Amorphous Ni-Ru-B/ZrO_2 catalyst was prepared by the means of chemical reduction,and selective CO methanation as a strategy for CO removal in fuel processing applications was investigated over the amorphous Ni-Ru-B/Zr...Amorphous Ni-Ru-B/ZrO_2 catalyst was prepared by the means of chemical reduction,and selective CO methanation as a strategy for CO removal in fuel processing applications was investigated over the amorphous Ni-Ru-B/ZrO_2 catalyst.The result showed that,at the temperature of 210-230℃,the catalyst was shown to be capable of reducing CO in a hydrogen-rich reformate to less than 10 ppm,while keeping the CO_2 conversion below 1.55%and the hydrogen consumption below 6.50%.展开更多
An ultrafine Ru-B amorphous alloy catalyst was prepared by chemical reduction with KBH4 in aqueous solution,which exhibited perfect selectivity to sorbitol(~100%)and very high activity during the liquid phase gluecose...An ultrafine Ru-B amorphous alloy catalyst was prepared by chemical reduction with KBH4 in aqueous solution,which exhibited perfect selectivity to sorbitol(~100%)and very high activity during the liquid phase gluecose hydrogenation,much higher than the corresponding crystallized Ru-B,the pure Ru powder,and Raney Ni catalysts.The correlation of the catalytic activity to both the structural and surface electronic characteristics was discussed bricfly.展开更多
Amorphous Ni-Ru-B/ZrO2 catalysts were prepared by chemical reduction method. The effects of Ni-Ru-B loading and Ru/Ni mole ratio on the catalytic performance for selective CO methanation from reformed fuel were studie...Amorphous Ni-Ru-B/ZrO2 catalysts were prepared by chemical reduction method. The effects of Ni-Ru-B loading and Ru/Ni mole ratio on the catalytic performance for selective CO methanation from reformed fuel were studied, and the catalysts were characterized by BET, ICP, XRD and TPD. The results showed that Ru strongly affected the catalytic activity and selectivity by increasing the thermal stability of amorphous structure, promoting the dispersion of the catalyst particle, and intensifying the CO adsorption. For the catalysts with Ru/Ni mole ratio under 0.15, the CO methanation conversion and selectivity increased significantly with the increasing Ru/Ni mole ratio. Among all the catalysts investigated, the 30 wt% Ni-Ru-B loading amorphous Ni61Ru9B30/ZrO2 catalyst with 0.15 Ru/Ni mole ratio presented the best catalytic performance,over which higher than 99.9%of CO conversion was obtained in the temperature range of 230℃~250℃,and the CO2 conversion was kept under the level of 0.9%.展开更多
Supported ionic liquid(IL) catalysts [C_nmim]_3PMo_(12)O_(40)/Am TiO_2(amorphous TiO_2) were synthesized through a one-step method for extraction coupled catalytic oxidative desulfurization(ECODS) system. Characteriza...Supported ionic liquid(IL) catalysts [C_nmim]_3PMo_(12)O_(40)/Am TiO_2(amorphous TiO_2) were synthesized through a one-step method for extraction coupled catalytic oxidative desulfurization(ECODS) system. Characterizations such as FTIR, DRS,wide-angle XRD, N_2 adsorption–desorption and XPS were applied to analyze the morphology and Keggin structure of the catalysts. In ECODS with hydrogen peroxide as the oxidant, it was found that ILs with longer alkyl chains in the cationic moiety had a better effect on the removal of dibenzothiophene. The desulfurization could reach 100% under optimal conditions, and GC–MS analysis was employed to detect the oxidized product after the reaction. Factors affecting the desulfurization efficiencies were discussed, and a possible mechanism was proposed. In addition, cyclic experiments were also conducted to investigate the recyclability of the supported catalyst. The catalytic activity of [C_(16)mim]_3 PMo_(12)O_(40)/Am TiO_2 only dropped from 100% to 92.9% after ten cycles, demonstrating the good recycling performance of the catalyst and its potential industrial application.展开更多
A supported Ni-B/TiO2 amorphous catalyst was prepared by impregnation and reduction. It was characterized by XRD, SAED, DSC, XPS, etc.. The catalytic activity of catalyst was measured through the hydrogenation of heav...A supported Ni-B/TiO2 amorphous catalyst was prepared by impregnation and reduction. It was characterized by XRD, SAED, DSC, XPS, etc.. The catalytic activity of catalyst was measured through the hydrogenation of heavy arenes in petrochemicals for the first time.展开更多
