The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective ...The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner.In this review,we investigate the development of industrialwaste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste.We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification,in which the active components,pore size,and phase structure can be altered.The review will discuss the potential of using industrial solid wastes,these modified materials,or synthesized materials from raw waste precursors for the removal of air pollutants,including SO_(2),NO_(x),Hg^(0),H_(2)S,VOCs,and CO_(2).The challenges still need to be addressed to realize this potential and the prospects for future research fully.The suggestions for future directions include determining the optimal composition of these materials,calculating the real reaction rate and turnover frequency,developing effective treatment methods,and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.展开更多
Reservoirs play a critical role in addressing water resources challenges.However,their vertical influence on the assembly mechanisms of different microbial communities,including prokaryotes and eukaryotes,remains uncl...Reservoirs play a critical role in addressing water resources challenges.However,their vertical influence on the assembly mechanisms of different microbial communities,including prokaryotes and eukaryotes,remains unclear.This study examined the vertical diversity patterns of abundant and rare subcommunities of prokaryotes and eukaryotes in an urban reservoir,using water depth as a geographical gradient and employing high-throughput sequencing.The impact of vertical environmental heterogeneity on community structure was quantified,and key drivers of these dynamics were identified.The results indicated that the urban reservoir exhibited statistically significant differences in the vertical distribution of water temperature and oxidation/reduction potential.The a-diversity of the abundant subcommunity displayed an opposing vertical pattern compared to that of the rare subcommunity,while the b-diversity for both subcommunities of prokaryotes and eukaryotes increased with water depth.Moreover,the distinct diversity patterns of abundant and rare subcommunities were associated with environmental heterogeneity and species adaptability.Notably,the b-diversity of the rare subcommunity of eukaryotes was primarily driven by species turnover in surface water,whereas nestedness became the dominant factor in deeper water.Furthermore,eukaryotic microbes exhibited a more pronounced response to changes in water depth than prokaryotes,consistent with the importance of heterogeneous selection to the eukaryotic community.Water temperature significantly affected the community composition of all groups,highlighting its importance in shaping community dynamics.This study provides valuable insights into the vertical distribution and assembly mechanisms of microbial communities in urban reservoirs,contributing to the protection and management of aquatic ecosystems under river regulation.展开更多
Enhancing soil organic matter characteristics,ameliorating physical structure,mitigating heavy metal toxicity,and hastening mineral weathering processes are crucial approaches to accomplish the transition of tailings ...Enhancing soil organic matter characteristics,ameliorating physical structure,mitigating heavy metal toxicity,and hastening mineral weathering processes are crucial approaches to accomplish the transition of tailings substrate to a soil-like substrate.The incorporation of biomass co-pyrolysis and plant colonization has been established to be a significant factor in soil substrate formation and soil pollutant remediation.Despite this,there is presently an absence of research efforts aimed at synergistically utilizing these two technologies to expedite the process of mining tailings soil substrate formation.The current study aimed to investigate the underlying mechanism of geochemical changes and rapid mineral weathering during the process of transforming tailings substrate into a soil-like substrate,under the combined effects of biomass co-smoldering pyrolysis and plant colonization.The findings of this study suggest that the incorporation of smoldering pyrolysis and plant colonization induces a high-temperature effect and biological effects,which enhance the physical and chemical properties of tailings,while simultaneously accelerating the rate of mineral weathering.Notable improvements include the amelioration of extreme pH levels,nutrient enrichment,the formation of aggregates,and an increase in enzyme activity,all of which collectively demonstrate the successful attainment of tailings substrate reconstruction.Evidence of the acceleratedweathering was verified by phase and surfacemorphology analysis using X-ray diffraction and scanning electron microscopy.Discovered corrosion and fragmentation on the surface ofminerals.The weathering resulted in corrosion and fragmentation of the surface of the treated mineral.This study confirms that co-smoldering pyrolysis of biomass,combined with plant colonization,can effectively promote the transformation of tailings into soil-like substrates.This method has can effectively address the key challenges that have previously hindered sustainable development of the mining industry and provides a novel approach for ecological restoration of tailings deposits.展开更多
Objective Recent studies have highlighted the critical role of NUDT19 in the initiation,progression,and prognosis of specific cancer types.However,its involvement in pan-cancer analysis has not been fully characterize...Objective Recent studies have highlighted the critical role of NUDT19 in the initiation,progression,and prognosis of specific cancer types.However,its involvement in pan-cancer analysis has not been fully characterized.This study aims to systematically explore the expression patterns,clinical significance,and immune-related functions of NUDT19 in various cancer types through multi-omics analysis,further revealing its potential role in cancer,particularly its functional and therapeutic target value in leukemia.Methods To achieve this goal,various bioinformatics approaches were employed to evaluate the expression patterns,clinical significance,and immune-related functions of NUDT19 in tumors and normal tissues.Additionally,we analyzed the mutation characteristics of NUDT19 and its relationship with epigenetic modifications.Using the single-cell analysis tool SingleCellBase,we explored the distribution of NUDT19 across different cell subpopulations in tumors.To validate these findings,qRT-PCR was used to measure NUDT19 expression levels in specific tumor cell lines,and we established acute myeloid leukemia(AML)cell lines(HL-60 and THP-1)to conduct NUDT19 knockdown and overexpression experiments,assessing its effects on leukemia cell proliferation,apoptosis,and invasion.Results Pan-cancer analysis revealed the dysregulated expression of NUDT19 across multiple cancer types,which was closely associated with poor prognosis,clinical staging,and diagnostic markers.Furthermore,NUDT19 was significantly correlated with tumor biomarkers,immune-related genes,and immune cell infiltration in different cancers.Mutation analysis showed that multiple mutations in NUDT19 were significantly associated with epigenetic changes.Single-cell analysis revealed the heterogeneity of NUDT19 expression in cancer cells,suggesting its potentially diverse functional roles in different cell subpopulations.qRT-PCR experiments confirmed the significant upregulation of NUDT19 in various tumor cell lines.In AML cell lines,NUDT19 knockdown led to reduced cell proliferation and invasion,with increased apoptosis,while NUDT19 overexpression significantly enhanced cell proliferation and invasion while reducing apoptosis.Conclusion This study demonstrates the diverse roles of NUDT19 in various cancer types,with a particularly prominent functional role in leukemia.NUDT19 is not only associated with tumor initiation and progression but may also influence cancer progression through the regulation of immune microenvironment and epigenetic mechanisms.Our research highlights the potential of NUDT19 as a therapeutic target,particularly for targeted therapies in malignancies such as leukemia,with significant clinical application prospects.展开更多
