Health-care waste contains potentially harmful microorganisms and compounds which can infect and affect hospital patients, healthcare workers, the general public and environment. Therefore, management of health care w...Health-care waste contains potentially harmful microorganisms and compounds which can infect and affect hospital patients, healthcare workers, the general public and environment. Therefore, management of health care waste requires safe handling, treatment and disposal procedures. While incineration reduces the volume and quantity of waste for final disposal, it leads to the production of fly and bottom ashes laden with toxic incomplete combustion products such as Polycyclic Aromatic Hydrocarbons (PAHs), dioxins, furans and heavy metals. This exposes workers who handle and dispose the bottom ashes, hospital patients, the general public and environment. The goal of this study was to determine the total and individual levels of 16 most prevalent and toxic PAHs. Bottom ash samples were collected from incinerators in five county hospitals in Kenya, namely;Moi-Voi, Narok, Kitale, Makindu and Isiolo. Bottom ash samples were collected over a period of six months from the five hospitals. The samples were then sieved, homogenised and stored at 4°C in amber coloured glass containers. The PAHs were extracted using 30 ml of a hexane-acetone solvent (1:1) mixture by ultrasonication at room temperature (23°C) for 45 minutes. The PAHs were then analyzed with a GC-MS spectrophotometer model (Shimadzu GCMS-QP2010 SE) connected to a computer work station was used for the PAHs analysis. The GC-MS was equipped with an SGE BPX5 GC capillary column (30 m × 0.25 mm × 0.25 μm) for the separation of compounds. Helium was used as the carrier gas at a flow rate of 15.5 ml/minute and 14.5 psi. 1 μl of the sample was injected at 280°C, split mode (10:1). The oven programming was set for a total runtime of 40 minutes, which included: 100°C (2-minute hold);10°C /min rise to 200°C;7°C /min rise to 249°C;3°C /min rise to 300°C (2-minute hold). The interface temperature was set at 290°C. Analysis was done in Selected Ion Monitoring (SIM) mode and the peak areas of each of the PAHs were collected from the chromatograph and used for quantification of the 16 PAHs listed by the U.S. Environmental Protection Agency (EPA) which included, BaA (benz[a]anthracene: 4 rings), BaP (benzo[a]pyrene: 5 rings), BbF (benzo [b]fluoranthene: 5 rings), BkF (benzo[k]fluoranthene: 5 rings), Chr (chrysene: 4 rings), DbA (dibenz[a,h]anthracene: 5 rings), InP (indeno[1,2,3 - cd] pyrene: 6 rings) and Acp (acenaphthene: 3 rings), Acpy (acenaphthylene: 3 rings), Ant (anthracene: 3 rings), BghiP (benzo[g,h,i]perylene: 6 rings), Flu (fluorene: 3 rings), FluA (fluoranthene: 4 rings), Nap (naphthalene: 2 rings), PhA (phenanthrene: 3 rings) and Pyr (pyrene: 4 rings). Ion source-interface temperature was set at 200°C - 250°C. Internal standards from Sigma Aldrich were used in the analysis and the acquired mass spectra data were then matched against the NIST 2014 library [1] [2]. The mean PAHs concentration in the bottom ashes of each hospital varied broadly from 0.001 mg/kg to 0.4845 mg/kg, and the mean total concentration levels of individual PAHs ranged from 0.0072 mg/kg to 1.171 mg/kg. Low molecular weight PAHs (Phenanthrene, Naphthalene and Fluorene) were predominant in all the hospital wastes whereas Kitale and Narok presented the lowest PAHs concentrations and the lowest number of individual PAHs. Moi/Voi recorded the highest total PAHs concentration at 1.3129 ± 0.0023 mg/kg from a total of 11 PAHs being detected from the bottom ash samples. Narok had only three PAHs being detected at