At present, all hydrogen storage alloys are poisoned by hydrogen mixed with CO, CO2, etc, which decreases the hydrogen storage property sharply. Zr-Co based hydrogen storage alloys with good poisoning resistance were ...At present, all hydrogen storage alloys are poisoned by hydrogen mixed with CO, CO2, etc, which decreases the hydrogen storage property sharply. Zr-Co based hydrogen storage alloys with good poisoning resistance were prepared by alloying, fluorinating, and electroless plating. The experiment results show that the poisoning resistance of the Zr-Co based alloy was improved remarkably after the treatments. The poisoning resistance mechanism of the Zr-Co based hydrogen storage alloys was analyzed.展开更多
Developing non-precious metal catalysts to selectively reduce functionalized nitroarenes with high efficiency is urgently desirable for the production of value-added amines.Herein,we report a novel,efficient,anti-pois...Developing non-precious metal catalysts to selectively reduce functionalized nitroarenes with high efficiency is urgently desirable for the production of value-added amines.Herein,we report a novel,efficient,anti-poisoning single-atom cobalt catalyst(Co-NAC)for the highly selective hydrogenation of the nitro to amino group for nitroarenes baring various functional groups,including vinyl,cyano,and halogen.Using a combination of structure characterization techniques,we have confirmed that the cobalt species are predominantly present in the form of four-coordinated Co single sites anchored on nitrogen-assembly carbon(NAC)as the ordered mesoporous support.Co-NAC catalysts enable the full conversion and>99%selectivity with molecular H2 as a green reductant under mild conditions(80℃,2 MPa H2).As for the selective hydrogenation of 3-nitrostyrene,Co-NAC catalyst affords high catalytic productivity(19.7 h-1),which is superior to the cobalt nanoparticles(NPs)catalysts and most of the recently reported Co-based catalysts.This is attributed to the highly accessible atomically-dispersed Co active sites,the high surface area with ordered-mesoporous morphology and the prominent high content of nitrogen dopants.Notably,Co-NAC catalyst displays resistance towards sulfur-containing poisons(20 equivalents)and strong non-oxidizing acid(8 M),showing great potential for continuous application in the chemical industry.展开更多
The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive.In this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification ...The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive.In this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification catalyst was innovatively synthesized by electrostatic interaction.The Chlorella@Mn composite denitrification catalyst prepared under the optimal conditions(0.54 g/L Mn^(2+)concentration,20 million chlorellas/mL concentration,450℃ calcination temperature)exhibited a well-developed pore structure and large specific surface area(122 m^(2)/g).Compared with MnOx alone,the Chlorella@Mn composite catalyst achieved superior performance,with~100%NH_(3)selective catalytic reduction(NH_(3)-SCR)denitrification activity at 100-225℃.The results of NH_(3)temperature-programmed desorption(NH_(3)-TPD)and H_(2)temperature-programmed reduction(H_(2)-TPR)showed that the catalyst had strong acid sites and good redox properties.Zeta potential testing showed that the electronegativity of the chlorella cell surface could be used to enrich with Mn^(2+).X-ray photoelectron spectroscopy(XPS)confirmed that Chlorella@Mn had a high content of Mn^(3+)and surface chemisorbed oxygen.In-situ diffuse refectance infrared Fourier transform spectroscopy(in-situ DRIFTS)experimental results showed that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms play a role in the denitrification process on the surface of the Chlorella@Mn catalyst,where the main intermediate nitrate species is monodentate nitrite.The presence of SO_(2)promoted the generation and strengthening of Bronsted acid sites,but also generated more sulfate species on the surface,thereby reducing the denitrification activity of the Chlorella@Mn catalyst.The Chlorella@Mn composite catalyst had the characteristics of short preparation time,simple process and low cost,making it promising for industrial application.展开更多
文摘At present, all hydrogen storage alloys are poisoned by hydrogen mixed with CO, CO2, etc, which decreases the hydrogen storage property sharply. Zr-Co based hydrogen storage alloys with good poisoning resistance were prepared by alloying, fluorinating, and electroless plating. The experiment results show that the poisoning resistance of the Zr-Co based alloy was improved remarkably after the treatments. The poisoning resistance mechanism of the Zr-Co based hydrogen storage alloys was analyzed.