Metal nanoparticle(NP_S)catalysts exhibit desirable activities in various catalytic reactions.However,the sintering of metal NPs at high-temperatures even in reducing atmospheres limits its practical application.In th...Metal nanoparticle(NP_S)catalysts exhibit desirable activities in various catalytic reactions.However,the sintering of metal NPs at high-temperatures even in reducing atmospheres limits its practical application.In this work,we successfully synthesized TPA-ZSM-5 with pit-type defects by treating the ZSM-5 with tetrahydroxy ammonium hydroxide(TPAOH),which was then used as a support to prepare Ag-based and Cu-based catalysts.Stability testing results show that the Ag/TPA-ZSM-5 catalyst treated at 800℃with H_(2) could maintain the high performance in NH_(3)-SCO and the Cu/TPA-ZSM-5 catalyst treated at 900℃ with N_(2) could maintained its excellent activity in NH_(3)-SCR,however,the activities of Ag/ZSM-5 and Cu/ZSM-5 were drastically decreased or even deactivated after high-temperature treatment.In addition,a series of characterization analyses revealed that the excellent thermal stability is attribute to the presence of pit-type defects in the TPA-ZSM-5 as physical barriers to slow down or even inhibit the Ag NPs and Cu NPs sintering process.The strategy of using the pit-type defects to inhibit the sintering of metal NPs and improve the thermal stability can greatly enhance the practical application of catalysts.展开更多
To improve the activity of Co/Al_(2)O_(3)catalysts in selective catalytic oxidation of ammonia(NH_(3)-SCO),valence state and size of active centers of Al_(2)O_(3)-supported Co catalysts were adjusted by conducting H_(...To improve the activity of Co/Al_(2)O_(3)catalysts in selective catalytic oxidation of ammonia(NH_(3)-SCO),valence state and size of active centers of Al_(2)O_(3)-supported Co catalysts were adjusted by conducting H_(2)reduction pretreatment.The NH_(3)-SCO activity of the adjusted 2Co/Al_(2)O_(3)catalyst was substantially improved,outperforming other catalysts with higher Co-loading.Fresh Co/Al_(2)O_(3)catalysts exhibited multitemperature reduction processes,enabling the control of the valence state of the Co-active centers by adjusting the reduction temperature.Changes in the state of the Co-active centers also led to differences in redox capacity of the catalysts,resulting in different reaction mechanisms for NH_(3)-SCO.However,in situ diffuse reflectance infrared Fourier transform spectra revealed that an excessive O_(2)activation capacity caused overoxidation of NH_(3)to NO and NO_(2).The NH_(3)-SCO activity of the 2Co/Al_(2)O_(3)catalyst with low redox capacity was successfully increased while controlling and optimizing the N_(2)selectivity by modulating the active centers via H_(2)pretreatment,which is a universalmethod used for enhancing the redox properties of catalysts.Thus,this method has great potential for application in the design of inexpensive and highly active catalysts.展开更多
In this study,a novel Pt-loaded Cu Pc/g-C_(3)N_(4)(Pt Cu CN)composite was synthesized for the selective photocatalytic reduction of CO_(2)to CH_(4)under visible light.The Pt Cu CN catalyst achieved a CH_(4)yield of 3...In this study,a novel Pt-loaded Cu Pc/g-C_(3)N_(4)(Pt Cu CN)composite was synthesized for the selective photocatalytic reduction of CO_(2)to CH_(4)under visible light.The Pt Cu CN catalyst achieved a CH_(4)yield of 39.8μmol g^(-1)h^(-1),significantly outperforming bulk g-C_(3)N_(4)and Cu Pc alone by factors of 2.5 and 3.1,respectively,with a high selectivity of 90%.In comparison with other commonly studied photocatalysts,such as g-C_(3)N_(4)-based catalysts,the Pt Cu CN composite exhibited superior CH_(4)yield and product selectivity,demonstrating its potential as a more efficient photocatalyst for CO_(2)reduction.X-ray photoelectron spectroscopy(XPS),density functional theory(DFT)calculations,and in-situ infrared(IR)analysis revealed that the Pt^(0)species effectively lower the activation energy for CH_(4)formation,while Cu Pc extends the light absorption range and enhances charge separation.The combined effects of these components in a Z-scheme heterojunction provide new insights into designing highly selective CO_(2)-to-CH_(4)photocatalysts.This work demonstrates the potential of Pt Cu CN as a highly efficient and stable catalyst for CO_(2)reduction to CH_(4)under visible light.展开更多
The ACF adsorbent with high Cu loading was treated with dielectric barrier discharge plasma to mitigate the negative effects of high Cu loading and enhance PH_(3)and H_(2)S adsorption and oxidation.Bruno-Emmett-Taylor...The ACF adsorbent with high Cu loading was treated with dielectric barrier discharge plasma to mitigate the negative effects of high Cu loading and enhance PH_(3)and H_(2)S adsorption and oxidation.Bruno-Emmett-Taylor(BET)result showed that the specific surface area of the adsorbent after air plasma modification was almost three times that before modification.X-ray photoelectron spectroscopy(XPS)findings revealed that the amino group was added to the adsorbent's surface,increasing lattice oxygen and chemisorbed oxygen.The adsorbent's large specific surface area,excellent surface active oxygen,and abundance of basic groups facilitate PH_(3)and H_(2)S adsorption and oxidation.The scanning electron microscopy showed that air plasma modification exposed more active components and uniformly dispersed them on the surface of adsorbent,thereby improving the adsorption performance.Activity evaluation results showed that the adsorbent has the best ability to capture PH_(3)and H_(2)S after being modified by air plasma at 4 kV voltage for 10 min.The adsorbent's breakthrough ability at high space velocity(WHSV:60,000 h^(−1))is 190 mg P/g and 146 mg S/g,respectively,which is 74%and 60%greater than that before modification.This is a great improvement over previous studies.In addition,the possible mechanism of adsorbent deactivation was proposed.展开更多
This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25,50,85,200,and 300,used for the removal of H_(2)S in lowtemperature,low-oxygen environments.The imp...This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25,50,85,200,and 300,used for the removal of H_(2)S in lowtemperature,low-oxygen environments.The impact of different Si/Al ratios on the adsorption oxidative performance of Cu_(30)/HZSM-5–85 adsorbents was investigated.According to the performance test results,Cu_(30)/HZSM-5–85 exhibited the highest breakthrough capacity,reaching 231.75 mg H_(2)S/g_(sorbent).Cu/HZSM-5 sorbent maintains a strong ability to remove H_(2)S even under humid conditions and shows excellent water resistance.XRD,BET,and XPS results revealed that CuO is the primary active species,with Cu_(30)/HZSM-5–85 having the largest surface area and highest CuO content,providing more active sites for H_(2)S adsorption.H_(2)-TPR and O_(2)-TPD results confirmed that Cu_(30)/HZSM-5–85 sorbent exhibits outstanding redox properties and oxygen storage capacity,contributing to excellent oxygen transferability in the molecular sieve adsorption-oxidation process.With notable characteristics such as a large surface area,high desulfurization efficiency,and water resistance,Cu_(30)/HZSM-5–85 sorbents hold significant importance for industrial applications.展开更多