very low concentrations of 0.0041 ± 0.00 mg/kg, 0.0076 ± 0.00 mg/kg and 0.012 ± 0.00 mg/kg for phenanthrene, anthracene and chrysene respectively. This study presents hospital incinerator bottom ash as containing detectable levels of both carcinogenic and non-carcinogenic PAHs. Continued unprotected exposure of hospital workers (waste handlers) to the bottom ash PAHs could be hazardous to their health because of their cumulative effect. Preventive measures e.g. the use of Personal protective equipment (PPE) should be prioritised to minimise direct contact with the bottom ash. The study recommends an upgrade on incinerator technology for efficient combustion processes thus for better pollution control.展开更多
Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the...Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.展开更多
The selective hydrogenation of polycyclic aromatic hydrocarbons(PAHs)from fluid catalytic cracking(FCC)slurry extract was conducted in a batch reactor over aγ-Al_(2)O_(3)-supported bimetallic Ni-W catalyst.For the Ni...The selective hydrogenation of polycyclic aromatic hydrocarbons(PAHs)from fluid catalytic cracking(FCC)slurry extract was conducted in a batch reactor over aγ-Al_(2)O_(3)-supported bimetallic Ni-W catalyst.For the Ni-W/γ-Al_(2)O_(3) catalyst,the experiment run was divided into three processes according to the reaction conditions used:(1)the absence of hydrogenation as both temperature and pressure increased;(2)the desulfurization of FCC slurry extract under a fixed pressure as the temperature increased;and(3)the selective hydrogenation of PAHs when both pressure and temperature remained constant.The hydrogen consumption could be accurately calculated from the Redlich–Kwong equation of state.The results for the removal of PAHs with hydrogenation displayed an excellent fit to the first-order kinetics.The apparent activation energy was determined to be 20.80 kJ/mol.展开更多
Levels of Polycyclic aromatic hydrocarbons (PAHs) from sediments collected in July 2017, a week after tanks oil leak in the bay of Wesha Peninsular, Pemba Island are reported. Four sampling points were chosen alongsid...Levels of Polycyclic aromatic hydrocarbons (PAHs) from sediments collected in July 2017, a week after tanks oil leak in the bay of Wesha Peninsular, Pemba Island are reported. Four sampling points were chosen alongside the mangroves where a total of twenty samples were collected during the low tides. Eight PAHs were detected with concentrations ranging from ND to 53.42 ng/g (dw). Total PAHs in sediments was 158.38 ng⋅g<sup>-1</sup>. Phenanthrene residues (lower molecular weight) were dominant followed by pyrene (higher molecular weight PAHs) accounting for 90% and 40% detection frequencies, respectively. Statistical analysis showed no significant difference in the concentrations of PAHs among sites (p < 0.05, ANOVA). Vertical distribution of PAHs shows no definite patterns with sediment depth, however, composition patterns of PAHs along sediment depth indicate that higher molecular weight PAHs tend to remain in middle layer (2 - 4 cm). The results advocate the needs of proper monitoring to avoid the possible consequences to the public health.展开更多
