的催化性能。在本...电催化二氧化碳(CO_(2))还原被认为是将CO_(2)转化为可再生能源产品的一种有前途的方法。开发性能优异的电催化剂高效完成这一重要反应是关键。镍基催化剂广泛应用于电催化CO_(2)还原研究,但是,镍纳米颗粒经常表现较差的催化性能。在本文中,通过在氮气气氛中高温热解镍基金属有机骨架(MOF)、尿素和炭黑混合物,获得了镍纳米颗粒负载于多孔碳氮中的催化材料(NiNPs-NC)。有趣的是,NiNPs-NC在H型和流动相电池中都表现出优异的CO_(2)电还原性能。在H型电解池和-0.67–-1.07 V vs.RHE(可逆氢电极)电位窗口内,NiNPs-NC催化CO_(2)还原为CO的法拉第效率大于90%,其中,在-0.87 V vs.RHE时,CO的法拉第效率约为100%。在流动相电解池和-0.50–-0.70 V vs.RHE电位窗口内,NiNPs-NC催化CO_(2)还原为CO的选择性大于95%。电化学阻抗谱图和塔菲尔斜率表征显示,NiNPs-NC的高催化活性归因于其在催化过程中的快速电荷转移。本文提供了一种制备高效CO_(2)电还原催化剂的方法。展开更多
GaN-based light-emitting diodes （LEDs） with surface-textured indium tin oxide （ITO） as a transparent current spreading layer were fabricated. The ITO surface was textured by inductively coupled plasma （ICP） etch...GaN-based light-emitting diodes （LEDs） with surface-textured indium tin oxide （ITO） as a transparent current spreading layer were fabricated. The ITO surface was textured by inductively coupled plasma （ICP） etching technology using a monolayer of nickel （Ni） nanoparticles as the etching mask. The luminance intensity of ITO surface-textured GaN-based LEDs was enhanced by about 34% compared to that of conventional LED without textured ITO layer. In addition, the fabricated ITO surface-textured GaN-based LEDs would present a quite good performance in electrical characteristics. The results indicate that the scattering of photons emitted in the active layer was greatly enhanced via the textured ITO surface, and the ITO surface-textured technique could have a potential application in improving photoelectric characteristics for manufacturing GaN-based LEDs of higher brightness.展开更多
The application of nickel in electrocatalytic reduction of CO2 has been largely restricted by side reaction (hydrogen evolution reaction) and catalyst poisoning.Here we report a new strategy to improve the electrocata...The application of nickel in electrocatalytic reduction of CO2 has been largely restricted by side reaction (hydrogen evolution reaction) and catalyst poisoning.Here we report a new strategy to improve the electrocatalytic performance of nickel for CO2 reduction by employing a nitrogen-carbon layer for nickel nanoparticles.Such a nickel electrocatalyst exhibits high Faradaic efficiency 97.5% at relatively low potential of-0.61 V for the conversion of CO2 to CO.Density functional theory calculation reveals that it is thermodynamically accomplishable for the reduction product CO to be removed from the catalyst surface,thus avoiding catalyst poisoning.Also,the catalyst renders hydrogen evolution reaction to be suppressed and hence reasonably improves catalytic performance.展开更多
Multi-layered functionally graded(FG)structure Ni-W/Er2O3 nanocomposite films were prepared by continuously changing the deposition parameters,in which the Er2O3 and W contents varied with thickness.The microstructure...Multi-layered functionally graded(FG)structure Ni-W/Er2O3 nanocomposite films were prepared by continuously changing the deposition parameters,in which the Er2O3 and W contents varied with thickness.The microstructure and chemical composition of the electrodeposited Ni-W/Er2O3 films were determined by scanning electron microscopy(SEM)and energy-dispersive X-ray spectroscopy(EDS).The anti-corrosion and wear properties of the electrodeposition films were investigated by electrochemical measurement and ball-on-disk friction test.The microhardness distribution of the cross section of nanocomposites was measured by nanoindentation.The results showed that with decreasing agitation rate or increasing average current density,the contents of Er2O3 nanoparticles and tungsten were distributed in a gradient along the thickness,and the contents on the surface were larger.By comparison,FG Ni-W/Er2O3 films had better anti-corrosion and wear properties than the uniform Ni-W/Er2O3 films.Atomic force microscopy(AFM)and profilometry measurements indicated that Er2O3 nanoparticles had an effect on the surface roughness.展开更多
We demonstrate a femtosecond mode-locked erbium-doped fiber laser（EDFL） using a nickel oxide（Ni O） as a saturable absorber（SA）. Ni O nanoparticles are hosted into polyethylene oxide film and attached to fiber fe...We demonstrate a femtosecond mode-locked erbium-doped fiber laser（EDFL） using a nickel oxide（Ni O） as a saturable absorber（SA）. Ni O nanoparticles are hosted into polyethylene oxide film and attached to fiber ferrule in the laser cavity. The Ni O-SA shows a 39% modulation depth with a 0.04 MW∕cm^2 saturation intensity. Our ring laser cavity based on erbium-doped active fiber with managed intracavity dispersion has the ability to generate ultrashort pulses with a full width at half-maximum（FWHM） of around 2.85 nm centered at 1561.8 nm.The pulses repeat at a frequency of 0.96 MHz and duration of 950 fs.展开更多