In this study,non-thermal plasma(NTP)was employed to modify the Cu/TiO_(2)adsorbent to efficiently purify H_(2)S in low-temperature and micro-oxygen environments.The effects of Cu loading amounts and atmospheres of NT...In this study,non-thermal plasma(NTP)was employed to modify the Cu/TiO_(2)adsorbent to efficiently purify H_(2)S in low-temperature and micro-oxygen environments.The effects of Cu loading amounts and atmospheres of NTP treatment on the adsorption-oxidation performance of the adsorbents were investigated.The NTP modification successfully boosted the H_(2)S removal capacity to varying degrees,and the optimized adsorbent treated by air plasma(Cu/TiO_(2)-Air)attained the best H_(2)S breakthrough capacity of 113.29 mg H_(2)S/gadsorbent,which was almost 5 times higher than that of the adsorbent without NTP modification.Further studies demonstrated that the superior performance of Cu/TiO_(2)-Air was attributed to increased mesoporous volume,more exposure of active sites(CuO)and functional groups(amino groups and hydroxyl groups),enhanced Ti-O-Cu interaction,and the favorable ratio of active oxygen species.Additionally,the X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS)results indicated the main reason for the deactivationwas the consumption of the active components(CuO)and the agglomeration of reaction products(CuS and SO_(4)^(2−))occupying the active sites on the surface and the inner pores of the adsorbents.展开更多
Biomass burning(BB)emits carbonaceous aerosols that significantly influence air quality in Southwest China during spring.To further understand the characteristics of spring BB and its original contribution to organic ...Biomass burning(BB)emits carbonaceous aerosols that significantly influence air quality in Southwest China during spring.To further understand the characteristics of spring BB and its original contribution to organic carbon(OC),daily fine particulate matter(PM_(2.5))samples were collected from March to May 2022 in Pu'er,Southwest China.The concentrations of OC,elemental carbon(EC),levoglucosan(Lev),and potassium from BB(K+BB)during the study period ranged from 5.3 to 31.2μg/m^(3),0.86-13.1μg/m^(3),0.06-0.82μg/m^(3),and 0.05-2.88μg/m^(3),respectively.To eliminate the effects of Lev degradation,this study uses the Aging of Air Mass(AAM)index to correct the atmospheric concentration of Lev and combines Bayesian mixture modeling with a molecular tracer method to assess the original contribution of BB to OC.The results indicated that the AAM index was 0.18±0.05,indicating that the degradation of Lev reached 82%.When considering the degradation of levoglucosan in the atmosphere,the primary source of BB aerosols was crop-straw combustion(71.1%),followed by the combustion of certain hardwoods and softwoods(24.9%)and grasses(4.0%).The original contribution of BB to OC was 62.4%,which was much greater than the contribution when levoglucosan degradation(23.7%)was ignored.The air mass inverse trajectories and Moderate Resolution Imaging Spectroradiometer(MODIS)fire hotspots indicated that the BB plume from Southeast Asia during spring could influence PM_(2.5)long-range transport in remote locations,and the contribution could reach 82%in Southwest China.展开更多
Large-scale damming has emerged as a prevalent global trend,significantly impacting nutrient transport and transformation,as well as the downstream ecological environment.Nitrogen and phosphorus are fundamental elemen...Large-scale damming has emerged as a prevalent global trend,significantly impacting nutrient transport and transformation,as well as the downstream ecological environment.Nitrogen and phosphorus are fundamental elements of primary productivity in aquatic ecosystems and serve as key limiting factors in reservoir eutrophication.This review focuses on the impact of damming on the transport and transformation of nitrogen and phosphorus,regarding changes in nutrient concentrations,fluxes,and proportions.Spatial changes in nitrogen and phosphorus concentrations primarily occur at the inlet and outlet of reservoirs,while temporal changes often exhibit seasonal patterns.At a global scale,phosphorus is preferentially removed from reservoirs compared to nitrogen.The factors influencing the transport and transformation processes of nitrogen and phosphorus in reservoirs include the physicochemical properties of water bodies and human activities.Additionally,nitrogen dynamics are affected by reservoir age,storage capacity,and water storage regulation modes,whereas phosphorus dynamics are also influenced by hydrodynamic conditions.Finally,this review summarizes the impact of damming on the downstream ecological environment and outlines future research directions,providing theoretical support for the management of river–reservoir ecosystems and promoting the green and sustainable development of hydropower in the context of carbon peaking and carbon neutrality goals.展开更多
Sand rice(Agriophyllum squarrosum),a pioneering annual plant thriving in deserts and sandy regions throughout the Asian interior,is believed to be a potential food and forage crop due to its significant nutritional an...Sand rice(Agriophyllum squarrosum),a pioneering annual plant thriving in deserts and sandy regions throughout the Asian interior,is believed to be a potential food and forage crop due to its significant nutritional and medicinal values.Previous metabolomics analyses have revealed that sand rice contains abundant flavonoid components,which are known for their wide applications in cosmetics,food,and pharmaceuticals.To optimize the use of flavonoids in sand rice,in this study,the response surface methodology(RSM)was selected to determine the optimal ultrasonic-assisted extraction(UAE)criteria for flavonoids extraction from the aerial part of sand rice firstly.Statistical analyses unveiled the optimum parameters for flavonoids extraction fromsand rice could be 62%of ethanol concentration,1:43 solid-toliquid ratio,160Wfor ultrasound power,and 52℃for extraction temperature with extraction time of 12 min.Under this condition,the experiment optimumtotal flavonoid yield could reach at 15.24 mg/g,which was correspond to the maximum predicted value of RSM with 15.22 mg/g.Subsequently,the antifungal efficacy of these extracts was evaluated against three common plant pathogenic fungi,showing a significant inhibitory effect with the highest rate of inhibition reaching 25.3%at a concentration of 4 mg/mL,underscoring its potential as a natural antimicrobial agent.This studywill not only provide a powerful method to extract flavonoids froma desert resource plant,but also pave the way for industrial development and application of the promising desert plants with high nutritional and medicinal values.展开更多
An in-depth mechanism in zonal activation of CO_(2)and H2molecular over dual-active sites has not been revealed yet.Here,Ni-Co-MgO was rationally constructed to elucidate the CO_(2)methanation mechanism.The abundant s...An in-depth mechanism in zonal activation of CO_(2)and H2molecular over dual-active sites has not been revealed yet.Here,Ni-Co-MgO was rationally constructed to elucidate the CO_(2)methanation mechanism.The abundant surface nickel and cobalt components as active sites led to strong Ni-Co interaction with charge transfer from nickel to cobalt.Notably,electron-enriched Coδ-species participated in efficient chemisorption and activation of CO_(2)to generate monodentate carbonate.Simultaneously,plentiful available Ni0sites facilitated H2dissociation,thus CO_(2)and H2were smoothly activated at zones of Coδ-species and Ni0,respectively.Detailed in situ DRIFTS,quasi situ XPS,TPSR,and DFT calculations substantiated a new formate evolution mechanism via monodentate carbonate instead of traditional bidentate carbonate based on synergistic catalysis of Coδ-species and Ni0.The zonal activation of CO_(2)and H2by tuning electron behaviors of double-center catalysts can boost heterogeneous catalytic hydrogenation performance.展开更多
