The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorp...The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorption temperature,adsorption time and adsorbent dosage on their adsorptive denitrification performance were systematically investigated.The experimental results demonstrated that under a fixed adsorbent dosage of 0.05 g and a simulated fuel volume of 10 mL,the optimal removal efficiency for aniline was achieved at 30℃ within 30 min,whereas higher temperatures and longer times(40℃and 40 min)were required for effective removal of pyridine and quinoline.Density Functional Theory(DFT)calculations were conducted via Materials Studio(MS)software to study the adsorptive denitrification mechanism of MIL-101(Cr)toward these three basic nitrogen-containing compounds.The simulation calculation results revealed that the interaction between pyridine and MIL-101(Cr)primarily involved coordination adsorption.In contrast,the interaction between aniline or quinoline and MIL-101(Cr)proceeded mainly through coordination,with additional contributions fromπ-complexation and hydrogen bonding.The overall adsorption strength order is pyridine>aniline>quinoline.During the adsorption process,pyridine and quinoline transfer electrons to the MIL-101(Cr)surface through the H→C→N→Cr^(3+)pathway,while aniline transfers electrons to the MIL-101(Cr)surface through various pathways,including N→Cr^(3+),N→C→Cr^(3+)and N→H→O.Furthermore,adsorption kinetics studies indicated that the adsorption processes for all three basic nitrogen-containing compounds followed the quasi second order kinetic models.The experimental results on the effect of benzene on the adsorptive denitrification performance of MIL-101(Cr)-0.5 demonstrated that benzene exerted a more significant impact on the adsorption of aniline and quinoline.Finally,the adsorbent was regenerated using ethanol washing.It was found that MIL-101(Cr)-0.5 retained stable denitrification performance after two regeneration cycles.展开更多
To identify the root causes of heavy metal contamination in soils as well as prevent and control such contamination from its sources,this study explored the accumulation patterns and ecological risks of heavy metals l...To identify the root causes of heavy metal contamination in soils as well as prevent and control such contamination from its sources,this study explored the accumulation patterns and ecological risks of heavy metals like Cd and Pb in solid waste in mining areas and across the water body,sediment,soil and agricultural product ecosystem surrounding the mining areas.Focusing on the residual solid waste samples in lead-zinc deposits in a certain area of Guizhou Province,along with samples of topsoils,irrigation water,river sediments,and crops from surrounding areas.This study analyzed the distributions of eight heavy metals,i.e.,Cd,As,Cr,Hg,Pb,Zn,Cu,and Ni,in the samples through field surveys and sample tests.Furthermore,this study assessed the contamination levels and ecological risks of heavy metals in soils,sediments,and agricultural products using methods such as the single-factor index,Nemerow composite index,and potential ecological risk assessment.The results indicate that heavy metals in the solid waste samples all exhibited concentrations exceeding their risk screening values,with 60%greater than their risk intervention values.The soils and sediments demonstrate slight and moderate comprehensive ecological risks of heavy metals.The single-factor potential ecological risks of heavy metals in both the soil and sediment samples decreased in the order of Hg,Cd,Pb,As,Cu,Zn,Cr,and Ni,suggesting the same sources of heavy metals in the soils and sediments.Most of the agricultural product samples exhibited over-limit concentrations of heavy metals dominated by Cd,Pb,Ni,and Cr,excluding Hg and As.The agricultural product assessment using the Nemerow composite index reveals that 35%of the agricultural product samples reached the heavy metal contamination level,implying that the agricultural products from farmland around the solid waste dumps have been contaminated with heavy metals.The eight heavy metals in the soil,sediment,and agricultural product samples manifested high coefficients of variation(CVs),indicating pronounced spatial variability.This suggests that their concentrations in soils,sediments,and agricultural products are significantly influenced by human mining activities.Additionally,the agricultural products exhibit strong transport and accumulation capacities for Cd,Cu,and Zn.展开更多
