Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly protocol.The structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a...Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly protocol.The structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a set of characterizations,and its catalytic activity was investigated for hydrodesulfurization(HDS)of 4,6-dimethyldibenzothiophene.It has confirmed that the incorporation of La profoundly facilitate the generation of“Type II”NiMoS phase by weakening the interaction of Mo–O–Al leakage and promoting the sulfidation of both Ni and Mo oxides as well as changing the morphology of Ni promoted MoS2 slabs,thereafter boosting the HDS performance substantially.The finding here may contribute to the fundamental understanding of structure-activity in ultra-deep desulfurization and inspire the advancement of highly-efficient HDS catalyst in future.展开更多
NiMo-based nanostructures are among the most active hydrogen evolution reaction(HER)catalysts under an alkaline environment due to their strong water dissociation ability.However,these nanostructures are vulnerable to...NiMo-based nanostructures are among the most active hydrogen evolution reaction(HER)catalysts under an alkaline environment due to their strong water dissociation ability.However,these nanostructures are vulnerable to the destructive effects of H_(2) production,especially at industry-standard current densities.Therefore,developing a strategy to improve their mechanical strength while maintaining or even further increasing the activity of these nanocatalysts is of great interest to both the research and industrial communities.Here,a hierarchical interconnected NiMoN(HW-NiMoN-2h)with a nanorod-nanowire morphology was synthesized based on a rational combination of hydrothermal and water bath processes.HW-NiMoN-2h is found to exhibit excellent HER activity due to the accomodation of abundant active sites on its hierarchical morphology,in which nanowires con-nect free-standing nanorods,concurrently strengthening its structural stability to withstand H_(2) production at 1 A cm^(−2).Seawater is an attractive feedstock for water electrolysis since H_(2) generation and water desalination can be addressed simultaneously in a single process.The HER performance of HW-NiMoN-2h in alkaline seawater suggests that the presence of Na+ions interferes with the reation kinetics,thus lowering its activity slightly.However,benefiting from its hierarchical and interconnected characteristics,HW-NiMoN-2h is found to deliver outstanding HER activity of 1 A cm^(−2) at 130 mV overpotential and to exhibit excellent stability at 1 A cm^(−2) over 70 h in 1 M KOH seawater.展开更多
Exploring and designing a high-performance non-noble metal catalyst for hydrogen evolution reaction(HER)are crucial for the large-scale application of H2 by water electrolysis.Here,novel catalysts with NiMo nanopartic...Exploring and designing a high-performance non-noble metal catalyst for hydrogen evolution reaction(HER)are crucial for the large-scale application of H2 by water electrolysis.Here,novel catalysts with NiMo nanoparticles decorated on reduced graphene oxide(NiMo@r GO)synthesized by a two-step hydrothermal method were reported.Physical characterization results showed that the prepared NiMo@r GO-1 had an irregular lamellar structure,and the NiMo nanoparticles were uniformly dispersed on the rGO.NiMo@rGO-1 exhibited outstanding HER performance in an alkaline environment and required only 93 and 180 mV overpotential for HER in 1.0 M KOH solution to obtain current densities of-10 and-50 mA·cm^(-2),respectively.Stability tests showed that NiMo@rGO-1 had a certain operating stability for32 h.Under the same condition,the performance of NiMo@rGO-1 can be comparable with that of commercial Pt/C catalysts at high current density.The synergistic effect between NiMo particles and lamellate graphene can remarkably promote charge transfer in electrocatalytic reactions.As a result,NiMo@rGO-1 presented the advantages of high intrinsic activity,large specific surface area,and small electrical impedance.The lamellar graphene played a role in dispersion to prevent the aggregation of nanoparticles.The prepared NiMo@rGO-1 can be used in anion exchange membrane water electrolysis to produce hydrogen.This study provides a simple preparation method for efficient and low-cost water electrolysis to produce hydrogen in the future.展开更多
基金supported by the Introduction and Cultivation Plan of Young Innovative Talents in Colleges and Universities of Shandong Province, Chinathe Natural Science Foundation of Shandong Province, China (No. ZR2020ME052)+1 种基金the Natural Science Research Fund for Colleges and Universities in Anhui Province, China (No. KJ2021A0387)Independent Cultivation Program of Innovation Team of Jinan City, China (No. 2019GXRC011)。
基金financial support of the National Natural Science Foundation of China(22002050,22178154)the Project of Jiangsu University Senior Talents Foundation(20JDG35)+1 种基金Postdoctoral Science Foundation of China(2022T150765,2020M683154)National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2020B01).