Dissolved organic matter(DOM)and iron minerals widely existing in the natural aquatic environment can mediate the migration and transformation of organic pollutants.However,the mechanism of interaction between DOM and...Dissolved organic matter(DOM)and iron minerals widely existing in the natural aquatic environment can mediate the migration and transformation of organic pollutants.However,the mechanism of interaction between DOM and iron minerals in the microbial degradation of pollutants deserves further investigation.In this study,the mechanism of 17 alphaethinylestradiol(EE2)biodegradation mediated by humic acid(HA)and three kinds of iron minerals(goethite,magnetite,and pyrite)was investigated.The results found that HA and iron minerals significantly accelerated the biodegradation process of EE2,and the highest degradation efficiency of EE2(48%)was observed in the HA-mediated microbial system with pyrite under aerobic conditions.Furthermore,it had been demonstrated that hydroxyl radicals(HO·)was the main active substance responsible for the microbial degradation of EE2.HO·is primarily generated through the reaction between hydrogen peroxide secreted by microorganisms and Fe(II),with aerobic conditions being more conducive.The presence of iron minerals and HA could change the microbial communities in the EE2 biodegradation system.These findings provide new information for exploring the migration and transformation of pollutants by microorganisms in iron-rich environments.展开更多
Phosphate ions promoted Cu-SAPO-34(P-Cu-SAPO-34)were prepared using bulk CuO particles as Cu^(2+)precursor by a solid-state ion exchange technique for the selective catalytic reduction of NO_(x) with NH_3(NH_3-SCR).Th...Phosphate ions promoted Cu-SAPO-34(P-Cu-SAPO-34)were prepared using bulk CuO particles as Cu^(2+)precursor by a solid-state ion exchange technique for the selective catalytic reduction of NO_(x) with NH_3(NH_3-SCR).The effects of high temperature(H-T)hydrothermal aging on the NO_(x) removal(de-NO_(x))performance of Cu-SAPO-34 with and without phosphate ions were systematically investigated at atomic level.The results displayed that both Cu-SAPO-34 and P-Cu-SAPO-34 presented relatively poor NO_(x) removal activity with a low conversion(<30%)at 250-500℃.However,after H-T hydrothermal treatment(800℃ for 10 hr at 10%H_2O),these two samples showed significantly satisfied NO_(x) elimination performance with a quite high conversion(70%-90%)at 250-500℃.Additionally,phosphate ions decoration can further enhance the catalytic performance of Cu-SAPO-34 after hydrothermal treatment(Cu-SAPO-34H).The textural properties,morphologies,structural feature,acidity,redox characteristic,and surface-active species of the fresh and hydrothermally aged samples were analyzed using various characterization methods.The systematical characterization results revealed that increases of 28%of the isolated Cu^(2+)active species(Cu^(2+)-2Z,Cu(OH)^(+)-Z)mainly from bulk CuO and 50%of the Bronsted acid sites,the high dispersion of isolated Cu^(2+)active component as well as the Bronsted acid sites were mainly responsible for the accepted catalytic activity of these two hydrothermally aged samples,especially for P-Cu-SAPO-34H.展开更多
To investigate the enhancing effect of Mn on the performance of simultaneous catalytic oxidation of AsH_(3)and PH_(3)by CuO-Al_(2)O_(3)in a reducing atmosphere under micro-oxygen conditions,Cu-Mn modifiedγ-Al_(2)O_(3...To investigate the enhancing effect of Mn on the performance of simultaneous catalytic oxidation of AsH_(3)and PH_(3)by CuO-Al_(2)O_(3)in a reducing atmosphere under micro-oxygen conditions,Cu-Mn modifiedγ-Al_(2)O_(3)catalysts were prepared.The characteristics of the catalysts showed that Mn reduced the crystallinity of the active CuO component,increased the number of oxygen vacancies and acidic sites on the catalyst surface,enhanced the mobility of surface oxygen,and the interaction between copper and manganese promoted the redox cycling ability of the catalysts and improved their oxidation performance,which increased the conversion frequency(TOF)by 2.54×10^(-2)to 3.07×10^(-2)sec^(-1).On the other hand,the introduction of Mn reduced the production of phosphate and As_(2)O_(3)on the catalyst surface by30.96%and 44.9%,which reduced the coverage and inerting of the active sites by phosphate and As_(2)O_(3),resulting in an 8 hr(6 hr)improvement in the stability of PH_(3)(AsH_(3))removal.展开更多
Waste calcium carbide slags(CS),which are widely applied to desulfurisation,are not typically used in denitration.Herein,to well achieve waste control by waste,a facile and highefficiency denitration strategy is devel...Waste calcium carbide slags(CS),which are widely applied to desulfurisation,are not typically used in denitration.Herein,to well achieve waste control by waste,a facile and highefficiency denitration strategy is developed using KOH to modify the calcium carbide slags(KCS).Various KCS samples were investigated using a series of physical and chemical characterisations.The performance test results showed that the KOH concentration and reaction temperature are the main factors affecting the denitration efficiency of KCS,and CS modified with 1.5 mol/L KOH(KCS-1.5)can achieve 100% denitration efficiency at 300℃.Such excellent removal efficiency is due to the catalytic oxidation of the oxygen-containing functional groups derived from the KCS.Further studies showed that KOH treatment significantly increased the concentration of oxygen vacancies,nitro compounds,and basic sites of CS.This study provides a novel strategy for the resource utilisation of waste CS in the future.展开更多
NH_(3) in ambient air directly leads to an increase in the aerosol content in the air. These substances lead to the formation of haze to various environmental problems after atmospheric circulation and diffusion. Cont...NH_(3) in ambient air directly leads to an increase in the aerosol content in the air. These substances lead to the formation of haze to various environmental problems after atmospheric circulation and diffusion. Controlling NH_(3) emissions caused by ammonia escaping from mobile and industrial sources can effectively reduce the NH_(3) content in ambient air. Among the various NH_(3) removal methods, the selective catalytic oxygen method (NH_(3)-SCO) is committed to oxidizing NH_(3) to environmentally harmless H_(2)O and N_(2);therefore, it is the most valuable and ideal ammonia removal method. In this review, the characteristics of loaded and core-shell catalysts in NH_(3)-SCO have been reviewed in the context of catalyst structure-activity relationships, and the H_(2)O resistance and SO2 resistance of the catalysts are discussed in the context of practical application conditions. Then the effects of the valence state of the active center, oxygen species on the catalyst surface, dispersion of the active center and acidic sites on the catalyst performance are discussed comprehensively. Finally, the shortcomings of the existing catalysts are summarized and the catalyst development is discussed based on the existing studies.展开更多
The application of metalDorganic frameworks(MOFs)is hindered by several crucial factors,including low photocatalytic efficiency,poor stability and challenges in recycling.In this study,MIL-53(Fe)was grown in situ on a...The application of metalDorganic frameworks(MOFs)is hindered by several crucial factors,including low photocatalytic efficiency,poor stability and challenges in recycling.In this study,MIL-53(Fe)was grown in situ on a charcoal sponge(CS)with a large surface area,excellent mechanical properties,and high photocatalytic efficiency using a solvothermal method,thus addressing the above-mentioned shortcomings of MOF materials.Notably,CS/MIL-53(Fe)has an amazing light-harvesting capacity in the visible range,leading to a significant improvement in the utilization of light.The results of the experiments indicate that CS/MIL-53(Fe)displays a higher photocatalytic activity(87%Cr(Ⅵ))when exposed to visible light than CS(58%)or MIL-53(Fe)(27%),attributing to the increased separation of photogenerated carriers.e-is the main reactive radical and dominates the photocatalytic reduction process,rooting from that e-can reduce Cr(Ⅵ)to low-toxicity Cr(Ⅲ).This study presents a novel method for constructing photocatalysts with large surface areas,superior mechanical characteristics,and enhanced photocatalytic performance.Additionally,it achieves the resource utilization of agricultural and forestry waste.展开更多
基金supported by National Natural Science Foundation of China(Grant No.52270106 and 22266021)Yunnan Major Scientific and Technological Projects(grant No.202202AG050005)Yunnan Fundamental Research Projects(grant No.202201AT070116).
