The destruction of toxic organic wastewaters from munitions demilitarization and complex industrial chemical clearly becomes an overwhelming problem if left to conventional treatment processes. Two options, incinerati...The destruction of toxic organic wastewaters from munitions demilitarization and complex industrial chemical clearly becomes an overwhelming problem if left to conventional treatment processes. Two options, incineration and supercritical water oxidation (SCWO), exist for the complete destruction of toxic organic wastewaters. Incinerator has associated problems such as very high cost and public resentment; on the other hand, SCWO has proved to be a very promising method for the treatment of many different wastewaters with extremely efficient organic waste destruction 99.99% with none of the emissions associated with incineration. In this review, the concepts of SCWO, result and present perspectives of application, and industrial status of SCWO are critically examined and discussed.展开更多
Hydrothermal decomposition of pentachlorophenol (PCP, C6HC150), as the probable human carcinogen, was investigated in a tubular reactor under subcritical and supercritical water with sodium hydroxide (NaOH) additi...Hydrothermal decomposition of pentachlorophenol (PCP, C6HC150), as the probable human carcinogen, was investigated in a tubular reactor under subcritical and supercritical water with sodium hydroxide (NaOH) addition. The experiments were conducted at a temperature range of 30(0-420℃ and a fixed pressure of 25 MPa, with a residence time that ranged from 10 s to 70 s. Under the reaction conditions, the initial PCP concentrations were varied from 0.25 to 1.39 mmol/L, and the NaOH concentrations were varied from 2.5 to 25 times of the concentrations of PCP. The result of this study showed that PCP conversion in supercritical water was highly dependent on the reaction temperature, residence time, and NaOH concentration. PCP conversion in subcritical water is, however, only dependent on reaction temperature. NaOH concentration and residence times were found to have little effect on PCP conversion in subcritical condition. It was found that NaOH concentration affected the dechlorinations of PCP in the supercritical water. The intermediates detected were proposed to be tetrachlorophenol and trichlorophenol, respectively.展开更多
The destruction of methylphosphonic acid (MPA), a final product by hydrolysis/neutralization of organophosphorus agents such as sarin and VX (O-ethyl S-[2-(diisopropylamino)ethyl] methylphosphonothionate), was i...The destruction of methylphosphonic acid (MPA), a final product by hydrolysis/neutralization of organophosphorus agents such as sarin and VX (O-ethyl S-[2-(diisopropylamino)ethyl] methylphosphonothionate), was investigated in a a bench-scale, continuous concentric vertical double wall reactor under supercritical water oxidation condition. The experiments were conducted at a temperature range of 450–600°C and a fixed pressure of 25 MPa. Hydrogen peroxide was used as an oxidant. The destruction efficiency (DE) was monitored by analyzing total organic carbon (TOC) and MPA concentrations using ion chromatography on the liquid effluent samples. The results showed that the DE of MPA up to 99.999% was achieved at a reaction temperature of 600°C, oxygen concentration of 113% storichiometric requirement, and reactor residence time of 8 sec. On the basis of the data derived from experiments, a global kinetic rate equation for the DE of MPA and DE of TOC were developed by nonlinear regression analysis. The model predictions agreed well with the experimental data.展开更多
Supercritical water oxidation (SCWO) has been drawing much attention due to effectively destroy a large variety of high-risk wastes resulting from munitions demilitarization and complex industrial chemical. An impor...Supercritical water oxidation (SCWO) has been drawing much attention due to effectively destroy a large variety of high-risk wastes resulting from munitions demilitarization and complex industrial chemical. An important design consideration in the development of supercritical water oxidation is the information of decomposition rate. In this paper, the decomposition rate of dimethyl methylphosphonate(DMMP), which is similar to the nerve agent VX and GB(Sarin) in its structure, was investigated under SCWO conditions. The experiments were performed in an isothermal tubular reactor with a H2O2 as an oxidant. The reaction temperatures were ranged from 398 to 633℃ at a fixed pressure of 24 MPa. The conversion of DMMP was monitored by analyzing total organic carbon (TOC) on the liquid effluent samples. It is found that the oxidative decomposition of DMMP proceeded rapidly and a high TOC decomposition up to 99.99% was obtained within 11 s at 555℃. On the basis of data derived from experiments, a global kinetic equation for the decomposition of DMMP was developed. The model predictions agreed well with the experimental data.展开更多