基金Supported by Basic Scientific Research Project of the Liaoning Provincial Department of Education Has Been Unveiled to Facilitate Local Project Funding (JYTMS20230835)Enhanced Scientific Research Project Funded by the Departmentof Higher Education in Liaoning Province (General program)(JYTMS20230852)。
文摘The adsorptive denitrification performance of MIL-101(Cr)-0.5 toward pyridine,aniline or quinoline in simulated fuels with basic nitrogen content of 1732μg/g was evaluated separately.Furthermore,the effects of adsorption temperature,adsorption time and adsorbent dosage on their adsorptive denitrification performance were systematically investigated.The experimental results demonstrated that under a fixed adsorbent dosage of 0.05 g and a simulated fuel volume of 10 mL,the optimal removal efficiency for aniline was achieved at 30℃ within 30 min,whereas higher temperatures and longer times(40℃and 40 min)were required for effective removal of pyridine and quinoline.Density Functional Theory(DFT)calculations were conducted via Materials Studio(MS)software to study the adsorptive denitrification mechanism of MIL-101(Cr)toward these three basic nitrogen-containing compounds.The simulation calculation results revealed that the interaction between pyridine and MIL-101(Cr)primarily involved coordination adsorption.In contrast,the interaction between aniline or quinoline and MIL-101(Cr)proceeded mainly through coordination,with additional contributions fromπ-complexation and hydrogen bonding.The overall adsorption strength order is pyridine>aniline>quinoline.During the adsorption process,pyridine and quinoline transfer electrons to the MIL-101(Cr)surface through the H→C→N→Cr^(3+)pathway,while aniline transfers electrons to the MIL-101(Cr)surface through various pathways,including N→Cr^(3+),N→C→Cr^(3+)and N→H→O.Furthermore,adsorption kinetics studies indicated that the adsorption processes for all three basic nitrogen-containing compounds followed the quasi second order kinetic models.The experimental results on the effect of benzene on the adsorptive denitrification performance of MIL-101(Cr)-0.5 demonstrated that benzene exerted a more significant impact on the adsorption of aniline and quinoline.Finally,the adsorbent was regenerated using ethanol washing.It was found that MIL-101(Cr)-0.5 retained stable denitrification performance after two regeneration cycles.
文摘To identify the root causes of heavy metal contamination in soils as well as prevent and control such contamination from its sources,this study explored the accumulation patterns and ecological risks of heavy metals like Cd and Pb in solid waste in mining areas and across the water body,sediment,soil and agricultural product ecosystem surrounding the mining areas.Focusing on the residual solid waste samples in lead-zinc deposits in a certain area of Guizhou Province,along with samples of topsoils,irrigation water,river sediments,and crops from surrounding areas.This study analyzed the distributions of eight heavy metals,i.e.,Cd,As,Cr,Hg,Pb,Zn,Cu,and Ni,in the samples through field surveys and sample tests.Furthermore,this study assessed the contamination levels and ecological risks of heavy metals in soils,sediments,and agricultural products using methods such as the single-factor index,Nemerow composite index,and potential ecological risk assessment.The results indicate that heavy metals in the solid waste samples all exhibited concentrations exceeding their risk screening values,with 60%greater than their risk intervention values.The soils and sediments demonstrate slight and moderate comprehensive ecological risks of heavy metals.The single-factor potential ecological risks of heavy metals in both the soil and sediment samples decreased in the order of Hg,Cd,Pb,As,Cu,Zn,Cr,and Ni,suggesting the same sources of heavy metals in the soils and sediments.Most of the agricultural product samples exhibited over-limit concentrations of heavy metals dominated by Cd,Pb,Ni,and Cr,excluding Hg and As.The agricultural product assessment using the Nemerow composite index reveals that 35%of the agricultural product samples reached the heavy metal contamination level,implying that the agricultural products from farmland around the solid waste dumps have been contaminated with heavy metals.The eight heavy metals in the soil,sediment,and agricultural product samples manifested high coefficients of variation(CVs),indicating pronounced spatial variability.This suggests that their concentrations in soils,sediments,and agricultural products are significantly influenced by human mining activities.Additionally,the agricultural products exhibit strong transport and accumulation capacities for Cd,Cu,and Zn.