基金supported by the National Key R&D Program of China(No.2016YFA0202900)the National Natural Science Foundation of China(Nos.21878266,22078288,and 22108243)+4 种基金L.Q.and Y.T.L.were supported by the U.S.Department of Energy(DOE),Office of Basic Energy Sciences,Division of Chemical Sciences,Geosciences,and BiosciencesThe Ames Laboratory is operated for the U.S.DOE by Iowa State University under Contract No.DE-AC02-07CH11358W.Y.H.,J.Q.Y.,and X.W.thank the support from Iowa State University.F.D.L.thanks the Startup Fund from the University of Central Florida(UCF)S.H.X.thanks the support from the Preeminent Postdoctoral Program(P3)at UCFThis research used beamline 7-BM(QAS)of the National Synchrotron Light Source II,a U.S.Department of Energy(DOE)Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No.DE-SC0012704.
文摘Developing non-precious metal catalysts to selectively reduce functionalized nitroarenes with high efficiency is urgently desirable for the production of value-added amines.Herein,we report a novel,efficient,anti-poisoning single-atom cobalt catalyst(Co-NAC)for the highly selective hydrogenation of the nitro to amino group for nitroarenes baring various functional groups,including vinyl,cyano,and halogen.Using a combination of structure characterization techniques,we have confirmed that the cobalt species are predominantly present in the form of four-coordinated Co single sites anchored on nitrogen-assembly carbon(NAC)as the ordered mesoporous support.Co-NAC catalysts enable the full conversion and>99%selectivity with molecular H2 as a green reductant under mild conditions(80℃,2 MPa H2).As for the selective hydrogenation of 3-nitrostyrene,Co-NAC catalyst affords high catalytic productivity(19.7 h-1),which is superior to the cobalt nanoparticles(NPs)catalysts and most of the recently reported Co-based catalysts.This is attributed to the highly accessible atomically-dispersed Co active sites,the high surface area with ordered-mesoporous morphology and the prominent high content of nitrogen dopants.Notably,Co-NAC catalyst displays resistance towards sulfur-containing poisons(20 equivalents)and strong non-oxidizing acid(8 M),showing great potential for continuous application in the chemical industry.
基金supported by the National Natural Science Foundation of China (No.U20A20130)the Fundamental Research Funds for the Central Universities (No.FRF-TP-20-03B)。
文摘The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and expensive.In this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification catalyst was innovatively synthesized by electrostatic interaction.The Chlorella@Mn composite denitrification catalyst prepared under the optimal conditions(0.54 g/L Mn^(2+)concentration,20 million chlorellas/mL concentration,450℃ calcination temperature)exhibited a well-developed pore structure and large specific surface area(122 m^(2)/g).Compared with MnOx alone,the Chlorella@Mn composite catalyst achieved superior performance,with~100%NH_(3)selective catalytic reduction(NH_(3)-SCR)denitrification activity at 100-225℃.The results of NH_(3)temperature-programmed desorption(NH_(3)-TPD)and H_(2)temperature-programmed reduction(H_(2)-TPR)showed that the catalyst had strong acid sites and good redox properties.Zeta potential testing showed that the electronegativity of the chlorella cell surface could be used to enrich with Mn^(2+).X-ray photoelectron spectroscopy(XPS)confirmed that Chlorella@Mn had a high content of Mn^(3+)and surface chemisorbed oxygen.In-situ diffuse refectance infrared Fourier transform spectroscopy(in-situ DRIFTS)experimental results showed that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms play a role in the denitrification process on the surface of the Chlorella@Mn catalyst,where the main intermediate nitrate species is monodentate nitrite.The presence of SO_(2)promoted the generation and strengthening of Bronsted acid sites,but also generated more sulfate species on the surface,thereby reducing the denitrification activity of the Chlorella@Mn catalyst.The Chlorella@Mn composite catalyst had the characteristics of short preparation time,simple process and low cost,making it promising for industrial application.