Clinopyroxene-enriched upper mantle xenoliths classified as wehrlites are common(~20% of all xenoliths) in the central part of the Nograd-G(o| ")m(o|")r Volcanic Field(NGVF),situated in the northern margin o...Clinopyroxene-enriched upper mantle xenoliths classified as wehrlites are common(~20% of all xenoliths) in the central part of the Nograd-G(o| ")m(o|")r Volcanic Field(NGVF),situated in the northern margin of the Pannonian Basin in northern Hungary and southern Slovakia.In this study,we thoroughly investigated 12 wehrlite xenoliths,two from each wehrlite-bearing occurrence,to determine the conditions of their formation.Specific textural features,including clinopyroxene-rich patches in an olivine-rich lithology,orthopyroxene remnants in the cores of newlyformed clinopyroxenes and vermicular spinel forms all suggest that wehrlites were formed as a result of intensive interaction between a metasomatic agent and the peridotite wall rock.Based on the major and trace element geochemistry of the rock-forming minerals,significant enrichment in basaltic(Fe,Mn,Ti) and high field strength elements(Nb,Ta,Hf,Zr) was observed,compared to compositions of common lherzolite xenoliths.The presence of orthopyroxene remnants and geochemical trends in rock-forming minerals suggest that the metasomatic process ceased before complete wehrlitization was achieved.The composition of the metasomatic agent is interpreted to be a mafic silicate melt,which was further confirmed by numerical modelling of trace elements using the plate model.The model results also show that the melt/rock ratio played a key role in the degree of petrographic and geochemical transformation.The lack of equilibrium and the conclusions drawn by using variable lherzolitic precursors in the model both suggest that wehrlitization was the last event that occurred shortly before xenolith entrainment in the host mafic melt.We suggest that the wehrlitization and the Plio-Pleistocene basaltic volcanism are related to the same magmatic event.展开更多
基金Project supported by the Korea Institute of Science and Technology (KIST).
文摘The destruction of toxic organic wastewaters from munitions demilitarization and complex industrial chemical clearly becomes an overwhelming problem if left to conventional treatment processes. Two options, incineration and supercritical water oxidation (SCWO), exist for the complete destruction of toxic organic wastewaters. Incinerator has associated problems such as very high cost and public resentment; on the other hand, SCWO has proved to be a very promising method for the treatment of many different wastewaters with extremely efficient organic waste destruction 99.99% with none of the emissions associated with incineration. In this review, the concepts of SCWO, result and present perspectives of application, and industrial status of SCWO are critically examined and discussed.
文摘Hydrothermal decomposition of pentachlorophenol (PCP, C6HC150), as the probable human carcinogen, was investigated in a tubular reactor under subcritical and supercritical water with sodium hydroxide (NaOH) addition. The experiments were conducted at a temperature range of 30(0-420℃ and a fixed pressure of 25 MPa, with a residence time that ranged from 10 s to 70 s. Under the reaction conditions, the initial PCP concentrations were varied from 0.25 to 1.39 mmol/L, and the NaOH concentrations were varied from 2.5 to 25 times of the concentrations of PCP. The result of this study showed that PCP conversion in supercritical water was highly dependent on the reaction temperature, residence time, and NaOH concentration. PCP conversion in subcritical water is, however, only dependent on reaction temperature. NaOH concentration and residence times were found to have little effect on PCP conversion in subcritical condition. It was found that NaOH concentration affected the dechlorinations of PCP in the supercritical water. The intermediates detected were proposed to be tetrachlorophenol and trichlorophenol, respectively.
