Extremely high-temperature and high-pressure requirement of Haber-Bosch process motivates the search for a sustainable ammonia synthesis approach under mild conditions.Photocatalytic technology is a potential solution...Extremely high-temperature and high-pressure requirement of Haber-Bosch process motivates the search for a sustainable ammonia synthesis approach under mild conditions.Photocatalytic technology is a potential solution to convert N2 to ammonia.However,the poor light absorption and low charge carrier separation efficiency in conventional semiconductors are bottlenecks for the application of this technology.Herein,a facile synthesis of anatase TiO_(2)nanosheets with an abundance of surface oxygen vacancies(TiO_(2)-OV)via the calcination treatment was reported.Photocatalytic experiments of the prepared anatase TiO_(2)samples showed that TiO_(2)-OV nanosheets exhibited remarkably increased ammonia yield for solar-driven N2 fixation in pure water,without adding any sacrificial agents.EPR,XPS,XRD,UV-Vis DRS,TEM,Raman,and PL techniques were employed to systematically explore the possible enhanced mechanism.Studies revealed that the introduced surface oxygen vacancies significantly extended the light absorption capability in the visible region,decreased the adsorption and activation barriers of inert N2,and improved the separation and transfer efficiency of the photogenerated electronhole pairs.Thus,a high rate of ammonia evolution in TiO_(2)-OV was realized.This work offers a promising and sustainable approach for the efficient artificial photosynthesis of ammonia.展开更多
Fresh blood of Tibetan sheep was subjected to protein separation and spray drying, and the effects of drying process on water content, yield and nitrogen soluble index of plasma powder from blood of Tibetan sheep were...Fresh blood of Tibetan sheep was subjected to protein separation and spray drying, and the effects of drying process on water content, yield and nitrogen soluble index of plasma powder from blood of Tibetan sheep were investigated. The results showed that the optimum separation parameters were a centrifugal speed at 6 000 r/min, centrifugal time of 20 min, a mass fraction of dry matter of 20%, an inlet air temperature at 180 ℃ and a feed rate at 400 ml/h, under which the plasma protein was a pale yellow powdery solid, indicating a good separation effect.展开更多
Water quality protection in Sweden has a more than 80-year history. The needed knowledge has by large been imported. Now, to some extent the development of phosphorus removal technology may be Swedish contribution to ...Water quality protection in Sweden has a more than 80-year history. The needed knowledge has by large been imported. Now, to some extent the development of phosphorus removal technology may be Swedish contribution to advanced knowledge. This paper presents the development in Sweden, mainly a close to 50-year period. Starting in the late 1960s, a standard of <0.5 mg P/l was the normally raised effluent criteria, regardless of the magnitude of the discharge flow. The successive sharpening of the discharge levels has today resulted in a level of 0.2 to 0.3 mg P/l typically. As a matter of fact, even levels of 0.1 to 0.15 mg P/l have been discussed. The period should a large extent demonstrated both improved technologies and a far better efficiency with respect to the use of chemicals and energy. Some important points in this development may be the understanding of the Oxygen Consumption Potential, as well as the identified needs for an improved nitrogen removal. Lately the problems of complex pollution agents and predominantly the remains of pharmaceutical agents have been identified. To illustrate the development during the 50-year period, two examples are presented from the Swedish context. The main conclusion in this paper is that the Swedish history on phosphorus removal illustrates how empirical science in practice sometimes works, including a never-ending need for an open mind and a readiness to take revised and improved knowledge on board.展开更多
Photocatalytic O_(2)activation to generate reactive oxygen species is crucially important for purifying organic pollutants,yet remains a challenge due to poor adsorption of O_(2)and low efficiency of electron transfer...Photocatalytic O_(2)activation to generate reactive oxygen species is crucially important for purifying organic pollutants,yet remains a challenge due to poor adsorption of O_(2)and low efficiency of electron transfer.Herein,we demonstrate that ultrafine MoO_(x)clusters anchored on graphitic carbon nitride(g-C_(3)N_(4))with dual nitrogen/oxygen defects promote the photocatalytic activation of O_(2)to generate·O_(2)−for the degradation of tetracycline hydrochloride(TCH).A range of characterization techniques and density functional theory(DFT)calculations reveal that the introduction of the nitrogen/oxygen dual defects and MoO_(x)clusters enhances the O_(2)adsorption energy from−2.77 to−2.94 eV.We find that MoO_(x)clusters with oxygen vacancies(Ov)and surface Ov-mediated Moδ+(3≥δ≥2)possess unpaired localized electrons,which act as electron capture centers to transfer electrons to the MoO_(x)clusters.These electrons can then transfer to the surface adsorbed O_(2),thus promoting the photocatalytic conversion of O_(2)to·O_(2)−and,simultaneously,realizing the efficient separation of photogenerated electron–hole pairs.Our fully-optimized MoO_(x)/g-C_(3)N_(4)catalyst with dual nitrogen/oxygen defects manifests outstanding photoactivities,achieving 79%degradation efficiency toward TCH within 120 min under visible light irradiation,representing nearly 7 times higher activity than pristine g-C_(3)N_(4).Finally,based on the results of liquid chromatograph mass spectrometry and DFT calculations,the possible photocatalytic degradation pathways of TCH were proposed.展开更多
基金supported by the National Natural Science Foundation of China(No.22108108,22205108,and No.22108106)China Postdoctoral Science Foundation No.2022M721381.