文摘Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly protocol.The structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a set of characterizations,and its catalytic activity was investigated for hydrodesulfurization(HDS)of 4,6-dimethyldibenzothiophene.It has confirmed that the incorporation of La profoundly facilitate the generation of“Type II”NiMoS phase by weakening the interaction of Mo–O–Al leakage and promoting the sulfidation of both Ni and Mo oxides as well as changing the morphology of Ni promoted MoS2 slabs,thereafter boosting the HDS performance substantially.The finding here may contribute to the fundamental understanding of structure-activity in ultra-deep desulfurization and inspire the advancement of highly-efficient HDS catalyst in future.
基金Element Resources,LLC,and Shell through UHETI,funded part of this work
文摘NiMo-based nanostructures are among the most active hydrogen evolution reaction(HER)catalysts under an alkaline environment due to their strong water dissociation ability.However,these nanostructures are vulnerable to the destructive effects of H_(2) production,especially at industry-standard current densities.Therefore,developing a strategy to improve their mechanical strength while maintaining or even further increasing the activity of these nanocatalysts is of great interest to both the research and industrial communities.Here,a hierarchical interconnected NiMoN(HW-NiMoN-2h)with a nanorod-nanowire morphology was synthesized based on a rational combination of hydrothermal and water bath processes.HW-NiMoN-2h is found to exhibit excellent HER activity due to the accomodation of abundant active sites on its hierarchical morphology,in which nanowires con-nect free-standing nanorods,concurrently strengthening its structural stability to withstand H_(2) production at 1 A cm^(−2).Seawater is an attractive feedstock for water electrolysis since H_(2) generation and water desalination can be addressed simultaneously in a single process.The HER performance of HW-NiMoN-2h in alkaline seawater suggests that the presence of Na+ions interferes with the reation kinetics,thus lowering its activity slightly.However,benefiting from its hierarchical and interconnected characteristics,HW-NiMoN-2h is found to deliver outstanding HER activity of 1 A cm^(−2) at 130 mV overpotential and to exhibit excellent stability at 1 A cm^(−2) over 70 h in 1 M KOH seawater.
基金financially supported by the National Natural Science Foundation of China(No.22278125)。
文摘Exploring and designing a high-performance non-noble metal catalyst for hydrogen evolution reaction(HER)are crucial for the large-scale application of H2 by water electrolysis.Here,novel catalysts with NiMo nanoparticles decorated on reduced graphene oxide(NiMo@r GO)synthesized by a two-step hydrothermal method were reported.Physical characterization results showed that the prepared NiMo@r GO-1 had an irregular lamellar structure,and the NiMo nanoparticles were uniformly dispersed on the rGO.NiMo@rGO-1 exhibited outstanding HER performance in an alkaline environment and required only 93 and 180 mV overpotential for HER in 1.0 M KOH solution to obtain current densities of-10 and-50 mA·cm^(-2),respectively.Stability tests showed that NiMo@rGO-1 had a certain operating stability for32 h.Under the same condition,the performance of NiMo@rGO-1 can be comparable with that of commercial Pt/C catalysts at high current density.The synergistic effect between NiMo particles and lamellate graphene can remarkably promote charge transfer in electrocatalytic reactions.As a result,NiMo@rGO-1 presented the advantages of high intrinsic activity,large specific surface area,and small electrical impedance.The lamellar graphene played a role in dispersion to prevent the aggregation of nanoparticles.The prepared NiMo@rGO-1 can be used in anion exchange membrane water electrolysis to produce hydrogen.This study provides a simple preparation method for efficient and low-cost water electrolysis to produce hydrogen in the future.
