Coal gasification slag(CGS)is a type of solid waste produced during coal gasification,in which heavy metals severely restrict its resource utilization.In this work,the mineral occurrence and distribution of typical he...Coal gasification slag(CGS)is a type of solid waste produced during coal gasification,in which heavy metals severely restrict its resource utilization.In this work,the mineral occurrence and distribution of typical heavy metal Cr in CGS is investigated.The leaching behavior of Cr under different conditions is studied in detail.Acid leaching-selective oxidation-coprecipitation method is proposed based on the characteristics of Cr in CGS.The detoxification of Cr in CGS is realized,and the detoxification mechanism is clarified.Results show that Cr is highly enriched in CGS.The speciation of Cr is mainly residual fraction(74.47%-86.12%),which is combined with amorphous aluminosilicate.Cr^(3+)and Cr^(6+)account for 90.93%-94.82%and 5.18%-9.07%of total Cr,respectively.High acid concentration and high liquid-solid ratio are beneficial to destroy the lattice structure of amorphous aluminosilicate,thus improving the leaching efficiency of Cr,which can reach 97.93%under the optimal conditions.Acid leaching-selective oxidation-coprecipitation method can realize the detoxification of Cr in CGS.Under the optimal conditions,the removal rates of Fe^(3+)and Cr^(3+)in the leaching solution are 80.99%-84.79%and 70.58%-71.69%,respectively,while the loss rate of Al^(3+)is only 1.10%-3.35%.Detoxification slag exists in the form of Fe-Cr coprecipitation(Fe_(1-x)Cr_xOOH),which can be used for smelting.The detoxification acid leaching solution can be used to prepare inorganic polymer composite coagulant poly-aluminum chloride(PAC).This study can provide theoretical and data guidance for detoxification of heavy metal Cr in CGS and achieve resource utilization of coal gasification solid waste.展开更多
The improper disposal of spent selective catalytic reduction (SCR) catalysts causes environmental pollution and metal resource waste.A novel process to recover anatase titanium dioxide (TiO_(2)) from spent SCR catalys...The improper disposal of spent selective catalytic reduction (SCR) catalysts causes environmental pollution and metal resource waste.A novel process to recover anatase titanium dioxide (TiO_(2)) from spent SCR catalysts was proposed.The process included alkali (NaOH) hydrothermal treatment,sulfuric acid washing,and calcination.Anatase TiO_(2) in spent SCR catalyst was reconstructed by forming Na_(2)Ti_(2)O_(4)(OH)_(2) nanosheet during NaOH hydrothermal treatment and H_(2)Ti_(2)O_(4)(OH)_(2) during sulfuric acid washing.Anatase TiO_(2) was recovered by decomposing H_(2)Ti_(2)O_(4)(OH)_(2) during calcination.The surface pore properties of the recovered anatase TiO_(2) were adequately improved,and its specific surface area (SSA) and pore volume (PV) were 85 m^(2)·g^(-1)and 0.40 cm^(3)·g^(-1),respectively.The elements affecting catalytic abilities(arsenic and sodium) were also removed.The SCR catalyst was resynthesized using the recovered TiO_(2) as raw material,and its catalytic performance in NO selective reduction was comparable with that of commercial SCR catalyst.This study realized the sustainable recycling of anatase TiO_(2) from spent SCR catalyst.展开更多
The kinetics of the decomposition of dimethylhexane-1,6-dicarbamate to 1,6-hexamethylene diisocyanate was studied. A consecutive reaction model was established and the reaction orders for the two steps were confirmed ...The kinetics of the decomposition of dimethylhexane-1,6-dicarbamate to 1,6-hexamethylene diisocyanate was studied. A consecutive reaction model was established and the reaction orders for the two steps were confirmed to be 1 and 1.3 by the integral test method and the numerical differential method, respectively. The activation energies of the two steps were(56.94 ± 5.90) k J·mol-1and(72.07 ± 3.47) k J·mol-1with the frequency factors exp(12.53 ± 1.42) min-1and(14.254 ± 0.84) mol-0.33·L0.33·min-1, respectively. Based on the kinetic model obtained, the progress of the reaction can be calculated under given conditions.展开更多
In Na_2O–CaO–SiO_2–H_2O system,systematic investigations of phase and morphology of calcium silicate in hydrothermal conditions were concisely conducted for high-value utilization of silicon resource in high-alumin...In Na_2O–CaO–SiO_2–H_2O system,systematic investigations of phase and morphology of calcium silicate in hydrothermal conditions were concisely conducted for high-value utilization of silicon resource in high-alumina fly ash(HAFA).The results show that crystal composition and phase may be affected by relatively low concentration of NaOH,and sodium ions are rearranged into the structure to form NaCaHSiO_4 and Na_2Ca_3H_8Si_2O_(12) with different C/S ratio at high concentration of Na OH.In addition,phases in wollastonite group possess the morphology of nano fiber.Formation of nano fiber is attributed to the difference of surface energies between axial and radial direction,and higher temperatures lead to easier growth along radial direction.The preparation of C–S–H with different phases and morphologies can guide for the application of silicate solution with high alkalinity with different purposes.展开更多