A novel Co-B amorphous alloy catalyst in the form of ultrafine particles was prepared by chemical reduction of CoCl2 with aqueous NaBH4, which exhibited excellent activity and selectivity during the hydrogenation of c...A novel Co-B amorphous alloy catalyst in the form of ultrafine particles was prepared by chemical reduction of CoCl2 with aqueous NaBH4, which exhibited excellent activity and selectivity during the hydrogenation of cinnamaldehyde to cinnamyl alcohol in liquid phase. The optimum yield of cinnamyl alcohol was 87.6%, much better than the yield of using Raney Ni, Raney Co and other Co-based catalysts.展开更多
The effect of La on the performance of a supported RuB amorphous alloy catalyst for benzene selective hydrogenation was studied by means of activity and selectivity tests, such as HRTEM, SAED, XPS, and XRD. The result...The effect of La on the performance of a supported RuB amorphous alloy catalyst for benzene selective hydrogenation was studied by means of activity and selectivity tests, such as HRTEM, SAED, XPS, and XRD. The results show that the addition of La to RuB amorphous alloy catalyst can evidently increase the activity and improve the thermal stability of RuB amorphous alloy to refrain its crystallization. The promoting effect of La on the activity of RuB amorphous alloy catalyst is because of the high dispersion of the active components.展开更多
Both the unsupported and supported NiB amorphous alloy catalysts (NiB and NiB/TiO2) were prepared by the chemical reduction method. Their catalytic activities were tested by the hydrogenation of sulfolene. The interac...Both the unsupported and supported NiB amorphous alloy catalysts (NiB and NiB/TiO2) were prepared by the chemical reduction method. Their catalytic activities were tested by the hydrogenation of sulfolene. The interactions between the NiB alloy and TiO2 were discussed for the first time by using XRD, ICP, SEM and TEM.展开更多
A new supported amorphous catalyst CoP/TiO2 was prepared by chemical reduction and characterized by ICP, XRD, TEM, BET and DSC. Its application in decomposing PH3 to high purity phosphor and its catalytic activity wer...A new supported amorphous catalyst CoP/TiO2 was prepared by chemical reduction and characterized by ICP, XRD, TEM, BET and DSC. Its application in decomposing PH3 to high purity phosphor and its catalytic activity were studied. The decomposition rate is over 95% at 450 ℃. For comparison, unsupported CoP amorphous catalyst was prepared by the same method. The result suggests that CoP/TiO2 exhibits higher thermal stability and catalytic activity than CoP, which is attributed to the high dispersion of CoP alloy particles on the support-TiO2.展开更多
A series of Ce-doped Ni-B amorphous alloy catalysts were prepared by a KBH4 reduction method, characterized by ICP, BET, XRD, H2-chemisorption, H2-TPD, etc., and tested in the hydrogenation of 2-ethylanthraquinone. Th...A series of Ce-doped Ni-B amorphous alloy catalysts were prepared by a KBH4 reduction method, characterized by ICP, BET, XRD, H2-chemisorption, H2-TPD, etc., and tested in the hydrogenation of 2-ethylanthraquinone. The results of characterization show that with the addition of Ce the amount of H2-chemisorption and H2-TPD areas first increases markedly and then decreases with the maximum appears at the atomic ratio of Ce to Ni of 0.036. The hydrogenation activity also shows the same trend. The effects of Ce are attributed to its dispersion of Ni particles, resulting in the formation of more surface Ni centers. However, much higher Ce contents may result in the decrease of the surface Ni contents. After heat treatment at higher temperatures, the amorphous structure of Ni-B is destroyed.展开更多
Uniform Ni-B amorphous alloys about 14 nm have been prepared on CNTs-A support, named Ni-B/CNTs-A. In comparison with the Ni-B/CNTs amorphous catalyst, Ni-B/CNTs-A showed higher nickel loading, determined by ICP and b...Uniform Ni-B amorphous alloys about 14 nm have been prepared on CNTs-A support, named Ni-B/CNTs-A. In comparison with the Ni-B/CNTs amorphous catalyst, Ni-B/CNTs-A showed higher nickel loading, determined by ICP and better catalytic activity and ethylene selectivity in the acetylene hydrogenation reaction.展开更多