文摘The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner.In this review,we investigate the development of industrialwaste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste.We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification,in which the active components,pore size,and phase structure can be altered.The review will discuss the potential of using industrial solid wastes,these modified materials,or synthesized materials from raw waste precursors for the removal of air pollutants,including SO_(2),NO_(x),Hg^(0),H_(2)S,VOCs,and CO_(2).The challenges still need to be addressed to realize this potential and the prospects for future research fully.The suggestions for future directions include determining the optimal composition of these materials,calculating the real reaction rate and turnover frequency,developing effective treatment methods,and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.
基金supported by the Key Program of the National Natural Science Foundation of China(Grant No.92047201)the Fundamental Research Funds for the Central Universities(Grant No.B230201026)+1 种基金the National Natural Science Foundation of China(Grants No.42377054 and 42007149)the Open Project of Jiangsu Key Laboratory for Eco-Agricultural Biotechnology around Hongze Lake(Grant No.HZHLAB2301).
文摘Reservoirs play a critical role in addressing water resources challenges.However,their vertical influence on the assembly mechanisms of different microbial communities,including prokaryotes and eukaryotes,remains unclear.This study examined the vertical diversity patterns of abundant and rare subcommunities of prokaryotes and eukaryotes in an urban reservoir,using water depth as a geographical gradient and employing high-throughput sequencing.The impact of vertical environmental heterogeneity on community structure was quantified,and key drivers of these dynamics were identified.The results indicated that the urban reservoir exhibited statistically significant differences in the vertical distribution of water temperature and oxidation/reduction potential.The a-diversity of the abundant subcommunity displayed an opposing vertical pattern compared to that of the rare subcommunity,while the b-diversity for both subcommunities of prokaryotes and eukaryotes increased with water depth.Moreover,the distinct diversity patterns of abundant and rare subcommunities were associated with environmental heterogeneity and species adaptability.Notably,the b-diversity of the rare subcommunity of eukaryotes was primarily driven by species turnover in surface water,whereas nestedness became the dominant factor in deeper water.Furthermore,eukaryotic microbes exhibited a more pronounced response to changes in water depth than prokaryotes,consistent with the importance of heterogeneous selection to the eukaryotic community.Water temperature significantly affected the community composition of all groups,highlighting its importance in shaping community dynamics.This study provides valuable insights into the vertical distribution and assembly mechanisms of microbial communities in urban reservoirs,contributing to the protection and management of aquatic ecosystems under river regulation.
基金supported by the National Natural Science Foundation of China(No.52060011).
文摘Enhancing soil organic matter characteristics,ameliorating physical structure,mitigating heavy metal toxicity,and hastening mineral weathering processes are crucial approaches to accomplish the transition of tailings substrate to a soil-like substrate.The incorporation of biomass co-pyrolysis and plant colonization has been established to be a significant factor in soil substrate formation and soil pollutant remediation.Despite this,there is presently an absence of research efforts aimed at synergistically utilizing these two technologies to expedite the process of mining tailings soil substrate formation.The current study aimed to investigate the underlying mechanism of geochemical changes and rapid mineral weathering during the process of transforming tailings substrate into a soil-like substrate,under the combined effects of biomass co-smoldering pyrolysis and plant colonization.The findings of this study suggest that the incorporation of smoldering pyrolysis and plant colonization induces a high-temperature effect and biological effects,which enhance the physical and chemical properties of tailings,while simultaneously accelerating the rate of mineral weathering.Notable improvements include the amelioration of extreme pH levels,nutrient enrichment,the formation of aggregates,and an increase in enzyme activity,all of which collectively demonstrate the successful attainment of tailings substrate reconstruction.Evidence of the acceleratedweathering was verified by phase and surfacemorphology analysis using X-ray diffraction and scanning electron microscopy.Discovered corrosion and fragmentation on the surface ofminerals.The weathering resulted in corrosion and fragmentation of the surface of the treated mineral.This study confirms that co-smoldering pyrolysis of biomass,combined with plant colonization,can effectively promote the transformation of tailings into soil-like substrates.This method has can effectively address the key challenges that have previously hindered sustainable development of the mining industry and provides a novel approach for ecological restoration of tailings deposits.
文摘Objective Recent studies have highlighted the critical role of NUDT19 in the initiation,progression,and prognosis of specific cancer types.However,its involvement in pan-cancer analysis has not been fully characterized.This study aims to systematically explore the expression patterns,clinical significance,and immune-related functions of NUDT19 in various cancer types through multi-omics analysis,further revealing its potential role in cancer,particularly its functional and therapeutic target value in leukemia.Methods To achieve this goal,various bioinformatics approaches were employed to evaluate the expression patterns,clinical significance,and immune-related functions of NUDT19 in tumors and normal tissues.Additionally,we analyzed the mutation characteristics of NUDT19 and its relationship with epigenetic modifications.Using the single-cell analysis tool SingleCellBase,we explored the distribution of NUDT19 across different cell subpopulations in tumors.To validate these findings,qRT-PCR was used to measure NUDT19 expression levels in specific tumor cell lines,and we established acute myeloid leukemia(AML)cell lines(HL-60 and THP-1)to conduct NUDT19 knockdown and overexpression experiments,assessing its effects on leukemia cell proliferation,apoptosis,and invasion.Results Pan-cancer analysis revealed the dysregulated expression of NUDT19 across multiple cancer types,which was closely associated with poor prognosis,clinical staging,and diagnostic markers.Furthermore,NUDT19 was significantly correlated with tumor biomarkers,immune-related genes,and immune cell infiltration in different cancers.Mutation analysis showed that multiple mutations in NUDT19 were significantly associated with epigenetic changes.Single-cell analysis revealed the heterogeneity of NUDT19 expression in cancer cells,suggesting its potentially diverse functional roles in different cell subpopulations.qRT-PCR experiments confirmed the significant upregulation of NUDT19 in various tumor cell lines.In AML cell lines,NUDT19 knockdown led to reduced cell proliferation and invasion,with increased apoptosis,while NUDT19 overexpression significantly enhanced cell proliferation and invasion while reducing apoptosis.Conclusion This study demonstrates the diverse roles of NUDT19 in various cancer types,with a particularly prominent functional role in leukemia.NUDT19 is not only associated with tumor initiation and progression but may also influence cancer progression through the regulation of immune microenvironment and epigenetic mechanisms.Our research highlights the potential of NUDT19 as a therapeutic target,particularly for targeted therapies in malignancies such as leukemia,with significant clinical application prospects.
基金supported by the National Natural Science Foundation of China(No.52370113)Yunnan Fundamental Research Projects(No.202101BE070001-001)。
文摘Metal nanoparticle(NP_S)catalysts exhibit desirable activities in various catalytic reactions.However,the sintering of metal NPs at high-temperatures even in reducing atmospheres limits its practical application.In this work,we successfully synthesized TPA-ZSM-5 with pit-type defects by treating the ZSM-5 with tetrahydroxy ammonium hydroxide(TPAOH),which was then used as a support to prepare Ag-based and Cu-based catalysts.Stability testing results show that the Ag/TPA-ZSM-5 catalyst treated at 800℃with H_(2) could maintain the high performance in NH_(3)-SCO and the Cu/TPA-ZSM-5 catalyst treated at 900℃ with N_(2) could maintained its excellent activity in NH_(3)-SCR,however,the activities of Ag/ZSM-5 and Cu/ZSM-5 were drastically decreased or even deactivated after high-temperature treatment.In addition,a series of characterization analyses revealed that the excellent thermal stability is attribute to the presence of pit-type defects in the TPA-ZSM-5 as physical barriers to slow down or even inhibit the Ag NPs and Cu NPs sintering process.The strategy of using the pit-type defects to inhibit the sintering of metal NPs and improve the thermal stability can greatly enhance the practical application of catalysts.
