低品位软锰矿碱浸预脱硅-流化焙烧制备锰酸钠（英文）
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摘要
采用低浓度碱浸对低品位软锰矿进行预脱硅处理,考察NaOH浓度、液固比、浸出温度、浸出时间及搅拌速率对硅浸出率的影响,研究碱浸过程动力学。结果表明:在NaOH起始浓度为20%、液固比为4:1、浸出温度为180°C、浸出时间为4h、搅拌速率为300r/min的条件下,硅浸出率达到91.2%。缩核模型表明,碱浸过程受化学表面反应控制,其表观反应活化能为53.31kJ/mol。通过正交试验对脱硅渣流化焙烧制备锰酸钠的条件进行优化,在硅浸出率为91.2%、NaOH/MnO_2质量比为3:1、焙烧温度为500°C、焙烧时间为4h的条件下,锰酸钠的转化率为89.7%,且锰酸钠转化率随硅浸出率的升高而增加。
Low concentration alkaline leaching was used for predesilication treatment of low-grade pyrolusite. The effects of initial NaOH concentration, liquid-to-solid ratio, leaching temperature, leaching time and stirring speed on silica leaching rate were investigated and the kinetics of alkaline leaching process was studied. The results show that silica leaching rate reached 91.2% under the conditions of initial NaOH concentration of 20%, liquid-to-solid ratio of 4:1, leaching temperature of 180 °C, leaching time of 4 h and stirring speed of 300 r/min. Shrinking-core model showed that the leaching process was controlled by the chemical surface reaction with activation energy Ea of 53.31 k J/mol. The fluidized roasting conditions for preparation of sodium manganate were optimized by the orthogonal experiments using the desiliconized residue. The conversion rate of sodium manganate was obtained to be 89.7% under the conditions of silica leaching rate of 91.2%, NaOH/MnO_2 mass ratio of 3:1, roasting temperature of 500 °C and roasting time of 4 h, and it increased with the increase of silicon leaching rate.
Low concentration alkaline leaching was used for predesilication treatment of low-grade pyrolusite. The effects of initial NaOH concentration, liquid-to-solid ratio, leaching temperature, leaching time and stirring speed on silica leaching rate were investigated and the kinetics of alkaline leaching process was studied. The results show that silica leaching rate reached 91.2% under the conditions of initial NaOH concentration of 20%, liquid-to-solid ratio of 4:1, leaching temperature of 180 °C, leaching time of 4 h and stirring speed of 300 r/min. Shrinking-core model showed that the leaching process was controlled by the chemical surface reaction with activation energy Ea of 53.31 k J/mol. The fluidized roasting conditions for preparation of sodium manganate were optimized by the orthogonal experiments using the desiliconized residue. The conversion rate of sodium manganate was obtained to be 89.7% under the conditions of silica leaching rate of 91.2%, NaOH/MnO_2 mass ratio of 3:1, roasting temperature of 500 °C and roasting time of 4 h, and it increased with the increase of silicon leaching rate.
引文
[1]TANG Qing,ZHONG Hong,WANG Shuai,LI Jin-zhong,LIU Guang-yi.Reductive leaching of manganese oxide ores using waste tea as reductant in sulfuric acid solution[J].Transactions of Nonferrous Metals Society of China,2014,24(3):861-867.
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[3]SU Hai-feng,WEN Yan-xuan,WANG Fan,SUN Ying-yun,TONG Zhang-fa.Reductive leaching of manganese from low-grade manganese ore in H2SO4 using cane molasses as reductant[J].Hydrometallurgy,2008,93(3-4):136-139.
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[11]CAI Zhen-lei,FENG Ya-li,LI Hao-ran,DU Zhu-wei,LIU Xin-wei.Co-recovery of manganese from low-grade pyrolusite and vanadium from stone coal using fluidized roasting coupling technology[J].Hydrometallurgy,2013,131-132(S1):s40-s45.
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[13]TOGNONVI M T,SORO J,GELET J L,ROSSIGNOL S.Physico-chemistry of silica/Na silicate interactions during consolidation.Part 2:Effect of p H[J].Journal of Non-crystalline Solids,2012,358(3):492-501.
[14]XIAO Qing-gui,CHEN Yin,GAO Yi-ying,XU Hong-bin,ZHANG Yi.Leaching of silica from vanadium-bearing steel slag in sodium hydroxide solution[J].Hydrometallurgy,2010,104(2):216-221.
[15]MA Jia-yu,ZHAI Kun-ming,LI Zhi-bao.Desilication of synthetic Bayer liquor with calcium sulfate dihydrate:Kinetics and modelling[J].Hydrometallurgy,2011,107(1-2):48-55.