Currently most of research efforts for selective electrocatalysis CO_(2) reduction to C2+products have relied on crystalline Cu-based catalysts;amorphous Cu with abundant low-coordinated atoms holds greater promise fo...Currently most of research efforts for selective electrocatalysis CO_(2) reduction to C2+products have relied on crystalline Cu-based catalysts;amorphous Cu with abundant low-coordinated atoms holds greater promise for this conversion yet remains relatively underexplored.Here we report an amorphous urchin-like Cu@nanosilica hybrid synthesized by electrostatic coupling Si polyanions with Cu salt in hydrothermal processes.The Cu@nanosilica electrocatalyst displays excellent CO_(2) electroreduction activity and selectivity with a Faradic efficiency of 70.5%for C2+product production,and higher stability compared to the crystalline Cu counterpart.The solar-driven CO_(2) electrolysis yields an energy efficiency of 20%for C2+product production.Mechanism study reveals that the urchin-like Cu@nanosilica catalyst with amorphous Cu/Cu^(+)dispersion enhances CO_(2) adsorption and activation to facilitate generation of CO_(2)^(-)*and possible CO^(*)intermediates,and suppresses hydrogen evolution concurrently.The combined effects of both aspects promote efficient C2+product production from CO_(2) electroreduction.展开更多
Electrochemical oxidation of small molecules(e.g.,water,urea,methanol,hydrazine,and glycerol)has gained growing scientific interest in the fields of electrochemical energy conversion/storage and environmental remediat...Electrochemical oxidation of small molecules(e.g.,water,urea,methanol,hydrazine,and glycerol)has gained growing scientific interest in the fields of electrochemical energy conversion/storage and environmental remediation.Designing cost-effective catalysts for the electrooxidation of small molecules(ESM)is thus crucial for improving reaction efficiency.Recently,earth-abundant amorphous transition metal(TM)-based nanomaterials have aroused souring interest owing to their earth-abundance,flexible structures,and excellent electrochemical activities.Hundreds of amorphous TM-based nanomaterials have been designed and used as promising ESM catalysts.Herein,recent advances in the design of amorphous TM-based ESM catalysts are comprehensively reviewed.The features(e.g.,large specific surface area,flexible electronic structure,and facile structure reconstruction)of amorphous TM-based ESM catalysts are first analyzed.Afterward,the design of various TM-based catalysts with advanced strategies(e.g.,nanostructure design,component regulation,heteroatom doping,and heterostructure construction)is fully scrutinized,and the catalysts’structure-performance correlation is emphasized.Future perspectives in the development of cost-effective amorphous TM-based catalysts are then outlined.This review is expected to provide practical strategies for the design of next-generation amorphous electrocatalysts.展开更多
基金supported by the National Natural Science Foundation of China(No.20576023)the Guangdong Province Natural Science Foundation(No.06025660).
文摘Amorphous Ni-Ru-B/ZrO_2 catalyst was prepared by the means of chemical reduction,and selective CO methanation as a strategy for CO removal in fuel processing applications was investigated over the amorphous Ni-Ru-B/ZrO_2 catalyst.The result showed that,at the temperature of 210-230℃,the catalyst was shown to be capable of reducing CO in a hydrogen-rich reformate to less than 10 ppm,while keeping the CO_2 conversion below 1.55%and the hydrogen consumption below 6.50%.
文摘An ultrafine Ru-B amorphous alloy catalyst was prepared by chemical reduction with KBH4 in aqueous solution,which exhibited perfect selectivity to sorbitol(~100%)and very high activity during the liquid phase gluecose hydrogenation,much higher than the corresponding crystallized Ru-B,the pure Ru powder,and Raney Ni catalysts.The correlation of the catalytic activity to both the structural and surface electronic characteristics was discussed bricfly.
