First-row(3 d)transition metal oxyhydroxides have attracted increasing attention due to their various advantages.Although investigating the oxidation mechanism and processing such materials into hierarchical architect...First-row(3 d)transition metal oxyhydroxides have attracted increasing attention due to their various advantages.Although investigating the oxidation mechanism and processing such materials into hierarchical architectures are greatly desired for their further development,it remains unclear how the oxidation state change occurs,and efforts to produce hierarchical oxyhydroxides in compliance with high ecological and economic standards have progressed slowly.Here,we describe a facile one-step coprecipitation route for the preparation of hierarchical CoOOH,NiOOH and MnOOH,which involves the diffusion of NH_(3)originating from ammonium hydroxide solution into an aqueous solution containing metal ion salts and K_(2)S_(2)O_(8).Comprehensive characterizations by scanning electron microscope,transmission electron microscopy,X-ray diffraction analysis,X-ray photoelectron spectroscopy,ultraviolet-visible spectroscopy and in situ p H measurement demonstrated that K_(2)S_(2)O_(8)induces the oxidation state change of metal ion species after the start of hydrolysis.Meanwhile,it was found that,benefiting from the OH–concentration gradient created by the NH_(3)diffusion method and the suitable growth environment provided by the presence of K_(2)S_(2)O_(8)(high nucleation rate and secondary nucleation),the formation of hierarchical oxyhydroxide structures can be realized in aqueous solution at ambient temperature without the use of heat energy and additional structure-directing agents.The hierarchical CoOOH structures are performed as the electrocatalysts for the oxygen evolution reaction in alkaline media,which exhibit good activity with an overpotential of 320 m V at 10 m A cm^(-2)and a low Tafel slope of 59.6 m V dec^(–1),outperforming many congeneric electrocatalysts.Overall,our study not only provides important insights to understand the formation mechanism of hierarchical oxyhydroxides,but also opens up new opportunities for the preparation of hierarchical oxyhydroxides via a facile,green and low-cost method.展开更多
In this paper,a two-layer hierarchical structure of optimization and control for polypropylene grade transition was raised to overcome process uncertain disturbances that led to the large deviation between the open-lo...In this paper,a two-layer hierarchical structure of optimization and control for polypropylene grade transition was raised to overcome process uncertain disturbances that led to the large deviation between the open-loop reference trajectory and the actual process.In the upper layer,the variant time scale based control vector parametric methods(VTS-CVP) was used for dynamic optimization of transition reference trajectory,while nonlinear model predictive controller(NMPC) based on closed-loop subspace and piece-wise linear(SSARX-PWL) model in the lower layer was tracking to the reference trajectory from the upper layer for overcoming high-frequency disturbances.Besides,mechanism about trajectory deviation detection and optimal trajectory updating online were introduced to ensure a smooth transition for the entire process.The proposed method was validated with the real data from an industrial double-loop propylene polymerization reaction process with developed dynamic mechanism mathematical model.展开更多
The aim of this work is to explore the impact of regional transit service on tour-based commuter travel behavior by using the Bayesian hierarchical multinomial logit model, accounting for the spatial heterogeneity of ...The aim of this work is to explore the impact of regional transit service on tour-based commuter travel behavior by using the Bayesian hierarchical multinomial logit model, accounting for the spatial heterogeneity of the people living in the same area.With two indicators, accessibility and connectivity measured at the zone level, the regional transit service is captured and then related to the travel mode choice behavior. The sample data are selected from Washington-Baltimore Household Travel Survey in 2007,including all the trips from home to workplace in morning hours in Baltimore city. Traditional multinomial logit model using Bayesian approach is also estimated. A comparison of the two different models shows that ignoring the spatial context can lead to a misspecification of the effects of the regional transit service on travel behavior. The results reveal that improving transit service at regional level can be effective in reducing auto use for commuters after controlling for socio-demographics and travel-related factors.This work provides insights for interpreting tour-based commuter travel behavior by using recently developed methodological approaches. The results of this work will be helpful for engineers, urban planners, and transit operators to decide the needs to improve regional transit service and spatial location efficiently.展开更多
