Atmospheric Oxygen(O2)is one of the dominating features that allow the earth to be a habitable planet with advanced civilization and diverse biology.However,since the late 1980 s,observational data have indicated a st...Atmospheric Oxygen(O2)is one of the dominating features that allow the earth to be a habitable planet with advanced civilization and diverse biology.However,since the late 1980 s,observational data have indicated a steady decline in O2 content on the scale of parts-per-million level.The current scientific consensus is that the decline is caused by the fossil-fuel combustion;however,few works have been done to quantitatively evaluate the response of O2 cycle under the anthropogenic impact,at both the global and regional scales.This paper manages to quantify the land O2 flux and makes the initial step to quantificationally describe the anthropogenic impacts on the global O2 budget.Our estimation reveals that the global O2 consumption has experienced an increase from 33.69±1.11 to47.63±0.80 Gt(gigaton,109 t)O2yr^-1 between 2000 and 2018,while the land production of O2(totaling 11.34±13.48 Gt O2yr^-1 averaged over the same period)increased only slightly.In 2018,the combustion of fossil-fuel and industrial activities(38.45±0.61 Gt O2yr^-1)contributed the most to consumption,followed by wildfires(4.97±0.48 Gt O2yr^-1)as well as livestock and human respiration processes(2.48±0.16 and 1.73±0.13 Gt O2yr^-1,respectively).Burning of fossil-fuel that causes large O2 fluxes occurs in East Asia,India,North America,and Europe,while wildfires that cause large fluxes in comparable magnitude are mainly distributed in central Africa.展开更多
The development of visible-light-responsive photocatalysts for promoting solar-driven oxygen(O2)production from water splitting is a potentially attractive but still a challenging scheme.In the present work,a(111)-typ...The development of visible-light-responsive photocatalysts for promoting solar-driven oxygen(O2)production from water splitting is a potentially attractive but still a challenging scheme.In the present work,a(111)-type layered perovskite oxynitride,Sr5Nb4O15-xNx,was synthesized via the nitridation treatment of the disk-like oxide precursor under the ammonia flow,which was fabricated using a flux method.The homogeneous dispersion of nitrogen(N)dopant in N-doped Sr5Nb4O15 was ascertained by energy-dispersive X-ray spectroscopy characterization,and the Sr5Nb4O15-xNx was found to be a direct semiconductor with a light absorption edge of approximately 640 nm.Density functional theory investigation implies that the hybridization between the outmost N 2p orbitals and O 2p orbitals upshifts the original valence band maximum of Sr5Nb4O15 and endows its visible-light-responsive characteristics.Loading with cobalt oxide(CoOx)as cocatalyst,the as-prepared Sr5Nb4O15-xNx exhibited an enhanced photocatalytic O2 evolution activity from water splitting under visible-light illumination(λ>420 nm).Moreover,another homogeneous N-doped layered perovskite-type niobium(Nb)-based oxynitride,Ba5Nb4O15-xNx,was also developed and investigated for the visible-light-actuated O2 production,highlighting the versatility of the present approach for exploring novel visible-light-responsive photocatalysts.展开更多
Magnetic CuO nanosheet(Mag-CuO), as a cheap, stable, efficient and easily separated peroxymonosulfate(PMS) activator, was prepared by a simple one-step precipitation method for the removal of organic compounds from sa...Magnetic CuO nanosheet(Mag-CuO), as a cheap, stable, efficient and easily separated peroxymonosulfate(PMS) activator, was prepared by a simple one-step precipitation method for the removal of organic compounds from salt-containing wastewater.The experiments showed that the removal efficiencies of various organic pollutants including Acid Orange 7, Methylene Blue, Rhodamine B and atrazine in a high-salinity system(0.2 mol/L Na2SO4) with the Mag-CuO/PMS process were 95.81%, 74.57%, 100% and 100%,respectively.Meanwhile, Mag-CuO still maintained excellent catalytic activity in other salt systems including one or more salt components(NaCl, NaNO3, Na2HPO4, NaHCO3).A radical-quenching study and electron paramagnetic resonance analysis confirmed that singlet oxygen(1O2) was the dominant reactive oxygen species for the oxidation of organic pollutants in high-salinity systems, which is less susceptible to hindrance by background constituents in wastewater than radicals(·OH or SO4·-).The surface hydroxylation of the catalyst and catalytic redox cycle including Cu and Fe are responsible for the generation of1O2.The developed Mag-CuO catalyst shows good application prospects for the removal of organic pollutants from saline wastewater.展开更多