基金supported by the National Natural Science Foundation of China (No: 20576023)the Guangdong Province Natural Science Foundation(No: 06025660)the Natural Science Foundation of Zhongkai University of Agriculture and Engineering (G3100026)
文摘Amorphous Ni-Ru-B/ZrO2 catalysts were prepared by chemical reduction method. The effects of Ni-Ru-B loading and Ru/Ni mole ratio on the catalytic performance for selective CO methanation from reformed fuel were studied, and the catalysts were characterized by BET, ICP, XRD and TPD. The results showed that Ru strongly affected the catalytic activity and selectivity by increasing the thermal stability of amorphous structure, promoting the dispersion of the catalyst particle, and intensifying the CO adsorption. For the catalysts with Ru/Ni mole ratio under 0.15, the CO methanation conversion and selectivity increased significantly with the increasing Ru/Ni mole ratio. Among all the catalysts investigated, the 30 wt% Ni-Ru-B loading amorphous Ni61Ru9B30/ZrO2 catalyst with 0.15 Ru/Ni mole ratio presented the best catalytic performance,over which higher than 99.9%of CO conversion was obtained in the temperature range of 230℃~250℃,and the CO2 conversion was kept under the level of 0.9%.
基金financially supported by the National Natural Science Foundation of China (Nos. 21576122, 21646001, 21506080)Natural Science Foundation of Jiangsu Province (Nos. BK20150485, BK20170528)+2 种基金China Postdoctoral Science Foundation (2017M611727)Jiangsu Planned Projects for Postdoctoral Research Funds (1701104B)supported by the Student Innovation and Entrepreneurship Training Program (201810299332 W)
文摘Supported ionic liquid(IL) catalysts [C_nmim]_3PMo_(12)O_(40)/Am TiO_2(amorphous TiO_2) were synthesized through a one-step method for extraction coupled catalytic oxidative desulfurization(ECODS) system. Characterizations such as FTIR, DRS,wide-angle XRD, N_2 adsorption–desorption and XPS were applied to analyze the morphology and Keggin structure of the catalysts. In ECODS with hydrogen peroxide as the oxidant, it was found that ILs with longer alkyl chains in the cationic moiety had a better effect on the removal of dibenzothiophene. The desulfurization could reach 100% under optimal conditions, and GC–MS analysis was employed to detect the oxidized product after the reaction. Factors affecting the desulfurization efficiencies were discussed, and a possible mechanism was proposed. In addition, cyclic experiments were also conducted to investigate the recyclability of the supported catalyst. The catalytic activity of [C_(16)mim]_3 PMo_(12)O_(40)/Am TiO_2 only dropped from 100% to 92.9% after ten cycles, demonstrating the good recycling performance of the catalyst and its potential industrial application.
基金the NNSFC, RFDP, NSFTC and NNSFCTJ for the financial support (20003006, 2000005520, 99380171 and 031606211).
文摘A supported Ni-B/TiO2 amorphous catalyst was prepared by impregnation and reduction. It was characterized by XRD, SAED, DSC, XPS, etc.. The catalytic activity of catalyst was measured through the hydrogenation of heavy arenes in petrochemicals for the first time.
基金This work was supported by the National Natural Science Foundation of China (29973025) and the Natural Science Foundation of Shanghai Science and Technology Committee (98QMA11402).
文摘A novel Co-B amorphous alloy catalyst in the form of ultrafine particles was prepared by chemical reduction of CoCl2 with aqueous NaBH4, which exhibited excellent activity and selectivity during the hydrogenation of cinnamaldehyde to cinnamyl alcohol in liquid phase. The optimum yield of cinnamyl alcohol was 87.6%, much better than the yield of using Raney Ni, Raney Co and other Co-based catalysts.
文摘The effect of La on the performance of a supported RuB amorphous alloy catalyst for benzene selective hydrogenation was studied by means of activity and selectivity tests, such as HRTEM, SAED, XPS, and XRD. The results show that the addition of La to RuB amorphous alloy catalyst can evidently increase the activity and improve the thermal stability of RuB amorphous alloy to refrain its crystallization. The promoting effect of La on the activity of RuB amorphous alloy catalyst is because of the high dispersion of the active components.
文摘Both the unsupported and supported NiB amorphous alloy catalysts (NiB and NiB/TiO2) were prepared by the chemical reduction method. Their catalytic activities were tested by the hydrogenation of sulfolene. The interactions between the NiB alloy and TiO2 were discussed for the first time by using XRD, ICP, SEM and TEM.
