Understanding the performance of reactive oxygen species(ROS)in photocatalysis is pivotal for advancing their application in environmental remediation.However,techniques for investigating the generation and transforma...Understanding the performance of reactive oxygen species(ROS)in photocatalysis is pivotal for advancing their application in environmental remediation.However,techniques for investigating the generation and transformation mechanism of ROS have been largely overlooked.In this study,considering g‐C3N4 to be a model photocatalyst,we have focused on the ROS generation and transformation for efficient photocatalytic NO removal.It was found that the key to improving the photocatalysis performance was to enhance the ROS transformation from·O2^-to·OH,elevating the production of·OH.The ROS directly participate in the photocatalytic NO removal and tailor the rate‐determining step,which is required to overcome the high activation energy of the intermediate conversion.Using a closely combined experimental and theoretical method,this work provides a new protocol to investigate the ROS behavior on g‐C3N4 for effective NO removal and clarifies the reaction mechanism at the atomic level,which enriches the understanding of ROS in photocatalytic environmental remediation.展开更多
A Pt-Rh three-way catalyst（M-DS） supported on CeO_2-ZrO_2-La_2O_3-Nd_2O_3 and its analogous supported catalyst（DS） were developed via a modified double-solvent method and conventional double-solvent method, respec...A Pt-Rh three-way catalyst（M-DS） supported on CeO_2-ZrO_2-La_2O_3-Nd_2O_3 and its analogous supported catalyst（DS） were developed via a modified double-solvent method and conventional double-solvent method, respectively. The as-prepared catalysts were characterized by N_2 adsorption-desorption, X-ray diffraction（XRD）, CO-chemisorption, X-ray photoelectron spectroscopy（XPS） and hydrogen temperature-programmed reduction（H_2-TPR）. The preformed Pt nanoparticles generated using ethanol as a reducing agent on M-DS presented enhanced Pt dispersion regardless of aging treatment as confirmed by XRD and CO-chemisorption measurements. The textural properties and reduction ability of M-DS were maintained to a large extent after aging treatment. This result was consistent with those of the N_2 adsorption-desorption and H_2-TPR, respectively. Meanwhile, the XPS analysis demonstrated that higher Pt^0 species and larger Ce^（3＋） concentration could be obtained for M-DS. In the conversion of a simulated compressed natural gas（CNG） vehicle exhaust, both fresh and aged M-DS showed a significant enhancement in the activity and N_2-selectivity. Particularly, the complete conversion temperature（T_（90）） of CH_4 over the aged M-DS catalyst was 65 oC lower than that over the aged catalyst by conventional double-solvent method.展开更多
基金the National Natural Science Foundation of China(51508356)Science and Technology Support Program of Sichuan Province(2014GZ0213,2016GZ0045)Youth Project in Science and Technology Innovation Program of Sichuan Province(17-YCG053)~~
文摘Understanding the performance of reactive oxygen species(ROS)in photocatalysis is pivotal for advancing their application in environmental remediation.However,techniques for investigating the generation and transformation mechanism of ROS have been largely overlooked.In this study,considering g‐C3N4 to be a model photocatalyst,we have focused on the ROS generation and transformation for efficient photocatalytic NO removal.It was found that the key to improving the photocatalysis performance was to enhance the ROS transformation from·O2^-to·OH,elevating the production of·OH.The ROS directly participate in the photocatalytic NO removal and tailor the rate‐determining step,which is required to overcome the high activation energy of the intermediate conversion.Using a closely combined experimental and theoretical method,this work provides a new protocol to investigate the ROS behavior on g‐C3N4 for effective NO removal and clarifies the reaction mechanism at the atomic level,which enriches the understanding of ROS in photocatalytic environmental remediation.
基金supported by the National Key Research and Development Program of China(2016YFC0204902)
文摘A Pt-Rh three-way catalyst（M-DS） supported on CeO_2-ZrO_2-La_2O_3-Nd_2O_3 and its analogous supported catalyst（DS） were developed via a modified double-solvent method and conventional double-solvent method, respectively. The as-prepared catalysts were characterized by N_2 adsorption-desorption, X-ray diffraction（XRD）, CO-chemisorption, X-ray photoelectron spectroscopy（XPS） and hydrogen temperature-programmed reduction（H_2-TPR）. The preformed Pt nanoparticles generated using ethanol as a reducing agent on M-DS presented enhanced Pt dispersion regardless of aging treatment as confirmed by XRD and CO-chemisorption measurements. The textural properties and reduction ability of M-DS were maintained to a large extent after aging treatment. This result was consistent with those of the N_2 adsorption-desorption and H_2-TPR, respectively. Meanwhile, the XPS analysis demonstrated that higher Pt^0 species and larger Ce^（3＋） concentration could be obtained for M-DS. In the conversion of a simulated compressed natural gas（CNG） vehicle exhaust, both fresh and aged M-DS showed a significant enhancement in the activity and N_2-selectivity. Particularly, the complete conversion temperature（T_（90）） of CH_4 over the aged M-DS catalyst was 65 oC lower than that over the aged catalyst by conventional double-solvent method.