基金finally supported by the National Natural Science Foundation of China(52174390,U1810205)Innovation Academy for Green Manufacture of the Chinese Academy of Sciences China(IAGM2022D04)Strategic Priority Research Program of the Chinese Academy of Sciences China(XDA21040601)。
文摘Coal gasification slag(CGS)is a type of solid waste produced during coal gasification,in which heavy metals severely restrict its resource utilization.In this work,the mineral occurrence and distribution of typical heavy metal Cr in CGS is investigated.The leaching behavior of Cr under different conditions is studied in detail.Acid leaching-selective oxidation-coprecipitation method is proposed based on the characteristics of Cr in CGS.The detoxification of Cr in CGS is realized,and the detoxification mechanism is clarified.Results show that Cr is highly enriched in CGS.The speciation of Cr is mainly residual fraction(74.47%-86.12%),which is combined with amorphous aluminosilicate.Cr^(3+)and Cr^(6+)account for 90.93%-94.82%and 5.18%-9.07%of total Cr,respectively.High acid concentration and high liquid-solid ratio are beneficial to destroy the lattice structure of amorphous aluminosilicate,thus improving the leaching efficiency of Cr,which can reach 97.93%under the optimal conditions.Acid leaching-selective oxidation-coprecipitation method can realize the detoxification of Cr in CGS.Under the optimal conditions,the removal rates of Fe^(3+)and Cr^(3+)in the leaching solution are 80.99%-84.79%and 70.58%-71.69%,respectively,while the loss rate of Al^(3+)is only 1.10%-3.35%.Detoxification slag exists in the form of Fe-Cr coprecipitation(Fe_(1-x)Cr_xOOH),which can be used for smelting.The detoxification acid leaching solution can be used to prepare inorganic polymer composite coagulant poly-aluminum chloride(PAC).This study can provide theoretical and data guidance for detoxification of heavy metal Cr in CGS and achieve resource utilization of coal gasification solid waste.
基金supported by the National Natural Science Foundation of China (52274411)the National Natural Science Foundation of China (51904287)the Innovation Academy for Green Manufacture,Chinese Academy of Sciences (IAGM2022D11)。
文摘The improper disposal of spent selective catalytic reduction (SCR) catalysts causes environmental pollution and metal resource waste.A novel process to recover anatase titanium dioxide (TiO_(2)) from spent SCR catalysts was proposed.The process included alkali (NaOH) hydrothermal treatment,sulfuric acid washing,and calcination.Anatase TiO_(2) in spent SCR catalyst was reconstructed by forming Na_(2)Ti_(2)O_(4)(OH)_(2) nanosheet during NaOH hydrothermal treatment and H_(2)Ti_(2)O_(4)(OH)_(2) during sulfuric acid washing.Anatase TiO_(2) was recovered by decomposing H_(2)Ti_(2)O_(4)(OH)_(2) during calcination.The surface pore properties of the recovered anatase TiO_(2) were adequately improved,and its specific surface area (SSA) and pore volume (PV) were 85 m^(2)·g^(-1)and 0.40 cm^(3)·g^(-1),respectively.The elements affecting catalytic abilities(arsenic and sodium) were also removed.The SCR catalyst was resynthesized using the recovered TiO_(2) as raw material,and its catalytic performance in NO selective reduction was comparable with that of commercial SCR catalyst.This study realized the sustainable recycling of anatase TiO_(2) from spent SCR catalyst.
基金the National Key Technology R&D Program(2013BAC11B03)the Knowledge Innovation Fund of Chinese Academy of Science(KGCX2-YW-215-2)the National Natural Science Foundation of China(21476244)
文摘The kinetics of the decomposition of dimethylhexane-1,6-dicarbamate to 1,6-hexamethylene diisocyanate was studied. A consecutive reaction model was established and the reaction orders for the two steps were confirmed to be 1 and 1.3 by the integral test method and the numerical differential method, respectively. The activation energies of the two steps were(56.94 ± 5.90) k J·mol-1and(72.07 ± 3.47) k J·mol-1with the frequency factors exp(12.53 ± 1.42) min-1and(14.254 ± 0.84) mol-0.33·L0.33·min-1, respectively. Based on the kinetic model obtained, the progress of the reaction can be calculated under given conditions.
基金Supported by the National Natural Science Foundation of China(51304184)the Coal Based Key Scientific and Technological Project of Shanxi Province(MC2014-06)
文摘In Na_2O–CaO–SiO_2–H_2O system,systematic investigations of phase and morphology of calcium silicate in hydrothermal conditions were concisely conducted for high-value utilization of silicon resource in high-alumina fly ash(HAFA).The results show that crystal composition and phase may be affected by relatively low concentration of NaOH,and sodium ions are rearranged into the structure to form NaCaHSiO_4 and Na_2Ca_3H_8Si_2O_(12) with different C/S ratio at high concentration of Na OH.In addition,phases in wollastonite group possess the morphology of nano fiber.Formation of nano fiber is attributed to the difference of surface energies between axial and radial direction,and higher temperatures lead to easier growth along radial direction.The preparation of C–S–H with different phases and morphologies can guide for the application of silicate solution with high alkalinity with different purposes.