基金supported by Agency for Defense Development,Korea and Korea Institute of Scienceand Technology
文摘The destruction of methylphosphonic acid (MPA), a final product by hydrolysis/neutralization of organophosphorus agents such as sarin and VX (O-ethyl S-[2-(diisopropylamino)ethyl] methylphosphonothionate), was investigated in a a bench-scale, continuous concentric vertical double wall reactor under supercritical water oxidation condition. The experiments were conducted at a temperature range of 450–600°C and a fixed pressure of 25 MPa. Hydrogen peroxide was used as an oxidant. The destruction efficiency (DE) was monitored by analyzing total organic carbon (TOC) and MPA concentrations using ion chromatography on the liquid effluent samples. The results showed that the DE of MPA up to 99.999% was achieved at a reaction temperature of 600°C, oxygen concentration of 113% storichiometric requirement, and reactor residence time of 8 sec. On the basis of the data derived from experiments, a global kinetic rate equation for the DE of MPA and DE of TOC were developed by nonlinear regression analysis. The model predictions agreed well with the experimental data.
文摘Supercritical water oxidation (SCWO) has been drawing much attention due to effectively destroy a large variety of high-risk wastes resulting from munitions demilitarization and complex industrial chemical. An important design consideration in the development of supercritical water oxidation is the information of decomposition rate. In this paper, the decomposition rate of dimethyl methylphosphonate(DMMP), which is similar to the nerve agent VX and GB(Sarin) in its structure, was investigated under SCWO conditions. The experiments were performed in an isothermal tubular reactor with a H2O2 as an oxidant. The reaction temperatures were ranged from 398 to 633℃ at a fixed pressure of 24 MPa. The conversion of DMMP was monitored by analyzing total organic carbon (TOC) on the liquid effluent samples. It is found that the oxidative decomposition of DMMP proceeded rapidly and a high TOC decomposition up to 99.99% was obtained within 11 s at 555℃. On the basis of data derived from experiments, a global kinetic equation for the decomposition of DMMP was developed. The model predictions agreed well with the experimental data.
基金This research was financially facilitated by Orlando Vasellisupported by the Bolyai Postdoctoral Fellowship Program,a Marie Curie International Reintegration Grant(Grant No.NAMS-230937)+3 种基金a postdoctoral grant(Grant No.PD101683)of the Hungarian Scientific Research Found(OTKA)to I.J.K.as well as a grant of the Hungarian Scientific Research Found(Grant No.78425)to Cs.supported by a grant from the U.S.National Science Foundation(EAR1624589)to R.J.supported by the GINOP-2.3.2-152016-00009 research program。
文摘Clinopyroxene-enriched upper mantle xenoliths classified as wehrlites are common(~20% of all xenoliths) in the central part of the Nograd-G(o| ")m(o|")r Volcanic Field(NGVF),situated in the northern margin of the Pannonian Basin in northern Hungary and southern Slovakia.In this study,we thoroughly investigated 12 wehrlite xenoliths,two from each wehrlite-bearing occurrence,to determine the conditions of their formation.Specific textural features,including clinopyroxene-rich patches in an olivine-rich lithology,orthopyroxene remnants in the cores of newlyformed clinopyroxenes and vermicular spinel forms all suggest that wehrlites were formed as a result of intensive interaction between a metasomatic agent and the peridotite wall rock.Based on the major and trace element geochemistry of the rock-forming minerals,significant enrichment in basaltic(Fe,Mn,Ti) and high field strength elements(Nb,Ta,Hf,Zr) was observed,compared to compositions of common lherzolite xenoliths.The presence of orthopyroxene remnants and geochemical trends in rock-forming minerals suggest that the metasomatic process ceased before complete wehrlitization was achieved.The composition of the metasomatic agent is interpreted to be a mafic silicate melt,which was further confirmed by numerical modelling of trace elements using the plate model.The model results also show that the melt/rock ratio played a key role in the degree of petrographic and geochemical transformation.The lack of equilibrium and the conclusions drawn by using variable lherzolitic precursors in the model both suggest that wehrlitization was the last event that occurred shortly before xenolith entrainment in the host mafic melt.We suggest that the wehrlitization and the Plio-Pleistocene basaltic volcanism are related to the same magmatic event.