[16]CHEN De-sheng,ZHAO Long-sheng,QI Tao,HU Guo-ping,ZHAO Hong-xin,LI Jie,WANG Li-na.Desilication from titanium–vanadium slag by alkaline leaching[J].Transactions of Nonferrous Metals Society of China,2013,23(10):3076-3082.
[17]HUANG Kun,CHEN Jing,CHEN Yi-ran,ZHAO Jia-chun,LI Qi-wei,YANG Qiu-xue.Recovery of precious metals from spent auto-catalysts by method of pressure alkaline treatment-cyanide leaching[J].Chinese Journal of Nonferrous Metals,2006,16(2):363-369.(in Chinese)
[18]HE Huan,ZHANG Xu,SHEN Qing-feng,LI Xiao-ming,MENG Hong-li,LIU Hong-fei,WU Hai-yan.Determination of silicon dioxide in copper slag acid leaching solution with silicon molybdenum yellow spectrophotometry[J].Chinese Journal of Analysis Laboratory,2016,35(2):176-179.(in Chinese)
[19]HAN L,AL-DAHHAN M H.Gas–liquid mass transfer in a high pressure bubble column reactor with different sparger designs[J].Chemical Engineering Science,2007,62(1-2):131-139.
[20]NAYL A A,ISMAIL I M,ALY H F.Recovery of pure Mn SO4?H2O by reductive leaching of manganese from pyrolusite ore by sulfuric acid and hydrogen peroxide[J].International Journal of Mineral Processing,2011,100(3-4):116-123.
[21]SANTOS F M F,PINA P S,PORCARO R,OLIVEIRA V A,SILVA C A,LEAO V A.The kinetics of zinc silicate leaching in sodium hydroxide[J].Hydrometallurgy,2010,102(1-4):43-49.
[22]LEVIEN K L,LEVENSPIEL O.Optimal product distribution from laminar flow reactors:Newtonian and other power-law fluids[J].Chemical Engineering Science,1999,54(13-14):2453-2458.
[23]WANG Wei-da,FENG Ya-li,LI Hao-ran,YANG Zhi-chao,ZHANG Xu.Recovering gold from cyanide residue by alkaline predesilication-cyanide leaching technique[J].Chinese Journal of Nonferrous Metals,2015,25(1):233-240.(in Chinese)
[24]WANG Ruo-chao,ZHAI Yu-chun,NING Zhi-qiang,MA Pei-hua.Kinetics of Si O2 leaching from Al2O3 extracted slag of fly ash with sodium hydroxide solution[J].Transactions of Nonferrous Metals Society of China,2014,24(6):1928-1936.
[25]WU X,LEUNG D Y C.Optimization of biodiesel production from camelina oil using orthogonal experiment[J].Applied Energy,2011,88(11):3615-3624.
[2]ZHAO Yu-qian,JIANG Qing-lai,WANG Wei-gang,DU Ke,HU Guo-rong.Effect of electrolytic Mn O2 pretreatment on performance of as-prepared Li Mn2O4[J].Transactions of Nonferrous Metals Society of China,2012,22(5):1146-1150.
[3]SU Hai-feng,WEN Yan-xuan,WANG Fan,SUN Ying-yun,TONG Zhang-fa.Reductive leaching of manganese from low-grade manganese ore in H2SO4 using cane molasses as reductant[J].Hydrometallurgy,2008,93(3-4):136-139.
[4]REIDIES A H.Manganese compounds[M].Porsgrunn:Ullmann’s Encyclopedia of Industrial Chemistry,2000.
[5]CHEN R J,CHIRAYIL T,ZAVALIJ P,WHITTINGHAM M.The hydrothermal synthesis of sodium manganese oxide and a lithium vanadium oxide[J].Solid State Ionics,1996,86-88:1-7.
[6]KAPPENSTEIN C,PIRAULT-ROY L,GUéRIN M,WAHDAN T,ALI A A.Monopropellant decomposition catalysts:V.Thermal decomposition and reduction of permanganates as models for the preparation of supported Mn Ox catalysts[J].Applied Catalysis A:General,2002,234(1-2):145-153.
[7]WANG Y,LI Z,LI H.A new process for leaching metal values from ocean polymetallic nodules[J].Minerals Engineering,2005,18(11):1093-1098.
[8]ZHANG B H,LIU Y,CHANG Z,YANG Y Q,WEN Z B,WU Y P,HOLZE R.Nanowire Na0.35Mn O2 from a hydrothermal method as a cathode material for aqueous asymmetric supercapacitors[J].Journal of Power Sources,2014,253(5):98-103.