文摘Extremely high-temperature and high-pressure requirement of Haber-Bosch process motivates the search for a sustainable ammonia synthesis approach under mild conditions.Photocatalytic technology is a potential solution to convert N2 to ammonia.However,the poor light absorption and low charge carrier separation efficiency in conventional semiconductors are bottlenecks for the application of this technology.Herein,a facile synthesis of anatase TiO_(2)nanosheets with an abundance of surface oxygen vacancies(TiO_(2)-OV)via the calcination treatment was reported.Photocatalytic experiments of the prepared anatase TiO_(2)samples showed that TiO_(2)-OV nanosheets exhibited remarkably increased ammonia yield for solar-driven N2 fixation in pure water,without adding any sacrificial agents.EPR,XPS,XRD,UV-Vis DRS,TEM,Raman,and PL techniques were employed to systematically explore the possible enhanced mechanism.Studies revealed that the introduced surface oxygen vacancies significantly extended the light absorption capability in the visible region,decreased the adsorption and activation barriers of inert N2,and improved the separation and transfer efficiency of the photogenerated electronhole pairs.Thus,a high rate of ammonia evolution in TiO_(2)-OV was realized.This work offers a promising and sustainable approach for the efficient artificial photosynthesis of ammonia.
基金Supported by"123"Science and Technology Support Program from Science and Technology Department of Qinghai Province(2014-GX-136A)~~
文摘Fresh blood of Tibetan sheep was subjected to protein separation and spray drying, and the effects of drying process on water content, yield and nitrogen soluble index of plasma powder from blood of Tibetan sheep were investigated. The results showed that the optimum separation parameters were a centrifugal speed at 6 000 r/min, centrifugal time of 20 min, a mass fraction of dry matter of 20%, an inlet air temperature at 180 ℃ and a feed rate at 400 ml/h, under which the plasma protein was a pale yellow powdery solid, indicating a good separation effect.
文摘Water quality protection in Sweden has a more than 80-year history. The needed knowledge has by large been imported. Now, to some extent the development of phosphorus removal technology may be Swedish contribution to advanced knowledge. This paper presents the development in Sweden, mainly a close to 50-year period. Starting in the late 1960s, a standard of <0.5 mg P/l was the normally raised effluent criteria, regardless of the magnitude of the discharge flow. The successive sharpening of the discharge levels has today resulted in a level of 0.2 to 0.3 mg P/l typically. As a matter of fact, even levels of 0.1 to 0.15 mg P/l have been discussed. The period should a large extent demonstrated both improved technologies and a far better efficiency with respect to the use of chemicals and energy. Some important points in this development may be the understanding of the Oxygen Consumption Potential, as well as the identified needs for an improved nitrogen removal. Lately the problems of complex pollution agents and predominantly the remains of pharmaceutical agents have been identified. To illustrate the development during the 50-year period, two examples are presented from the Swedish context. The main conclusion in this paper is that the Swedish history on phosphorus removal illustrates how empirical science in practice sometimes works, including a never-ending need for an open mind and a readiness to take revised and improved knowledge on board.
基金supported by the National Natural Science Foundation of China(No.21972010)the National Key Research and Development Program of China(No.2022YFC2105900).
文摘Photocatalytic O_(2)activation to generate reactive oxygen species is crucially important for purifying organic pollutants,yet remains a challenge due to poor adsorption of O_(2)and low efficiency of electron transfer.Herein,we demonstrate that ultrafine MoO_(x)clusters anchored on graphitic carbon nitride(g-C_(3)N_(4))with dual nitrogen/oxygen defects promote the photocatalytic activation of O_(2)to generate·O_(2)−for the degradation of tetracycline hydrochloride(TCH).A range of characterization techniques and density functional theory(DFT)calculations reveal that the introduction of the nitrogen/oxygen dual defects and MoO_(x)clusters enhances the O_(2)adsorption energy from−2.77 to−2.94 eV.We find that MoO_(x)clusters with oxygen vacancies(Ov)and surface Ov-mediated Moδ+(3≥δ≥2)possess unpaired localized electrons,which act as electron capture centers to transfer electrons to the MoO_(x)clusters.These electrons can then transfer to the surface adsorbed O_(2),thus promoting the photocatalytic conversion of O_(2)to·O_(2)−and,simultaneously,realizing the efficient separation of photogenerated electron–hole pairs.Our fully-optimized MoO_(x)/g-C_(3)N_(4)catalyst with dual nitrogen/oxygen defects manifests outstanding photoactivities,achieving 79%degradation efficiency toward TCH within 120 min under visible light irradiation,representing nearly 7 times higher activity than pristine g-C_(3)N_(4).Finally,based on the results of liquid chromatograph mass spectrometry and DFT calculations,the possible photocatalytic degradation pathways of TCH were proposed.