Ni nanoparticles embedded in nitrogen-doped carbon（Ni@C-N） materials were prepared by ther-molysis of a Ni-containing metal-organic framework （Ni-MOF） under inert atmosphere. The as-synthesized Ni@C-N materials we...Ni nanoparticles embedded in nitrogen-doped carbon（Ni@C-N） materials were prepared by ther-molysis of a Ni-containing metal-organic framework （Ni-MOF） under inert atmosphere. The as-synthesized Ni@C-N materials were characterized by powder X-ray diffraction, N_2 adsorp-tion-desorption analysis, scanning electron microscopy, transmission electron microscopy, atomic absorption spectroscopy, and X-ray photoelectron spectroscopy. The MOF-derived Ni-based mate-rials were then examined as heterogeneous catalysts for the oxidation of alkanes under mild reac-tion conditions. The Ni@C-N composites displayed high activity and selectivity toward the oxidation of a variety of saturated C–H bonds, affording the corresponding oxidation products in good-to-excellent yields. Furthermore, the catalysts could be recycled and reused for at least four times without any significant loss in activity and selectivity under the investigated conditions.展开更多
Thermal stability has long been recognized as a major limitation for the application of ligand modification in high-temperature reactions. Herein, we demonstrate polymeric phosphate as an efficient and stable ligand t...Thermal stability has long been recognized as a major limitation for the application of ligand modification in high-temperature reactions. Herein, we demonstrate polymeric phosphate as an efficient and stable ligand to tune the selectivity of propane oxidative dehydrogenation. Beneficial from the weakened affinity of propene, NiO modified with polymeric phosphate shows a selectivity 2–3 times higher than NiO towards the production of propene. The success of this regulation verifies the feasibility of ligand modification in high-temperature gas-phase reactions and shines a light on its applications in other important industrial reactions.展开更多
基金supported by National Natural Science Foundation of China(21271153,21373181,21222307,U1402233)Major Research Plan of National Natural Science Foundation of China(91545113)the Fundamental Research Funds for the Central Universities(2014XZZX003-02)~~
文摘The solvent‐free oxidation of benzyl alcohol was studied using supported Pd‐Ni bimetallic nanoparticles.Compared with monometallic Pd,the addition of Ni to Pd was found to be effective in suppressing the nondesired product toluene,thereby enhancing the selectivity towards benzaldehyde.This result was attributed to a dual effect of Ni addition:the weakening of dissociative adsorption of benzyl alcohol and the promotion of oxygen species involved in the oxidation pathway.
文摘The development of cost-effective oxygen reduction reaction （ORR） catalysts with a high methanol tolerance and enhanced durability is highly desirable for direct methanol fuel cells. This work focuses on the conversion of PtNi nanoparticles from a disordered solid solution to an ordered intermetallic compound. Here the effect of this conversion on ORR activity, durability, and methanol tolerance are characterized. X-ray diffraction and transmission electron microscopy results confirm the formation of ordered PtNi intermetallic nanoparticles with high dispersion and a mean particle size of about 7.6 nm. The PtNi intermetallic nanoparticles exhibited enhanced mass and specific activities toward the methanol-tolerant ORR in pure and methanol-containing electrolytes. The specific activity of the ORR at 0.85 V on the PtNi intermetallic nanoparticles is almost 6 times greater than on commercial Pt/C and 3 times greater than on disordered PtNi alloy. Durability tests indicated a minimal loss of ORR activity for PtNi intermetallic nanoparticles after 5,000 potential cycles, whereas the ORR activity decreased by 28% for disordered PtNi alloy. The enhanced methanoltolerant ORR activity and durability may be attributed to the structural and compositional stabilities of the ordered PtNi intermetallic nanoparticles compared relative to the stabilities of the disordered PtNi alloy, strongly suggesting that the PtNi intermetallic nanoparticles may serve as highly active and durable methanol-tolerant ORR electrocatalysts for practical applications.
