Oxidation of coke deposited on spent catalytic cracking catalysts was compared with that of coal and coal char via the non-isothermal oxidation means, i.e. the thermal-gravimetric analysis （TGA） and the differential...Oxidation of coke deposited on spent catalytic cracking catalysts was compared with that of coal and coal char via the non-isothermal oxidation means, i.e. the thermal-gravimetric analysis （TGA） and the differential thermal analysis （DTA）. Oxidation kinetic parameters were further investigated by model-fitting methods. The test results showed that the oxidation of spent catalysts was a quite mild process, while coal and coal char experienced sharp weight loss during oxidation. The temperature for commencement and termination of oxidation increased in the following order： coal〈coal char〈spent catalysts, and the oxidation of the three tested materials displayed a self-catalytic nature, with their largest oxidation rate appearing at a weight percent of 24.96%, 34.21% and 57.93%, respectively. The oxidation of spent catalysts obeyed a random nucleation model for the first-order reaction, with Ea=206.13 kJ/mol and lgA=10.10, and the oxidation of coal could be a diffusion-controlled reaction mechanism, with Ea=161.61 kJ/mol and lgA=7.74, while the oxidation of coal char also obeyed a random nucleation model for the first-order reaction, with Ea= 149.36 k J/mol and lgA=7.89.展开更多
Nitric humic acid was prepared by catalytic oxidation between nitric acid and Guizhou coal, with added catalysts. We investigated catalytic oxidation processes and the factors that affect the reactions. The effects of...Nitric humic acid was prepared by catalytic oxidation between nitric acid and Guizhou coal, with added catalysts. We investigated catalytic oxidation processes and the factors that affect the reactions. The effects of different catalysts, including NiSO4 support on active carbon （AC-NiS04）, NiS04 support on sil- icon dioxide （SiO2-NiSO4）, composites of SO42-1Fe203, Zr-iron and vanadium-iron composite were stud- ied. As well, we investigated nitric humic acid yields and the chemical structure of products by element analysis, FT-IR and E4/E6 （an absorbance ratio at wavelengths of 465 and 665 nm of humic acid alkaline extraction solutions）. The results show that the catalytic oxidation reaction with added catalysts can increase humic acid yields by 18.7%, 16.36% 12.94%, 5.61% and 8.59%, respectively. The highest yield of humic acid, i.e., 36.0%, was obtained with AC-NiSO4 as the catalyst. The amounts of C and H decreased with the amount of nitrogen. The increase in the E4/E6 ratio in catalytic oxidation of （Guizhou） coal shows that small molecular weights and high yields of nitric humic acid can be obtained by catalytic oxidation reactions.展开更多
Coal electro-oxidation in sodium hydroxide solution with catalysts, K3Fe（CN）6, sodium hypochlorite and sup- ported FeS, were investigated, respectively. Gas produced from electro-analysis of coal slurry was collecte...Coal electro-oxidation in sodium hydroxide solution with catalysts, K3Fe（CN）6, sodium hypochlorite and sup- ported FeS, were investigated, respectively. Gas produced from electro-analysis of coal slurry was collected by drainage-method and l-t curves were recorded to testify the catalysis of each catalyst for coal oxidation. The results show that the three kinds of catalysts can obviously improve the coal oxidation current. Furthermore, K3Fe（CN）6 and sodium hypochlorite played an indirect oxidation role in the electrolysis process. Catalysts bridge the coal par- ticles and the solid electrode surface, thus increase the coal oxidation rates. The changes of catalyst content during the electrolysis were further determined by quantitative titration to discuss the catalytic Mechanism. The dynamic transition of K3Fe（CN）6/K4Fe（CN）6 and ClO^-/Cl^- are proposed by iodometric method.展开更多
Sewage sludge from a biological wastewater treatment plant was converted into sewage sludge based activated carbon（SBAC） with Zn Cl2 as activation agent, which was used as a support for ferric oxides to form a catal...Sewage sludge from a biological wastewater treatment plant was converted into sewage sludge based activated carbon（SBAC） with Zn Cl2 as activation agent, which was used as a support for ferric oxides to form a catalyst（Fe Ox/SBAC） by a simple impregnation method.The new material was then used to improve the performance of Fenton oxidation of real biologically pretreated coal gasification wastewater（CGW）. The results indicated that the prepared Fe Ox/SBAC significantly enhanced the pollutant removal performance in the Fenton process, so that the treated wastewater was more biodegradable and less toxic. The best performance was obtained over a wide p H range from 2 to 7, temperature 30°C, 15 mg/L of H2O2 and 1 g/L of catalyst, and the treated effluent concentrations of COD, total phenols,BOD5 and TOC all met the discharge limits in China. Meanwhile, on the basis of significant inhibition by a radical scavenger in the heterogeneous Fenton process as well as the evolution of FT-IR spectra of pollutant-saturated Fe Ox/BAC with and without H2O2, it was deduced that the catalytic activity was responsible for generating hydroxyl radicals, and a possible reaction pathway and interface mechanism were proposed. Moreover, Fe Ox/SBAC showed superior stability over five successive oxidation runs. Thus, heterogeneous Fenton oxidation of biologically pretreated CGW by Fe Ox/SBAC, with the advantages of being economical, efficient and sustainable, holds promise for engineering application.展开更多
文摘Oxidation of coke deposited on spent catalytic cracking catalysts was compared with that of coal and coal char via the non-isothermal oxidation means, i.e. the thermal-gravimetric analysis （TGA） and the differential thermal analysis （DTA）. Oxidation kinetic parameters were further investigated by model-fitting methods. The test results showed that the oxidation of spent catalysts was a quite mild process, while coal and coal char experienced sharp weight loss during oxidation. The temperature for commencement and termination of oxidation increased in the following order： coal〈coal char〈spent catalysts, and the oxidation of the three tested materials displayed a self-catalytic nature, with their largest oxidation rate appearing at a weight percent of 24.96%, 34.21% and 57.93%, respectively. The oxidation of spent catalysts obeyed a random nucleation model for the first-order reaction, with Ea=206.13 kJ/mol and lgA=10.10, and the oxidation of coal could be a diffusion-controlled reaction mechanism, with Ea=161.61 kJ/mol and lgA=7.74, while the oxidation of coal char also obeyed a random nucleation model for the first-order reaction, with Ea= 149.36 k J/mol and lgA=7.89.