基金funded by the Deutsche Forschungsgemeinschaft DFG and the Sino-German Center for Research Promotion(Grants GZ 1351 and CO 194/19-1)funded by a Chinese Scholarship Council stipend。
文摘First-row(3 d)transition metal oxyhydroxides have attracted increasing attention due to their various advantages.Although investigating the oxidation mechanism and processing such materials into hierarchical architectures are greatly desired for their further development,it remains unclear how the oxidation state change occurs,and efforts to produce hierarchical oxyhydroxides in compliance with high ecological and economic standards have progressed slowly.Here,we describe a facile one-step coprecipitation route for the preparation of hierarchical CoOOH,NiOOH and MnOOH,which involves the diffusion of NH_(3)originating from ammonium hydroxide solution into an aqueous solution containing metal ion salts and K_(2)S_(2)O_(8).Comprehensive characterizations by scanning electron microscope,transmission electron microscopy,X-ray diffraction analysis,X-ray photoelectron spectroscopy,ultraviolet-visible spectroscopy and in situ p H measurement demonstrated that K_(2)S_(2)O_(8)induces the oxidation state change of metal ion species after the start of hydrolysis.Meanwhile,it was found that,benefiting from the OH–concentration gradient created by the NH_(3)diffusion method and the suitable growth environment provided by the presence of K_(2)S_(2)O_(8)(high nucleation rate and secondary nucleation),the formation of hierarchical oxyhydroxide structures can be realized in aqueous solution at ambient temperature without the use of heat energy and additional structure-directing agents.The hierarchical CoOOH structures are performed as the electrocatalysts for the oxygen evolution reaction in alkaline media,which exhibit good activity with an overpotential of 320 m V at 10 m A cm^(-2)and a low Tafel slope of 59.6 m V dec^(–1),outperforming many congeneric electrocatalysts.Overall,our study not only provides important insights to understand the formation mechanism of hierarchical oxyhydroxides,but also opens up new opportunities for the preparation of hierarchical oxyhydroxides via a facile,green and low-cost method.
基金Supported by the Electronic Information Industry Development Foundation of China(20140806)the National Natural Science Foundation of China(61374121,61134007)
文摘In this paper,a two-layer hierarchical structure of optimization and control for polypropylene grade transition was raised to overcome process uncertain disturbances that led to the large deviation between the open-loop reference trajectory and the actual process.In the upper layer,the variant time scale based control vector parametric methods(VTS-CVP) was used for dynamic optimization of transition reference trajectory,while nonlinear model predictive controller(NMPC) based on closed-loop subspace and piece-wise linear(SSARX-PWL) model in the lower layer was tracking to the reference trajectory from the upper layer for overcoming high-frequency disturbances.Besides,mechanism about trajectory deviation detection and optimal trajectory updating online were introduced to ensure a smooth transition for the entire process.The proposed method was validated with the real data from an industrial double-loop propylene polymerization reaction process with developed dynamic mechanism mathematical model.
基金Project(71173061)supported by the National Natural Science Foundation of ChinaProject(2013U-6)supported by Key Laboratory of Eco Planning & Green Building,Ministry of Education(Tsinghua University),China
文摘The aim of this work is to explore the impact of regional transit service on tour-based commuter travel behavior by using the Bayesian hierarchical multinomial logit model, accounting for the spatial heterogeneity of the people living in the same area.With two indicators, accessibility and connectivity measured at the zone level, the regional transit service is captured and then related to the travel mode choice behavior. The sample data are selected from Washington-Baltimore Household Travel Survey in 2007,including all the trips from home to workplace in morning hours in Baltimore city. Traditional multinomial logit model using Bayesian approach is also estimated. A comparison of the two different models shows that ignoring the spatial context can lead to a misspecification of the effects of the regional transit service on travel behavior. The results reveal that improving transit service at regional level can be effective in reducing auto use for commuters after controlling for socio-demographics and travel-related factors.This work provides insights for interpreting tour-based commuter travel behavior by using recently developed methodological approaches. The results of this work will be helpful for engineers, urban planners, and transit operators to decide the needs to improve regional transit service and spatial location efficiently.