基金supported by the National Natural Science Foundation of China(No.52260013)Yunnan Major Scientific and Technological Projects(No.202202AG050005).
文摘To improve the activity of Co/Al_(2)O_(3)catalysts in selective catalytic oxidation of ammonia(NH_(3)-SCO),valence state and size of active centers of Al_(2)O_(3)-supported Co catalysts were adjusted by conducting H_(2)reduction pretreatment.The NH_(3)-SCO activity of the adjusted 2Co/Al_(2)O_(3)catalyst was substantially improved,outperforming other catalysts with higher Co-loading.Fresh Co/Al_(2)O_(3)catalysts exhibited multitemperature reduction processes,enabling the control of the valence state of the Co-active centers by adjusting the reduction temperature.Changes in the state of the Co-active centers also led to differences in redox capacity of the catalysts,resulting in different reaction mechanisms for NH_(3)-SCO.However,in situ diffuse reflectance infrared Fourier transform spectra revealed that an excessive O_(2)activation capacity caused overoxidation of NH_(3)to NO and NO_(2).The NH_(3)-SCO activity of the 2Co/Al_(2)O_(3)catalyst with low redox capacity was successfully increased while controlling and optimizing the N_(2)selectivity by modulating the active centers via H_(2)pretreatment,which is a universalmethod used for enhancing the redox properties of catalysts.Thus,this method has great potential for application in the design of inexpensive and highly active catalysts.
基金financial support from the National Natural Science Foundation of China(Grant NO.22466023,52470119,52260013)the Applied Basic Research Foundation of Yunnan Province(Grant NO.202401AT070408)+1 种基金Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials(Grant NO.202205AG070067)Yunnan Technological Innovation Center of Phosphorus Resources(Grant NO.202305AK340002)。
文摘In this study,a novel Pt-loaded Cu Pc/g-C_(3)N_(4)(Pt Cu CN)composite was synthesized for the selective photocatalytic reduction of CO_(2)to CH_(4)under visible light.The Pt Cu CN catalyst achieved a CH_(4)yield of 39.8μmol g^(-1)h^(-1),significantly outperforming bulk g-C_(3)N_(4)and Cu Pc alone by factors of 2.5 and 3.1,respectively,with a high selectivity of 90%.In comparison with other commonly studied photocatalysts,such as g-C_(3)N_(4)-based catalysts,the Pt Cu CN composite exhibited superior CH_(4)yield and product selectivity,demonstrating its potential as a more efficient photocatalyst for CO_(2)reduction.X-ray photoelectron spectroscopy(XPS),density functional theory(DFT)calculations,and in-situ infrared(IR)analysis revealed that the Pt^(0)species effectively lower the activation energy for CH_(4)formation,while Cu Pc extends the light absorption range and enhances charge separation.The combined effects of these components in a Z-scheme heterojunction provide new insights into designing highly selective CO_(2)-to-CH_(4)photocatalysts.This work demonstrates the potential of Pt Cu CN as a highly efficient and stable catalyst for CO_(2)reduction to CH_(4)under visible light.
基金supported by Yunnan Major Scientific and Technological Projects(No.202202AG050005)Yunnan Fundamental Research Projects(No.202101BE070001-001).
文摘The ACF adsorbent with high Cu loading was treated with dielectric barrier discharge plasma to mitigate the negative effects of high Cu loading and enhance PH_(3)and H_(2)S adsorption and oxidation.Bruno-Emmett-Taylor(BET)result showed that the specific surface area of the adsorbent after air plasma modification was almost three times that before modification.X-ray photoelectron spectroscopy(XPS)findings revealed that the amino group was added to the adsorbent's surface,increasing lattice oxygen and chemisorbed oxygen.The adsorbent's large specific surface area,excellent surface active oxygen,and abundance of basic groups facilitate PH_(3)and H_(2)S adsorption and oxidation.The scanning electron microscopy showed that air plasma modification exposed more active components and uniformly dispersed them on the surface of adsorbent,thereby improving the adsorption performance.Activity evaluation results showed that the adsorbent has the best ability to capture PH_(3)and H_(2)S after being modified by air plasma at 4 kV voltage for 10 min.The adsorbent's breakthrough ability at high space velocity(WHSV:60,000 h^(−1))is 190 mg P/g and 146 mg S/g,respectively,which is 74%and 60%greater than that before modification.This is a great improvement over previous studies.In addition,the possible mechanism of adsorbent deactivation was proposed.
基金supported by the National Natural Science Foundation of China(Nos.52270106 and 22266021)Yunnan Major Scientific and Technological Projects(No.202202AG050005)Yunnan Fundamental Research Projects(No.202201AT070116).
文摘This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25,50,85,200,and 300,used for the removal of H_(2)S in lowtemperature,low-oxygen environments.The impact of different Si/Al ratios on the adsorption oxidative performance of Cu_(30)/HZSM-5–85 adsorbents was investigated.According to the performance test results,Cu_(30)/HZSM-5–85 exhibited the highest breakthrough capacity,reaching 231.75 mg H_(2)S/g_(sorbent).Cu/HZSM-5 sorbent maintains a strong ability to remove H_(2)S even under humid conditions and shows excellent water resistance.XRD,BET,and XPS results revealed that CuO is the primary active species,with Cu_(30)/HZSM-5–85 having the largest surface area and highest CuO content,providing more active sites for H_(2)S adsorption.H_(2)-TPR and O_(2)-TPD results confirmed that Cu_(30)/HZSM-5–85 sorbent exhibits outstanding redox properties and oxygen storage capacity,contributing to excellent oxygen transferability in the molecular sieve adsorption-oxidation process.With notable characteristics such as a large surface area,high desulfurization efficiency,and water resistance,Cu_(30)/HZSM-5–85 sorbents hold significant importance for industrial applications.
基金supported by the National Natural Science Foundation of China (Nos.52260013,51968034,and 21876071)the Yunnan Major Scientific and Technological Projects (No.202202AG050005).
文摘In this study,non-thermal plasma(NTP)was employed to modify the Cu/TiO_(2)adsorbent to efficiently purify H_(2)S in low-temperature and micro-oxygen environments.The effects of Cu loading amounts and atmospheres of NTP treatment on the adsorption-oxidation performance of the adsorbents were investigated.The NTP modification successfully boosted the H_(2)S removal capacity to varying degrees,and the optimized adsorbent treated by air plasma(Cu/TiO_(2)-Air)attained the best H_(2)S breakthrough capacity of 113.29 mg H_(2)S/gadsorbent,which was almost 5 times higher than that of the adsorbent without NTP modification.Further studies demonstrated that the superior performance of Cu/TiO_(2)-Air was attributed to increased mesoporous volume,more exposure of active sites(CuO)and functional groups(amino groups and hydroxyl groups),enhanced Ti-O-Cu interaction,and the favorable ratio of active oxygen species.Additionally,the X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS)results indicated the main reason for the deactivationwas the consumption of the active components(CuO)and the agglomeration of reaction products(CuS and SO_(4)^(2−))occupying the active sites on the surface and the inner pores of the adsorbents.