基金sponsored by the Shaanxi Key Scientific and Technological Project, China (No. 2010K07-20)the National Science and Technology Major Project (No. 2011ZX05037-003)
文摘Nitric humic acid was prepared by catalytic oxidation between nitric acid and Guizhou coal, with added catalysts. We investigated catalytic oxidation processes and the factors that affect the reactions. The effects of different catalysts, including NiSO4 support on active carbon （AC-NiS04）, NiS04 support on sil- icon dioxide （SiO2-NiSO4）, composites of SO42-1Fe203, Zr-iron and vanadium-iron composite were stud- ied. As well, we investigated nitric humic acid yields and the chemical structure of products by element analysis, FT-IR and E4/E6 （an absorbance ratio at wavelengths of 465 and 665 nm of humic acid alkaline extraction solutions）. The results show that the catalytic oxidation reaction with added catalysts can increase humic acid yields by 18.7%, 16.36% 12.94%, 5.61% and 8.59%, respectively. The highest yield of humic acid, i.e., 36.0%, was obtained with AC-NiSO4 as the catalyst. The amounts of C and H decreased with the amount of nitrogen. The increase in the E4/E6 ratio in catalytic oxidation of （Guizhou） coal shows that small molecular weights and high yields of nitric humic acid can be obtained by catalytic oxidation reactions.
基金Project supported by the National Natural Science Foundation of China （Nos. 20673071, 20873083）, the Funding of Shanghai Education Commission Fifth Key Disciplines （No. J50102） and the State Key Laboratory of Chemical Engineering （No. S KL-ChE-08A01）.
文摘Coal electro-oxidation in sodium hydroxide solution with catalysts, K3Fe（CN）6, sodium hypochlorite and sup- ported FeS, were investigated, respectively. Gas produced from electro-analysis of coal slurry was collected by drainage-method and l-t curves were recorded to testify the catalysis of each catalyst for coal oxidation. The results show that the three kinds of catalysts can obviously improve the coal oxidation current. Furthermore, K3Fe（CN）6 and sodium hypochlorite played an indirect oxidation role in the electrolysis process. Catalysts bridge the coal par- ticles and the solid electrode surface, thus increase the coal oxidation rates. The changes of catalyst content during the electrolysis were further determined by quantitative titration to discuss the catalytic Mechanism. The dynamic transition of K3Fe（CN）6/K4Fe（CN）6 and ClO^-/Cl^- are proposed by iodometric method.
基金supported by the State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology) (No.2015DX02)
文摘Sewage sludge from a biological wastewater treatment plant was converted into sewage sludge based activated carbon（SBAC） with Zn Cl2 as activation agent, which was used as a support for ferric oxides to form a catalyst（Fe Ox/SBAC） by a simple impregnation method.The new material was then used to improve the performance of Fenton oxidation of real biologically pretreated coal gasification wastewater（CGW）. The results indicated that the prepared Fe Ox/SBAC significantly enhanced the pollutant removal performance in the Fenton process, so that the treated wastewater was more biodegradable and less toxic. The best performance was obtained over a wide p H range from 2 to 7, temperature 30°C, 15 mg/L of H2O2 and 1 g/L of catalyst, and the treated effluent concentrations of COD, total phenols,BOD5 and TOC all met the discharge limits in China. Meanwhile, on the basis of significant inhibition by a radical scavenger in the heterogeneous Fenton process as well as the evolution of FT-IR spectra of pollutant-saturated Fe Ox/BAC with and without H2O2, it was deduced that the catalytic activity was responsible for generating hydroxyl radicals, and a possible reaction pathway and interface mechanism were proposed. Moreover, Fe Ox/SBAC showed superior stability over five successive oxidation runs. Thus, heterogeneous Fenton oxidation of biologically pretreated CGW by Fe Ox/SBAC, with the advantages of being economical, efficient and sustainable, holds promise for engineering application.