基金supported by the National Natural Science Foundation of China(21322606 and 21436005)the Specialized Research Fund for the Doctoral Program of Higher Education(20120172110012)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Natural Science Foundation of Guangdong Province(S2011020002397 and 2013B090500027)~~
文摘Ni@Pd core-shell nanoparticles with a mean particle size of 8–9 nm were prepared by solvothermal reduction of bivalent nickel and palladium in oleylamine and trioctylphosphine.Subsequently,the first-ever deposition of Ni@Pd core-shell nanoparticles having different compositions on a metal-organic framework（MIL-101）was accomplished by wet impregnation in n-hexane.The Ni@Pd/MIL-101 materials were characterized by powder X-ray diffraction,Fourier transform infrared spectroscopy,transmission electron microscopy,and energy-dispersive X-ray spectroscopy and also investigated as catalysts for the hydrogenation of nitrobenzene under mild reaction conditions.At 30 °C and 0.1 MPa of H2 pressure,the Ni@Pd/MIL-101 gives a TOF as high as 375 h–1 for the hydrogenation of nitrobenzene and is applicable to a wide range of substituted nitroarenes.The exceptional performance of this catalyst is believed to result from the significant Ni-Pd interaction in the core-shell structure,together with promotion of the conversions of aromatics by uncoordinated Lewis acidic Cr sites on the MIL-101 support.
文摘电催化二氧化碳(CO_(2))还原被认为是将CO_(2)转化为可再生能源产品的一种有前途的方法。开发性能优异的电催化剂高效完成这一重要反应是关键。镍基催化剂广泛应用于电催化CO_(2)还原研究,但是,镍纳米颗粒经常表现较差的催化性能。在本文中,通过在氮气气氛中高温热解镍基金属有机骨架(MOF)、尿素和炭黑混合物,获得了镍纳米颗粒负载于多孔碳氮中的催化材料(NiNPs-NC)。有趣的是,NiNPs-NC在H型和流动相电池中都表现出优异的CO_(2)电还原性能。在H型电解池和-0.67–-1.07 V vs.RHE(可逆氢电极)电位窗口内,NiNPs-NC催化CO_(2)还原为CO的法拉第效率大于90%,其中,在-0.87 V vs.RHE时,CO的法拉第效率约为100%。在流动相电解池和-0.50–-0.70 V vs.RHE电位窗口内,NiNPs-NC催化CO_(2)还原为CO的选择性大于95%。电化学阻抗谱图和塔菲尔斜率表征显示,NiNPs-NC的高催化活性归因于其在催化过程中的快速电荷转移。本文提供了一种制备高效CO_(2)电还原催化剂的方法。
基金Project supported by the Production and Research Program of Guangdong Province and Ministry of Education (Grant No.2009B090300338)Guangdong Natural Science Foundation of China (Grant No.8251063101000007)+1 种基金Guangdong Science and Technology Plan of China (Grant No.2008B010200004)the Student Research Project of South China Normal University (Grant No.09XXKC03)
文摘GaN-based light-emitting diodes （LEDs） with surface-textured indium tin oxide （ITO） as a transparent current spreading layer were fabricated. The ITO surface was textured by inductively coupled plasma （ICP） etching technology using a monolayer of nickel （Ni） nanoparticles as the etching mask. The luminance intensity of ITO surface-textured GaN-based LEDs was enhanced by about 34% compared to that of conventional LED without textured ITO layer. In addition, the fabricated ITO surface-textured GaN-based LEDs would present a quite good performance in electrical characteristics. The results indicate that the scattering of photons emitted in the active layer was greatly enhanced via the textured ITO surface, and the ITO surface-textured technique could have a potential application in improving photoelectric characteristics for manufacturing GaN-based LEDs of higher brightness.
基金the National Natural Science Foundation of China (Nos.21525316,21802146,and 21673254)Ministry of Science and Technology of China (No.2017YFA0403003)+1 种基金Chinese Academy of Sciences (No.QYZDY-SSW-SLH013)Beijing Municipal Science & Technology Commission (No.Z181100004218004).