基金supported by the Basic Research Key Project of Science and Technology Department of Yunnan Province(No.202401AS070116)the National Natural Science Foundation of China(No.21966016)。
文摘Biomass burning(BB)emits carbonaceous aerosols that significantly influence air quality in Southwest China during spring.To further understand the characteristics of spring BB and its original contribution to organic carbon(OC),daily fine particulate matter(PM_(2.5))samples were collected from March to May 2022 in Pu'er,Southwest China.The concentrations of OC,elemental carbon(EC),levoglucosan(Lev),and potassium from BB(K+BB)during the study period ranged from 5.3 to 31.2μg/m^(3),0.86-13.1μg/m^(3),0.06-0.82μg/m^(3),and 0.05-2.88μg/m^(3),respectively.To eliminate the effects of Lev degradation,this study uses the Aging of Air Mass(AAM)index to correct the atmospheric concentration of Lev and combines Bayesian mixture modeling with a molecular tracer method to assess the original contribution of BB to OC.The results indicated that the AAM index was 0.18±0.05,indicating that the degradation of Lev reached 82%.When considering the degradation of levoglucosan in the atmosphere,the primary source of BB aerosols was crop-straw combustion(71.1%),followed by the combustion of certain hardwoods and softwoods(24.9%)and grasses(4.0%).The original contribution of BB to OC was 62.4%,which was much greater than the contribution when levoglucosan degradation(23.7%)was ignored.The air mass inverse trajectories and Moderate Resolution Imaging Spectroradiometer(MODIS)fire hotspots indicated that the BB plume from Southeast Asia during spring could influence PM_(2.5)long-range transport in remote locations,and the contribution could reach 82%in Southwest China.
基金supported by the General Project of the National Natural Science Foundation of China(Grant No.42377054)the National Natural Science Fund for Young Scholars(Grant No.42007149)the Key Project of the Major Research Plan of the National Natural Science Foundation of China(Grant No.92047201).
文摘Large-scale damming has emerged as a prevalent global trend,significantly impacting nutrient transport and transformation,as well as the downstream ecological environment.Nitrogen and phosphorus are fundamental elements of primary productivity in aquatic ecosystems and serve as key limiting factors in reservoir eutrophication.This review focuses on the impact of damming on the transport and transformation of nitrogen and phosphorus,regarding changes in nutrient concentrations,fluxes,and proportions.Spatial changes in nitrogen and phosphorus concentrations primarily occur at the inlet and outlet of reservoirs,while temporal changes often exhibit seasonal patterns.At a global scale,phosphorus is preferentially removed from reservoirs compared to nitrogen.The factors influencing the transport and transformation processes of nitrogen and phosphorus in reservoirs include the physicochemical properties of water bodies and human activities.Additionally,nitrogen dynamics are affected by reservoir age,storage capacity,and water storage regulation modes,whereas phosphorus dynamics are also influenced by hydrodynamic conditions.Finally,this review summarizes the impact of damming on the downstream ecological environment and outlines future research directions,providing theoretical support for the management of river–reservoir ecosystems and promoting the green and sustainable development of hydropower in the context of carbon peaking and carbon neutrality goals.
基金support received from the Lanzhou Youth Science and Technology Talent Innovation Project(Grant No.:2023-QN-140)National Natural Science Foundation of China(Grant Nos.:31901079,32171608,32271695 and 32201378)the Chinese Academy of Sciences Strategic Biological Resources Program(Grant No.:KFJ-BRP-007-015).
文摘Sand rice(Agriophyllum squarrosum),a pioneering annual plant thriving in deserts and sandy regions throughout the Asian interior,is believed to be a potential food and forage crop due to its significant nutritional and medicinal values.Previous metabolomics analyses have revealed that sand rice contains abundant flavonoid components,which are known for their wide applications in cosmetics,food,and pharmaceuticals.To optimize the use of flavonoids in sand rice,in this study,the response surface methodology(RSM)was selected to determine the optimal ultrasonic-assisted extraction(UAE)criteria for flavonoids extraction from the aerial part of sand rice firstly.Statistical analyses unveiled the optimum parameters for flavonoids extraction fromsand rice could be 62%of ethanol concentration,1:43 solid-toliquid ratio,160Wfor ultrasound power,and 52℃for extraction temperature with extraction time of 12 min.Under this condition,the experiment optimumtotal flavonoid yield could reach at 15.24 mg/g,which was correspond to the maximum predicted value of RSM with 15.22 mg/g.Subsequently,the antifungal efficacy of these extracts was evaluated against three common plant pathogenic fungi,showing a significant inhibitory effect with the highest rate of inhibition reaching 25.3%at a concentration of 4 mg/mL,underscoring its potential as a natural antimicrobial agent.This studywill not only provide a powerful method to extract flavonoids froma desert resource plant,but also pave the way for industrial development and application of the promising desert plants with high nutritional and medicinal values.
基金funded by the Science and Technology Project of Southwest United Graduate School of Yunnan Province(No.202302AQ370002)the National Natural Science Foundation of China(No.22206066)。
文摘An in-depth mechanism in zonal activation of CO_(2)and H2molecular over dual-active sites has not been revealed yet.Here,Ni-Co-MgO was rationally constructed to elucidate the CO_(2)methanation mechanism.The abundant surface nickel and cobalt components as active sites led to strong Ni-Co interaction with charge transfer from nickel to cobalt.Notably,electron-enriched Coδ-species participated in efficient chemisorption and activation of CO_(2)to generate monodentate carbonate.Simultaneously,plentiful available Ni0sites facilitated H2dissociation,thus CO_(2)and H2were smoothly activated at zones of Coδ-species and Ni0,respectively.Detailed in situ DRIFTS,quasi situ XPS,TPSR,and DFT calculations substantiated a new formate evolution mechanism via monodentate carbonate instead of traditional bidentate carbonate based on synergistic catalysis of Coδ-species and Ni0.The zonal activation of CO_(2)and H2by tuning electron behaviors of double-center catalysts can boost heterogeneous catalytic hydrogenation performance.
基金supported by the National Natural Science Foundation of China(Nos.42207450,21866017,and 42067056)the Yunnan Fundamental Research Projects(No.202101BE070001-013)the Foundation for Distinguished Young Talents of Yunnan Province(No.202101AV070006)。
文摘Dissolved organic matter(DOM)and iron minerals widely existing in the natural aquatic environment can mediate the migration and transformation of organic pollutants.However,the mechanism of interaction between DOM and iron minerals in the microbial degradation of pollutants deserves further investigation.In this study,the mechanism of 17 alphaethinylestradiol(EE2)biodegradation mediated by humic acid(HA)and three kinds of iron minerals(goethite,magnetite,and pyrite)was investigated.The results found that HA and iron minerals significantly accelerated the biodegradation process of EE2,and the highest degradation efficiency of EE2(48%)was observed in the HA-mediated microbial system with pyrite under aerobic conditions.Furthermore,it had been demonstrated that hydroxyl radicals(HO·)was the main active substance responsible for the microbial degradation of EE2.HO·is primarily generated through the reaction between hydrogen peroxide secreted by microorganisms and Fe(II),with aerobic conditions being more conducive.The presence of iron minerals and HA could change the microbial communities in the EE2 biodegradation system.These findings provide new information for exploring the migration and transformation of pollutants by microorganisms in iron-rich environments.