文摘Health-care waste contains potentially harmful microorganisms and compounds which can infect and affect hospital patients, healthcare workers, the general public and environment. Therefore, management of health care waste requires safe handling, treatment and disposal procedures. While incineration reduces the volume and quantity of waste for final disposal, it leads to the production of fly and bottom ashes laden with toxic incomplete combustion products such as Polycyclic Aromatic Hydrocarbons (PAHs), dioxins, furans and heavy metals. This exposes workers who handle and dispose the bottom ashes, hospital patients, the general public and environment. The goal of this study was to determine the total and individual levels of 16 most prevalent and toxic PAHs. Bottom ash samples were collected from incinerators in five county hospitals in Kenya, namely;Moi-Voi, Narok, Kitale, Makindu and Isiolo. Bottom ash samples were collected over a period of six months from the five hospitals. The samples were then sieved, homogenised and stored at 4°C in amber coloured glass containers. The PAHs were extracted using 30 ml of a hexane-acetone solvent (1:1) mixture by ultrasonication at room temperature (23°C) for 45 minutes. The PAHs were then analyzed with a GC-MS spectrophotometer model (Shimadzu GCMS-QP2010 SE) connected to a computer work station was used for the PAHs analysis. The GC-MS was equipped with an SGE BPX5 GC capillary column (30 m × 0.25 mm × 0.25 μm) for the separation of compounds. Helium was used as the carrier gas at a flow rate of 15.5 ml/minute and 14.5 psi. 1 μl of the sample was injected at 280°C, split mode (10:1). The oven programming was set for a total runtime of 40 minutes, which included: 100°C (2-minute hold);10°C /min rise to 200°C;7°C /min rise to 249°C;3°C /min rise to 300°C (2-minute hold). The interface temperature was set at 290°C. Analysis was done in Selected Ion Monitoring (SIM) mode and the peak areas of each of the PAHs were collected from the chromatograph and used for quantification of the 16 PAHs listed by the U.S. Environmental Protection Agency (EPA) which included, BaA (benz[a]anthracene: 4 rings), BaP (benzo[a]pyrene: 5 rings), BbF (benzo [b]fluoranthene: 5 rings), BkF (benzo[k]fluoranthene: 5 rings), Chr (chrysene: 4 rings), DbA (dibenz[a,h]anthracene: 5 rings), InP (indeno[1,2,3 - cd] pyrene: 6 rings) and Acp (acenaphthene: 3 rings), Acpy (acenaphthylene: 3 rings), Ant (anthracene: 3 rings), BghiP (benzo[g,h,i]perylene: 6 rings), Flu (fluorene: 3 rings), FluA (fluoranthene: 4 rings), Nap (naphthalene: 2 rings), PhA (phenanthrene: 3 rings) and Pyr (pyrene: 4 rings). Ion source-interface temperature was set at 200°C - 250°C. Internal standards from Sigma Aldrich were used in the analysis and the acquired mass spectra data were then matched against the NIST 2014 library [1] [2]. The mean PAHs concentration in the bottom ashes of each hospital varied broadly from 0.001 mg/kg to 0.4845 mg/kg, and the mean total concentration levels of individual PAHs ranged from 0.0072 mg/kg to 1.171 mg/kg. Low molecular weight PAHs (Phenanthrene, Naphthalene and Fluorene) were predominant in all the hospital wastes whereas Kitale and Narok presented the lowest PAHs concentrations and the lowest number of individual PAHs. Moi/Voi recorded the highest total PAHs concentration at 1.3129 ± 0.0023 mg/kg from a total of 11 PAHs being detected from the bottom ash samples. Narok had only three PAHs being detected at very low concentrations of 0.0041 ± 0.00 mg/kg, 0.0076 ± 0.00 mg/kg and 0.012 ± 0.00 mg/kg for phenanthrene, anthracene and chrysene respectively. This study presents hospital incinerator bottom ash as containing detectable levels of both carcinogenic and non-carcinogenic PAHs. Continued unprotected exposure of hospital workers (waste handlers) to the bottom ash PAHs could be hazardous to their health because of their cumulative effect. Preventive measures e.g. the use of Personal protective equipment (PPE) should be prioritised to minimise direct contact with the bottom ash. The study recommends an upgrade on incinerator technology for efficient combustion processes thus for better pollution control.
