As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an...As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an attractive route for generating efficient electrocatalysts with high mass transport capabilities.Herein,we report an efficient hard templating pathway to design and synthesize three-dimensional(3-D)mesoporous ternary nickel iron nitride(Ni3FeN).The as-synthesized electrocatalyst shows good OER performance in an alkaline solution with low overpotential(259 mV)and a small Tafel slope(54 mV dec?1),giving superior performance to IrO2 and RuO2 catalysts.The highly active contact area,the hierarchical porosity,and the synergistic effect of bimetal atoms contributed to the improved electrocatalytic performance toward OER.In a practical rechargeable Zn–air battery,mesoporous Ni3FeN is also shown to deliver a lower charging voltage and longer lifetime than RuO2.This work opens up a new promising approach to synthesize active OER electrocatalysts for energy-related devices.展开更多
The carbonization process of a sucrose‐RuCl3/SBA‐15composite towards a Ru‐containing ordered mesoporous carbon(Ru‐OMC)catalyst was studied by in situ temperature‐programmed infrared spectroscopy to identify the s...The carbonization process of a sucrose‐RuCl3/SBA‐15composite towards a Ru‐containing ordered mesoporous carbon(Ru‐OMC)catalyst was studied by in situ temperature‐programmed infrared spectroscopy to identify the stabilization role of organic carbon precursors during the formation of highly dispersed Ru nanoparticles.The results show that the formation of metal carbonyl species results in the formation of homogeneously distributed Ru nanoparticles,and the rigid silica support and carbon matrix around the Ru(CO)x complex can significantly avoid the sintering and agglomeration of Ru metal particles during elevated temperature thermal treatment.These results ultimately demonstrate that sucrose plays important roles in the formation of homogeneously distributed Ru nanoparticles in a porous carbon matrix.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
The active sites for hydrogenation over Ru/SBA‐15catalysts were identified using in situ Fourier‐transform infrared spectroscopy.The amount of active sites was proportional to the interfacial circumference of the Ru...The active sites for hydrogenation over Ru/SBA‐15catalysts were identified using in situ Fourier‐transform infrared spectroscopy.The amount of active sites was proportional to the interfacial circumference of the Ru particles.In contrast,the rate of hydrogen spillover from Ru to the support was inversely proportional to the size of the Ru metal particles.Consequently,a catalyst with small Ru metal particles has a high rate of hydrogen spillover but a low density of active sites,whereas one with large Ru particles has a low rate of hydrogen spillover but a high density of active sites.The formation of these active sites is probably an intermediate step in hydrogen spillover.展开更多
基金supported by Chinese Academy of Sciences(Grant No.2018PS0011)100 Talent Plan of Chinese Academy of Sciences+4 种基金Natural Science Foundation of China(Grant No.61971405)the Department of Science and Technology(GoI)for support through the Project Nos.DST FILE NO.YSS/2015/001712,DST 11-IFAPH-07 and DST FILE NO.DST/TMD/SERI/HUBthe financial support from Equipment Research Program(Grant No.6140721050215)the Ontario Ministry of Research and Innovation(ER15-11-123)the Natural Science and Engineering Council of Canada(RGPIN-2019-05994).
文摘As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an attractive route for generating efficient electrocatalysts with high mass transport capabilities.Herein,we report an efficient hard templating pathway to design and synthesize three-dimensional(3-D)mesoporous ternary nickel iron nitride(Ni3FeN).The as-synthesized electrocatalyst shows good OER performance in an alkaline solution with low overpotential(259 mV)and a small Tafel slope(54 mV dec?1),giving superior performance to IrO2 and RuO2 catalysts.The highly active contact area,the hierarchical porosity,and the synergistic effect of bimetal atoms contributed to the improved electrocatalytic performance toward OER.In a practical rechargeable Zn–air battery,mesoporous Ni3FeN is also shown to deliver a lower charging voltage and longer lifetime than RuO2.This work opens up a new promising approach to synthesize active OER electrocatalysts for energy-related devices.
基金supported by the Natural Science Foundation of Zhejiang Province(LY17B030010)~~
文摘The carbonization process of a sucrose‐RuCl3/SBA‐15composite towards a Ru‐containing ordered mesoporous carbon(Ru‐OMC)catalyst was studied by in situ temperature‐programmed infrared spectroscopy to identify the stabilization role of organic carbon precursors during the formation of highly dispersed Ru nanoparticles.The results show that the formation of metal carbonyl species results in the formation of homogeneously distributed Ru nanoparticles,and the rigid silica support and carbon matrix around the Ru(CO)x complex can significantly avoid the sintering and agglomeration of Ru metal particles during elevated temperature thermal treatment.These results ultimately demonstrate that sucrose plays important roles in the formation of homogeneously distributed Ru nanoparticles in a porous carbon matrix.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
基金supported by the National Natural Science Foundation of China(21303163)the Natural Science Foundation of Zhejiang Province(LY13B030006,LY17B060006)+1 种基金the Qianjiang Talent Project in Zhejiang Province(QJD1302011)the Scientific Research Fund of Zhejiang Provincial Education Department(Y201328681)~~
文摘The active sites for hydrogenation over Ru/SBA‐15catalysts were identified using in situ Fourier‐transform infrared spectroscopy.The amount of active sites was proportional to the interfacial circumference of the Ru particles.In contrast,the rate of hydrogen spillover from Ru to the support was inversely proportional to the size of the Ru metal particles.Consequently,a catalyst with small Ru metal particles has a high rate of hydrogen spillover but a low density of active sites,whereas one with large Ru particles has a low rate of hydrogen spillover but a high density of active sites.The formation of these active sites is probably an intermediate step in hydrogen spillover.