[9]WHITACRE J F,TEVAR A,SHARMA S.Na4Mn9O18 as a positive electrode material for an aqueous electrolyte sodium-ion energy storage device[J].Electrochemistry Communications,2010,12(3):463-466.
[10]PENG Dong,WANG Ji-kun.Reaction kinetics of potassium manganate prepared by three-phase compression oxidation process[J].Journal of the Chinese Ceramic Society,2012,40(12):1767-1772.(in Chinese)
[11]CAI Zhen-lei,FENG Ya-li,LI Hao-ran,DU Zhu-wei,LIU Xin-wei.Co-recovery of manganese from low-grade pyrolusite and vanadium from stone coal using fluidized roasting coupling technology[J].Hydrometallurgy,2013,131-132(S1):s40-s45.
[12]SANTOS O D S H,CARVALHO C D F,SILVA G A,SANTOS C G D.Manganese ore tailing:Optimization of acid leaching conditions and recovery of soluble manganese[J].Journal of Environmental Management,2015,147:314-320.
[13]TOGNONVI M T,SORO J,GELET J L,ROSSIGNOL S.Physico-chemistry of silica/Na silicate interactions during consolidation.Part 2:Effect of p H[J].Journal of Non-crystalline Solids,2012,358(3):492-501.
[14]XIAO Qing-gui,CHEN Yin,GAO Yi-ying,XU Hong-bin,ZHANG Yi.Leaching of silica from vanadium-bearing steel slag in sodium hydroxide solution[J].Hydrometallurgy,2010,104(2):216-221.
[15]MA Jia-yu,ZHAI Kun-ming,LI Zhi-bao.Desilication of synthetic Bayer liquor with calcium sulfate dihydrate:Kinetics and modelling[J].Hydrometallurgy,2011,107(1-2):48-55.
[16]CHEN De-sheng,ZHAO Long-sheng,QI Tao,HU Guo-ping,ZHAO Hong-xin,LI Jie,WANG Li-na.Desilication from titanium–vanadium slag by alkaline leaching[J].Transactions of Nonferrous Metals Society of China,2013,23(10):3076-3082.
[17]HUANG Kun,CHEN Jing,CHEN Yi-ran,ZHAO Jia-chun,LI Qi-wei,YANG Qiu-xue.Recovery of precious metals from spent auto-catalysts by method of pressure alkaline treatment-cyanide leaching[J].Chinese Journal of Nonferrous Metals,2006,16(2):363-369.(in Chinese)
[18]HE Huan,ZHANG Xu,SHEN Qing-feng,LI Xiao-ming,MENG Hong-li,LIU Hong-fei,WU Hai-yan.Determination of silicon dioxide in copper slag acid leaching solution with silicon molybdenum yellow spectrophotometry[J].Chinese Journal of Analysis Laboratory,2016,35(2):176-179.(in Chinese)
[19]HAN L,AL-DAHHAN M H.Gas–liquid mass transfer in a high pressure bubble column reactor with different sparger designs[J].Chemical Engineering Science,2007,62(1-2):131-139.
[20]NAYL A A,ISMAIL I M,ALY H F.Recovery of pure Mn SO4?H2O by reductive leaching of manganese from pyrolusite ore by sulfuric acid and hydrogen peroxide[J].International Journal of Mineral Processing,2011,100(3-4):116-123.
[21]SANTOS F M F,PINA P S,PORCARO R,OLIVEIRA V A,SILVA C A,LEAO V A.The kinetics of zinc silicate leaching in sodium hydroxide[J].Hydrometallurgy,2010,102(1-4):43-49.
[22]LEVIEN K L,LEVENSPIEL O.Optimal product distribution from laminar flow reactors:Newtonian and other power-law fluids[J].Chemical Engineering Science,1999,54(13-14):2453-2458.
[23]WANG Wei-da,FENG Ya-li,LI Hao-ran,YANG Zhi-chao,ZHANG Xu.Recovering gold from cyanide residue by alkaline predesilication-cyanide leaching technique[J].Chinese Journal of Nonferrous Metals,2015,25(1):233-240.(in Chinese)
[24]WANG Ruo-chao,ZHAI Yu-chun,NING Zhi-qiang,MA Pei-hua.Kinetics of Si O2 leaching from Al2O3 extracted slag of fly ash with sodium hydroxide solution[J].Transactions of Nonferrous Metals Society of China,2014,24(6):1928-1936.
[25]WU X,LEUNG D Y C.Optimization of biodiesel production from camelina oil using orthogonal experiment[J].Applied Energy,2011,88(11):3615-3624.