基金financial support from the National Natural Science Foundation of China(21991092,21991090,22022202,21972142,21902153,21974138)the Chinese Academy of Sciences(QYZDY-SSW-SC024)the Dalian Institute of Chemical Physics(DICP I201926,DICP I201947)。
文摘Low-carbon process for resource utilization of polycyclic aromatic hydrocarbons(PAHs)in zeolitecatalyzed processes,geared to carbon neutrality-a prominent trend throughout human activities,has been bottlenecked by the lack of a complete mechanistic understanding of coking and decoking chemistry,involving the speciation and molecular evolution of PAHs,the plethora of which causes catalyst deactivation and forces regeneration,rendering significant CO_(2) emission.Herein,by exploiting the high-resolution matrix-assisted laser desorption/ionization Fourier-transform ion cyclotron resonance mass spectrometry(MALDI FT-ICR MS),we unveil the missing fingerprints of the mechanistic pathways for both formation and decomposition of cross-linked cage-passing PAHs for SAPO-34-catalyzed,industrially relevant methanol-to-olefins(MTO)as a model reaction.Notable is the molecule-resolved symmetrical signature:their speciation originates exclusively from the direct coupling of in-cage hydrocarbon pool(HCP)species,whereas water-promoted decomposition of cage-passing PAHs initiates with selective cracking of inter-cage local structures at 8-rings followed by deep aromatic steam reforming.Molecular deciphering the reversibly dynamic evolution trajectory(fate)of full-spectrum aromatic hydrocarbons and fulfilling the real-time quantitative carbon resource footprints advance the fundamental knowledge of deactivation and regeneration phenomena(decay and recovery motifs of autocatalysis)and disclose the underlying mechanisms of especially the chemistry of coking and decoking in zeolite catalysis.The positive yet divergent roles of water in these two processes are disentangled.These unprecedented insights ultimately lead us to a steam regeneration strategy with valuable CO and H_(2) as main products,negligible CO_(2) emission in steam reforming and full catalyst activity recovery,which further proves feasible in other important chemical processes,promising to be a sustainable and potent approach that contributes to carbon-neutral chemical industry.
基金financially supported by the Natural Science Foundation of Jiangsu Province (Grant number:BK20140260)the Joint Project of Industry-UniversityResearch of Jiangsu Province (Grant number:BY2018158 and BY2021590)+1 种基金the CNPC-CZU Innovation Alliance,the Jiangsu Province Key Laboratory of Fine Petrochemical Engineering (Grant number:KF2302)the State Key Laboratory of Heavy Oil Processing。
文摘The selective hydrogenation of polycyclic aromatic hydrocarbons(PAHs)from fluid catalytic cracking(FCC)slurry extract was conducted in a batch reactor over aγ-Al_(2)O_(3)-supported bimetallic Ni-W catalyst.For the Ni-W/γ-Al_(2)O_(3) catalyst,the experiment run was divided into three processes according to the reaction conditions used:(1)the absence of hydrogenation as both temperature and pressure increased;(2)the desulfurization of FCC slurry extract under a fixed pressure as the temperature increased;and(3)the selective hydrogenation of PAHs when both pressure and temperature remained constant.The hydrogen consumption could be accurately calculated from the Redlich–Kwong equation of state.The results for the removal of PAHs with hydrogenation displayed an excellent fit to the first-order kinetics.The apparent activation energy was determined to be 20.80 kJ/mol.
文摘Levels of Polycyclic aromatic hydrocarbons (PAHs) from sediments collected in July 2017, a week after tanks oil leak in the bay of Wesha Peninsular, Pemba Island are reported. Four sampling points were chosen alongside the mangroves where a total of twenty samples were collected during the low tides. Eight PAHs were detected with concentrations ranging from ND to 53.42 ng/g (dw). Total PAHs in sediments was 158.38 ng⋅g<sup>-1</sup>. Phenanthrene residues (lower molecular weight) were dominant followed by pyrene (higher molecular weight PAHs) accounting for 90% and 40% detection frequencies, respectively. Statistical analysis showed no significant difference in the concentrations of PAHs among sites (p < 0.05, ANOVA). Vertical distribution of PAHs shows no definite patterns with sediment depth, however, composition patterns of PAHs along sediment depth indicate that higher molecular weight PAHs tend to remain in middle layer (2 - 4 cm). The results advocate the needs of proper monitoring to avoid the possible consequences to the public health.
