As a substitute for synthetic ammonia under mild condition, electrocatalytic nitrogen reduction reaction(NRR) provides a hopeful approach for the development of ammonia. Nevertheless, the current development of NRR el...As a substitute for synthetic ammonia under mild condition, electrocatalytic nitrogen reduction reaction(NRR) provides a hopeful approach for the development of ammonia. Nevertheless, the current development of NRR electrocatalysts is far from enough and a systematic research is needed to gain a better improvement. This article presents that 2 D C_(3)N_(4)-NV with a large specific surface area and abundant nitrogen vacancies is prepared by a simple and feasible method, and used as a metal-free catalyst for electrocatalytic NRR. Experiment result and density functional theory(DFT) calculation reveal that nitrogen vacancies in 2 D C_(3)N_(4)-NV can act as an efficient active site for catalytic NRR, which is conducive to capturing and activating N_(2), lowering Gibbs free energy(DG) in reaction and inhibiting hydrogen evolution reaction(HER) at the same time. In addition, the larger specific surface area also makes more active site exposed, which is good for the contact between the electrolyte and the active site, thus enhancing its NRR activity. The electrocatalyst shows an excellent catalytic activity for NRR in 0.1 M HCl, including Faradaic efficiency of 10.96%, NH_(3) yields of 17.85 lg h^(-1) mg_(cat)^(-1)., and good stability(over 20 h).展开更多
The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon m...The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.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
A series of alumina samples were prepared using β-cyclodextrin as the non-surfactant template. These samples were characterized by XRD, BET and TEM. The results showed that the alumina samples prepared using β-cyclo...A series of alumina samples were prepared using β-cyclodextrin as the non-surfactant template. These samples were characterized by XRD, BET and TEM. The results showed that the alumina samples prepared using β-cyclodextrin template had the higher surface areas （124-484 m^2/g）, larger pore volumes （0.7-1.27 mL/g） and more thermal stability than samples prepared without using β-cyclodextrin.展开更多
The carbon dioxide reduction reaction(CO_(2)RR)for the synthesis of high-energy-density and high-value multi-carbon(C_(2+))products has demonstrated consider-able potential for practical applications.In this work,we d...The carbon dioxide reduction reaction(CO_(2)RR)for the synthesis of high-energy-density and high-value multi-carbon(C_(2+))products has demonstrated consider-able potential for practical applications.In this work,we design a novel copper oxide foam(OD-Cu foam)catalyst through a high-temperature calcination pro-cess,characterized by a substantial specific surface area.The distinctive three-dimensional structure of the OD-Cu foam catalyst and the metal oxide particles covered on its surface provide abundant active sites.The total Faradaic efficiency of 57.3%for C_(2+)products over the OD-Cu foam is achieved at-0.85 V versus reversible hydrogen electrode(RHE).Furthermore,the partial current density for C_(2+)products over the OD-Cu foam reaches 44.1 mA cm^(-2)at-0.95 V versus RHE,surpassing significantly that both of Cu foam(3.4 mA cm^(-2))and copper oxide foil(OD-Cu foil)(1.6 mA cm^(-2)).In addition,the integrated structure of the OD-Cu foam,which does not require complex preparation processes,facilitates its application in CO_(2)RR.These results underscore the significance of three-dimensional structure and high specific surface area,emphasizing the consider-able potential of this catalyst for effective and sustainable CO_(2)conversion.展开更多
基金funded by the National Natural Science Foundation of China (21802058 and 21872066)the Fundamental Research Funds for the Central Universities (China, lzujbky-2020-42)the Natural Science Foundation of Gansu Province (20JR5RA225)。
文摘As a substitute for synthetic ammonia under mild condition, electrocatalytic nitrogen reduction reaction(NRR) provides a hopeful approach for the development of ammonia. Nevertheless, the current development of NRR electrocatalysts is far from enough and a systematic research is needed to gain a better improvement. This article presents that 2 D C_(3)N_(4)-NV with a large specific surface area and abundant nitrogen vacancies is prepared by a simple and feasible method, and used as a metal-free catalyst for electrocatalytic NRR. Experiment result and density functional theory(DFT) calculation reveal that nitrogen vacancies in 2 D C_(3)N_(4)-NV can act as an efficient active site for catalytic NRR, which is conducive to capturing and activating N_(2), lowering Gibbs free energy(DG) in reaction and inhibiting hydrogen evolution reaction(HER) at the same time. In addition, the larger specific surface area also makes more active site exposed, which is good for the contact between the electrolyte and the active site, thus enhancing its NRR activity. The electrocatalyst shows an excellent catalytic activity for NRR in 0.1 M HCl, including Faradaic efficiency of 10.96%, NH_(3) yields of 17.85 lg h^(-1) mg_(cat)^(-1)., and good stability(over 20 h).
文摘The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.
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A series of alumina samples were prepared using β-cyclodextrin as the non-surfactant template. These samples were characterized by XRD, BET and TEM. The results showed that the alumina samples prepared using β-cyclodextrin template had the higher surface areas （124-484 m^2/g）, larger pore volumes （0.7-1.27 mL/g） and more thermal stability than samples prepared without using β-cyclodextrin.
基金supported by the Jiangxi Gan Po Talent Support Program(20232BCJ22028).
文摘The carbon dioxide reduction reaction(CO_(2)RR)for the synthesis of high-energy-density and high-value multi-carbon(C_(2+))products has demonstrated consider-able potential for practical applications.In this work,we design a novel copper oxide foam(OD-Cu foam)catalyst through a high-temperature calcination pro-cess,characterized by a substantial specific surface area.The distinctive three-dimensional structure of the OD-Cu foam catalyst and the metal oxide particles covered on its surface provide abundant active sites.The total Faradaic efficiency of 57.3%for C_(2+)products over the OD-Cu foam is achieved at-0.85 V versus reversible hydrogen electrode(RHE).Furthermore,the partial current density for C_(2+)products over the OD-Cu foam reaches 44.1 mA cm^(-2)at-0.95 V versus RHE,surpassing significantly that both of Cu foam(3.4 mA cm^(-2))and copper oxide foil(OD-Cu foil)(1.6 mA cm^(-2)).In addition,the integrated structure of the OD-Cu foam,which does not require complex preparation processes,facilitates its application in CO_(2)RR.These results underscore the significance of three-dimensional structure and high specific surface area,emphasizing the consider-able potential of this catalyst for effective and sustainable CO_(2)conversion.