基金Supported by the National Natural Science Foundation of China (41521004)China 111 Project (B13045)
文摘Atmospheric Oxygen(O2)is one of the dominating features that allow the earth to be a habitable planet with advanced civilization and diverse biology.However,since the late 1980 s,observational data have indicated a steady decline in O2 content on the scale of parts-per-million level.The current scientific consensus is that the decline is caused by the fossil-fuel combustion;however,few works have been done to quantitatively evaluate the response of O2 cycle under the anthropogenic impact,at both the global and regional scales.This paper manages to quantify the land O2 flux and makes the initial step to quantificationally describe the anthropogenic impacts on the global O2 budget.Our estimation reveals that the global O2 consumption has experienced an increase from 33.69±1.11 to47.63±0.80 Gt(gigaton,109 t)O2yr^-1 between 2000 and 2018,while the land production of O2(totaling 11.34±13.48 Gt O2yr^-1 averaged over the same period)increased only slightly.In 2018,the combustion of fossil-fuel and industrial activities(38.45±0.61 Gt O2yr^-1)contributed the most to consumption,followed by wildfires(4.97±0.48 Gt O2yr^-1)as well as livestock and human respiration processes(2.48±0.16 and 1.73±0.13 Gt O2yr^-1,respectively).Burning of fossil-fuel that causes large O2 fluxes occurs in East Asia,India,North America,and Europe,while wildfires that cause large fluxes in comparable magnitude are mainly distributed in central Africa.
基金the financial support from the National Key R&D Program of China(No.2020YFA0406102)the National Natural Science Foundation of China(Nos.21633009 and 21925206)+2 种基金the International Partnership Program of Chinese Academy of Sciences(No.121421KYSB20190025)the Dalian National Laboratory for Clean Energy(DNL)Cooperation Fund,CAS(No.DNL 201913)the DICP Foundation of Innovative Research(No.DICP I201927)。
文摘The development of visible-light-responsive photocatalysts for promoting solar-driven oxygen(O2)production from water splitting is a potentially attractive but still a challenging scheme.In the present work,a(111)-type layered perovskite oxynitride,Sr5Nb4O15-xNx,was synthesized via the nitridation treatment of the disk-like oxide precursor under the ammonia flow,which was fabricated using a flux method.The homogeneous dispersion of nitrogen(N)dopant in N-doped Sr5Nb4O15 was ascertained by energy-dispersive X-ray spectroscopy characterization,and the Sr5Nb4O15-xNx was found to be a direct semiconductor with a light absorption edge of approximately 640 nm.Density functional theory investigation implies that the hybridization between the outmost N 2p orbitals and O 2p orbitals upshifts the original valence band maximum of Sr5Nb4O15 and endows its visible-light-responsive characteristics.Loading with cobalt oxide(CoOx)as cocatalyst,the as-prepared Sr5Nb4O15-xNx exhibited an enhanced photocatalytic O2 evolution activity from water splitting under visible-light illumination(λ>420 nm).Moreover,another homogeneous N-doped layered perovskite-type niobium(Nb)-based oxynitride,Ba5Nb4O15-xNx,was also developed and investigated for the visible-light-actuated O2 production,highlighting the versatility of the present approach for exploring novel visible-light-responsive photocatalysts.
基金supported by the National Water Pollution Control and Management Program of China (No.2017ZX07107002).
文摘Magnetic CuO nanosheet(Mag-CuO), as a cheap, stable, efficient and easily separated peroxymonosulfate(PMS) activator, was prepared by a simple one-step precipitation method for the removal of organic compounds from salt-containing wastewater.The experiments showed that the removal efficiencies of various organic pollutants including Acid Orange 7, Methylene Blue, Rhodamine B and atrazine in a high-salinity system(0.2 mol/L Na2SO4) with the Mag-CuO/PMS process were 95.81%, 74.57%, 100% and 100%,respectively.Meanwhile, Mag-CuO still maintained excellent catalytic activity in other salt systems including one or more salt components(NaCl, NaNO3, Na2HPO4, NaHCO3).A radical-quenching study and electron paramagnetic resonance analysis confirmed that singlet oxygen(1O2) was the dominant reactive oxygen species for the oxidation of organic pollutants in high-salinity systems, which is less susceptible to hindrance by background constituents in wastewater than radicals(·OH or SO4·-).The surface hydroxylation of the catalyst and catalytic redox cycle including Cu and Fe are responsible for the generation of1O2.The developed Mag-CuO catalyst shows good application prospects for the removal of organic pollutants from saline wastewater.