基金Natural Science Foundation of Tianjin(No.043801311)
文摘A new supported amorphous catalyst CoP/TiO2 was prepared by chemical reduction and characterized by ICP, XRD, TEM, BET and DSC. Its application in decomposing PH3 to high purity phosphor and its catalytic activity were studied. The decomposition rate is over 95% at 450 ℃. For comparison, unsupported CoP amorphous catalyst was prepared by the same method. The result suggests that CoP/TiO2 exhibits higher thermal stability and catalytic activity than CoP, which is attributed to the high dispersion of CoP alloy particles on the support-TiO2.
文摘A series of Ce-doped Ni-B amorphous alloy catalysts were prepared by a KBH4 reduction method, characterized by ICP, BET, XRD, H2-chemisorption, H2-TPD, etc., and tested in the hydrogenation of 2-ethylanthraquinone. The results of characterization show that with the addition of Ce the amount of H2-chemisorption and H2-TPD areas first increases markedly and then decreases with the maximum appears at the atomic ratio of Ce to Ni of 0.036. The hydrogenation activity also shows the same trend. The effects of Ce are attributed to its dispersion of Ni particles, resulting in the formation of more surface Ni centers. However, much higher Ce contents may result in the decrease of the surface Ni contents. After heat treatment at higher temperatures, the amorphous structure of Ni-B is destroyed.
基金The National Natural Science Foundation of China(No.20263003)supported this work.
文摘Uniform Ni-B amorphous alloys about 14 nm have been prepared on CNTs-A support, named Ni-B/CNTs-A. In comparison with the Ni-B/CNTs amorphous catalyst, Ni-B/CNTs-A showed higher nickel loading, determined by ICP and better catalytic activity and ethylene selectivity in the acetylene hydrogenation reaction.
基金supported by the National Natural Science Foundation of China(No.21872147 and 21805277)the Natural Science Foundation of Fujian Province(No.2018J05030 and 2019J05152)+2 种基金the Key Research Program of Frontier Sciences,CAS(No.ZDBSLY-SLH028)the DNL Cooperation Fund,CAS(DNL201924)the Strategic Priority Research Program,CAS(No.XDB20000000)。
文摘Currently most of research efforts for selective electrocatalysis CO_(2) reduction to C2+products have relied on crystalline Cu-based catalysts;amorphous Cu with abundant low-coordinated atoms holds greater promise for this conversion yet remains relatively underexplored.Here we report an amorphous urchin-like Cu@nanosilica hybrid synthesized by electrostatic coupling Si polyanions with Cu salt in hydrothermal processes.The Cu@nanosilica electrocatalyst displays excellent CO_(2) electroreduction activity and selectivity with a Faradic efficiency of 70.5%for C2+product production,and higher stability compared to the crystalline Cu counterpart.The solar-driven CO_(2) electrolysis yields an energy efficiency of 20%for C2+product production.Mechanism study reveals that the urchin-like Cu@nanosilica catalyst with amorphous Cu/Cu^(+)dispersion enhances CO_(2) adsorption and activation to facilitate generation of CO_(2)^(-)*and possible CO^(*)intermediates,and suppresses hydrogen evolution concurrently.The combined effects of both aspects promote efficient C2+product production from CO_(2) electroreduction.
基金Australian Research Council,Grant/Award Number:DP220101139。
文摘Electrochemical oxidation of small molecules(e.g.,water,urea,methanol,hydrazine,and glycerol)has gained growing scientific interest in the fields of electrochemical energy conversion/storage and environmental remediation.Designing cost-effective catalysts for the electrooxidation of small molecules(ESM)is thus crucial for improving reaction efficiency.Recently,earth-abundant amorphous transition metal(TM)-based nanomaterials have aroused souring interest owing to their earth-abundance,flexible structures,and excellent electrochemical activities.Hundreds of amorphous TM-based nanomaterials have been designed and used as promising ESM catalysts.Herein,recent advances in the design of amorphous TM-based ESM catalysts are comprehensively reviewed.The features(e.g.,large specific surface area,flexible electronic structure,and facile structure reconstruction)of amorphous TM-based ESM catalysts are first analyzed.Afterward,the design of various TM-based catalysts with advanced strategies(e.g.,nanostructure design,component regulation,heteroatom doping,and heterostructure construction)is fully scrutinized,and the catalysts’structure-performance correlation is emphasized.Future perspectives in the development of cost-effective amorphous TM-based catalysts are then outlined.This review is expected to provide practical strategies for the design of next-generation amorphous electrocatalysts.