文摘The application of nickel in electrocatalytic reduction of CO2 has been largely restricted by side reaction (hydrogen evolution reaction) and catalyst poisoning.Here we report a new strategy to improve the electrocatalytic performance of nickel for CO2 reduction by employing a nitrogen-carbon layer for nickel nanoparticles.Such a nickel electrocatalyst exhibits high Faradaic efficiency 97.5% at relatively low potential of-0.61 V for the conversion of CO2 to CO.Density functional theory calculation reveals that it is thermodynamically accomplishable for the reduction product CO to be removed from the catalyst surface,thus avoiding catalyst poisoning.Also,the catalyst renders hydrogen evolution reaction to be suppressed and hence reasonably improves catalytic performance.
基金the National Natural Science Foundation of China(Nos.51625504,51675421,51427805,51435002,91748209,51705406,and91748209)the Joint fund of the Ministry of Education of China(Nos.6141A0231 and 6141A0202)partially sponsored by National Key R&D Program of China(Nos.2016YFF0100700 and 2017YFF0204803)。
文摘Multi-layered functionally graded(FG)structure Ni-W/Er2O3 nanocomposite films were prepared by continuously changing the deposition parameters,in which the Er2O3 and W contents varied with thickness.The microstructure and chemical composition of the electrodeposited Ni-W/Er2O3 films were determined by scanning electron microscopy(SEM)and energy-dispersive X-ray spectroscopy(EDS).The anti-corrosion and wear properties of the electrodeposition films were investigated by electrochemical measurement and ball-on-disk friction test.The microhardness distribution of the cross section of nanocomposites was measured by nanoindentation.The results showed that with decreasing agitation rate or increasing average current density,the contents of Er2O3 nanoparticles and tungsten were distributed in a gradient along the thickness,and the contents on the surface were larger.By comparison,FG Ni-W/Er2O3 films had better anti-corrosion and wear properties than the uniform Ni-W/Er2O3 films.Atomic force microscopy(AFM)and profilometry measurements indicated that Er2O3 nanoparticles had an effect on the surface roughness.
文摘We demonstrate a femtosecond mode-locked erbium-doped fiber laser（EDFL） using a nickel oxide（Ni O） as a saturable absorber（SA）. Ni O nanoparticles are hosted into polyethylene oxide film and attached to fiber ferrule in the laser cavity. The Ni O-SA shows a 39% modulation depth with a 0.04 MW∕cm^2 saturation intensity. Our ring laser cavity based on erbium-doped active fiber with managed intracavity dispersion has the ability to generate ultrashort pulses with a full width at half-maximum（FWHM） of around 2.85 nm centered at 1561.8 nm.The pulses repeat at a frequency of 0.96 MHz and duration of 950 fs.
基金supported by the National Natural Science Foundation of China (21322606,21436005,21576095)the State Key Laboratory of Pulp and Paper Engineering (2015TS03)+2 种基金the Doctoral Fund of Ministry of Education of China (20120172110012)Fundamental Research Funds for the Central Universities (2015ZP002,2015PT004)Guangdong Natural Science Foundation (2013B090500027)
文摘Ni nanoparticles embedded in nitrogen-doped carbon（Ni@C-N） materials were prepared by ther-molysis of a Ni-containing metal-organic framework （Ni-MOF） under inert atmosphere. The as-synthesized Ni@C-N materials were characterized by powder X-ray diffraction, N_2 adsorp-tion-desorption analysis, scanning electron microscopy, transmission electron microscopy, atomic absorption spectroscopy, and X-ray photoelectron spectroscopy. The MOF-derived Ni-based mate-rials were then examined as heterogeneous catalysts for the oxidation of alkanes under mild reac-tion conditions. The Ni@C-N composites displayed high activity and selectivity toward the oxidation of a variety of saturated C–H bonds, affording the corresponding oxidation products in good-to-excellent yields. Furthermore, the catalysts could be recycled and reused for at least four times without any significant loss in activity and selectivity under the investigated conditions.
基金was supported by the National Natural Science Foundation of China(91545113,21703050)the China Postdoctoral Science Foundation(2017M610363,2018T110584)+2 种基金Shell Global Solutions International B.V.(PT71423,PT74557)the Fok Ying Tong Education Foundation(131015)the Science&Technology Program of Ningbo(2017C50014)~~
文摘Thermal stability has long been recognized as a major limitation for the application of ligand modification in high-temperature reactions. Herein, we demonstrate polymeric phosphate as an efficient and stable ligand to tune the selectivity of propane oxidative dehydrogenation. Beneficial from the weakened affinity of propene, NiO modified with polymeric phosphate shows a selectivity 2–3 times higher than NiO towards the production of propene. The success of this regulation verifies the feasibility of ligand modification in high-temperature gas-phase reactions and shines a light on its applications in other important industrial reactions.