基金supported by the National Natural Science Foundation of China (No.NSFC22166020)。
文摘Phosphate ions promoted Cu-SAPO-34(P-Cu-SAPO-34)were prepared using bulk CuO particles as Cu^(2+)precursor by a solid-state ion exchange technique for the selective catalytic reduction of NO_(x) with NH_3(NH_3-SCR).The effects of high temperature(H-T)hydrothermal aging on the NO_(x) removal(de-NO_(x))performance of Cu-SAPO-34 with and without phosphate ions were systematically investigated at atomic level.The results displayed that both Cu-SAPO-34 and P-Cu-SAPO-34 presented relatively poor NO_(x) removal activity with a low conversion(<30%)at 250-500℃.However,after H-T hydrothermal treatment(800℃ for 10 hr at 10%H_2O),these two samples showed significantly satisfied NO_(x) elimination performance with a quite high conversion(70%-90%)at 250-500℃.Additionally,phosphate ions decoration can further enhance the catalytic performance of Cu-SAPO-34 after hydrothermal treatment(Cu-SAPO-34H).The textural properties,morphologies,structural feature,acidity,redox characteristic,and surface-active species of the fresh and hydrothermally aged samples were analyzed using various characterization methods.The systematical characterization results revealed that increases of 28%of the isolated Cu^(2+)active species(Cu^(2+)-2Z,Cu(OH)^(+)-Z)mainly from bulk CuO and 50%of the Bronsted acid sites,the high dispersion of isolated Cu^(2+)active component as well as the Bronsted acid sites were mainly responsible for the accepted catalytic activity of these two hydrothermally aged samples,especially for P-Cu-SAPO-34H.
基金supported by the National Natural Science Foundation of China (Nos.51868030,52070090,52100122,22266019,and 21876071)the Science and Technology Planning Project of Yunnan Province (Nos.202001AU070031,202101BE070001-030,and 202101BC070001-009)Applied Basic Research Program of Yunnan Province (No.2019FD043)。
文摘To investigate the enhancing effect of Mn on the performance of simultaneous catalytic oxidation of AsH_(3)and PH_(3)by CuO-Al_(2)O_(3)in a reducing atmosphere under micro-oxygen conditions,Cu-Mn modifiedγ-Al_(2)O_(3)catalysts were prepared.The characteristics of the catalysts showed that Mn reduced the crystallinity of the active CuO component,increased the number of oxygen vacancies and acidic sites on the catalyst surface,enhanced the mobility of surface oxygen,and the interaction between copper and manganese promoted the redox cycling ability of the catalysts and improved their oxidation performance,which increased the conversion frequency(TOF)by 2.54×10^(-2)to 3.07×10^(-2)sec^(-1).On the other hand,the introduction of Mn reduced the production of phosphate and As_(2)O_(3)on the catalyst surface by30.96%and 44.9%,which reduced the coverage and inerting of the active sites by phosphate and As_(2)O_(3),resulting in an 8 hr(6 hr)improvement in the stability of PH_(3)(AsH_(3))removal.
基金supported by the National Natural Science Foundation of China(No.51968075)the Scientific Research Fund project of Yunnan Education Department(Nos.2022J0441 and 2022J0442)。
文摘Waste calcium carbide slags(CS),which are widely applied to desulfurisation,are not typically used in denitration.Herein,to well achieve waste control by waste,a facile and highefficiency denitration strategy is developed using KOH to modify the calcium carbide slags(KCS).Various KCS samples were investigated using a series of physical and chemical characterisations.The performance test results showed that the KOH concentration and reaction temperature are the main factors affecting the denitration efficiency of KCS,and CS modified with 1.5 mol/L KOH(KCS-1.5)can achieve 100% denitration efficiency at 300℃.Such excellent removal efficiency is due to the catalytic oxidation of the oxygen-containing functional groups derived from the KCS.Further studies showed that KOH treatment significantly increased the concentration of oxygen vacancies,nitro compounds,and basic sites of CS.This study provides a novel strategy for the resource utilisation of waste CS in the future.
基金the National Natural Science Foundation of China(No.52000093)Yunnan Fundamental Research Projects(No.202101BE070001-001)National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019B03).
文摘NH_(3) in ambient air directly leads to an increase in the aerosol content in the air. These substances lead to the formation of haze to various environmental problems after atmospheric circulation and diffusion. Controlling NH_(3) emissions caused by ammonia escaping from mobile and industrial sources can effectively reduce the NH_(3) content in ambient air. Among the various NH_(3) removal methods, the selective catalytic oxygen method (NH_(3)-SCO) is committed to oxidizing NH_(3) to environmentally harmless H_(2)O and N_(2);therefore, it is the most valuable and ideal ammonia removal method. In this review, the characteristics of loaded and core-shell catalysts in NH_(3)-SCO have been reviewed in the context of catalyst structure-activity relationships, and the H_(2)O resistance and SO2 resistance of the catalysts are discussed in the context of practical application conditions. Then the effects of the valence state of the active center, oxygen species on the catalyst surface, dispersion of the active center and acidic sites on the catalyst performance are discussed comprehensively. Finally, the shortcomings of the existing catalysts are summarized and the catalyst development is discussed based on the existing studies.
基金supported by the Key Technologies of Carbonization and Sustainable Utilization of Urban Perishable Waste Driven by Data and Knowledge(No.2022YFE0196000)Zhejiang Province“Three Rural Nine”Science and Technology Cooperation Plan Unveiled the Project(No.2023SNJF075)+2 种基金the National Natural Science Foundation of China(Nos.22006135 and 22201251)Major Projects for Science and Technology Development of Zhejiang Province(No.2020C01017)the Basic Research Expenses of Zhejiang University of Science and Technology(No.XJ2023004901)。
文摘The application of metalDorganic frameworks(MOFs)is hindered by several crucial factors,including low photocatalytic efficiency,poor stability and challenges in recycling.In this study,MIL-53(Fe)was grown in situ on a charcoal sponge(CS)with a large surface area,excellent mechanical properties,and high photocatalytic efficiency using a solvothermal method,thus addressing the above-mentioned shortcomings of MOF materials.Notably,CS/MIL-53(Fe)has an amazing light-harvesting capacity in the visible range,leading to a significant improvement in the utilization of light.The results of the experiments indicate that CS/MIL-53(Fe)displays a higher photocatalytic activity(87%Cr(Ⅵ))when exposed to visible light than CS(58%)or MIL-53(Fe)(27%),attributing to the increased separation of photogenerated carriers.e-is the main reactive radical and dominates the photocatalytic reduction process,rooting from that e-can reduce Cr(Ⅵ)to low-toxicity Cr(Ⅲ).This study presents a novel method for constructing photocatalysts with large surface areas,superior mechanical characteristics,and enhanced photocatalytic performance.Additionally,it achieves the resource utilization of agricultural and forestry waste.
