Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is chall...Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.展开更多
Excessive exposure to ultraviolet(UV)radiation harms humans and ecosystems.The level of surface UV radiation had increased due to declines in stratospheric ozone in the late 1970s in response to emissions of chloroflu...Excessive exposure to ultraviolet(UV)radiation harms humans and ecosystems.The level of surface UV radiation had increased due to declines in stratospheric ozone in the late 1970s in response to emissions of chlorofluorocarbons.Following the implementation of the Montreal Protocol,the stratospheric loading of chlorine/bromine peaked in the late 1990s and then decreased;subsequently,stratospheric ozone and surface UV radiation would be expected to recover and decrease,respectively.Here,we show,based on multiple data sources,that the May–September surface UV radiation in the tropics and Northern Hemisphere mid-latitudes has undergone a statistically significant increasing trend[about 60.0 J m^(–2)(10 yr)^(–1)]at the 2σlevel for the period 2010–20,due to the onset of total column ozone(TCO)depletion[about−3.5 DU(10 yr)^(–1)].Further analysis shows that the declines in stratospheric ozone after 2010 could be related to an increase in stratospheric nitrogen oxides due to increasing emissions of the source gas nitrous oxide(N_(2)O).展开更多
制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时...制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时,废水中4BS的去除率达到了93 7%.与均相UV Fenton体系不同,非均相UV Fe Cu Mn Y H2O2体系在碱性条件下(pH=10 5)仍可高效去除CODCr.动力学研究得到催化氧化4BS废水的模型方程,该模型可以为非均相UV Fe Cu Mn Y H2O2体系处理高色度的实际染料废水提供指导.展开更多
采用UV/H2O2技术对污染水体中的MTBE进行了氧化降解试验,考察了不同MTBE初始浓度,不同H2O2浓度,不同pH值,不同波长的紫外光对降解效果的影响,以及不同Cl-、HCO3-浓度的抑制作用.结果表明,在室温条件下,当紫外光波长为254 nm,H2O2为15 m ...采用UV/H2O2技术对污染水体中的MTBE进行了氧化降解试验,考察了不同MTBE初始浓度,不同H2O2浓度,不同pH值,不同波长的紫外光对降解效果的影响,以及不同Cl-、HCO3-浓度的抑制作用.结果表明,在室温条件下,当紫外光波长为254 nm,H2O2为15 m mol/L,pH为3.0时对起始浓度为1 m mol/L的MTBE具有较好的降解效果;反应60 min,MTBE去除率可达97.6%.实验证明,UV/H2O2氧化技术是降解MTBE的一种有效方法.展开更多
文摘Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+) on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2) generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+) interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H_(4) formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of *CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2) products at the Cu^(0)/Cu^(+) interface than that of H_(2) under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2) products.
基金Funding for this work was provided by the National Natural Science Foundation of China(Grant Nos.42122037,42105016,41975047).
文摘Excessive exposure to ultraviolet(UV)radiation harms humans and ecosystems.The level of surface UV radiation had increased due to declines in stratospheric ozone in the late 1970s in response to emissions of chlorofluorocarbons.Following the implementation of the Montreal Protocol,the stratospheric loading of chlorine/bromine peaked in the late 1990s and then decreased;subsequently,stratospheric ozone and surface UV radiation would be expected to recover and decrease,respectively.Here,we show,based on multiple data sources,that the May–September surface UV radiation in the tropics and Northern Hemisphere mid-latitudes has undergone a statistically significant increasing trend[about 60.0 J m^(–2)(10 yr)^(–1)]at the 2σlevel for the period 2010–20,due to the onset of total column ozone(TCO)depletion[about−3.5 DU(10 yr)^(–1)].Further analysis shows that the declines in stratospheric ozone after 2010 could be related to an increase in stratospheric nitrogen oxides due to increasing emissions of the source gas nitrous oxide(N_(2)O).
文摘制备了负载在Na Y分子筛上的Fe Cu Mn Y复合催化剂,并对其在非均相UV Fe Cu Mn Y H2O2体系中催化氧化4BS染料废水进行了研究.结果表明,非均相UV Fe Cu Mn Y H2O2体系对4BS染料废水的处理具有很高的效率.在基准条件下,反应时间为20min时,废水中4BS的去除率达到了93 7%.与均相UV Fenton体系不同,非均相UV Fe Cu Mn Y H2O2体系在碱性条件下(pH=10 5)仍可高效去除CODCr.动力学研究得到催化氧化4BS废水的模型方程,该模型可以为非均相UV Fe Cu Mn Y H2O2体系处理高色度的实际染料废水提供指导.
文摘采用UV/H2O2技术对污染水体中的MTBE进行了氧化降解试验,考察了不同MTBE初始浓度,不同H2O2浓度,不同pH值,不同波长的紫外光对降解效果的影响,以及不同Cl-、HCO3-浓度的抑制作用.结果表明,在室温条件下,当紫外光波长为254 nm,H2O2为15 m mol/L,pH为3.0时对起始浓度为1 m mol/L的MTBE具有较好的降解效果;反应60 min,MTBE去除率可达97.6%.实验证明,UV/H2O2氧化技术是降解MTBE的一种有效方法.
