硫酸铵分解过程及其热分解动力学研究
收稿日期: 2022-03-08
网络出版日期: 2023-10-16
Study on decomposition process and thermal decomposition kinetics of ammonium sulfate
Received date: 2022-03-08
Online published: 2023-10-16
硫酸铵热分解能为硫酸氢铵溶液浸出粉煤灰提取氧化铝工艺过程提供硫酸氢铵溶液和氨水，研究硫酸铵热分解过程的机理和热分解动力学具有重要意义。通过X射线衍射、质谱和傅里叶变换红外光谱等对硫酸铵热分解过程的产物进行了表征，结果表明硫酸铵的热分解产物为硫酸氢铵、焦硫酸铵、氨气、水、氮气和二氧化硫。采用X射线衍射、质谱和傅里叶变换红外光谱等表征方法并与热重分析技术联用对硫酸铵进行了分析，结果发现硫酸铵的热分解过程分为3个阶段：硫酸铵分解形成硫酸氢铵和氨气；硫酸氢铵脱水形成焦硫酸铵；焦硫酸铵分解。采用Ozawa-Flynn-Wall和Kissinger-Akahira-Sunose无模型方法计算每个阶段的活化能。采用Coats-Redfern方法确定每个阶段最可能的机理函数。结果表明：第一阶段的平均活化能（E）为125.21 kJ/mol，ln A为18.46；第二阶段的平均活化能（E）为110.21 kJ/mol，ln A为13.94；第三阶段的平均活化能（E）为97.70 kJ/mol，ln A为8.44。
吴迪 , 李来时 , 王俊凯 , 吴玉胜 , 王昱征 , 李明春 . 硫酸铵分解过程及其热分解动力学研究[J]. 无机盐工业, 2023 , 55(10) : 86 -92 . DOI: 10.19964/j.issn.1006-4990.2022-0105
Thermal decomposition of ammonium sulfate can provide ammonium bisulfate solution and ammonia water for the process of leaching fly ash with ammonium bisulfate solution to extract alumina.It is of great significance to study the mechanism and thermal decomposition kinetics of its thermal decomposition process.The products of the decomposition process were characterized by X-ray diffraction，mass spectrometry and Fourier transform infrared spectroscopy，proving that the decomposition products of ammonium sulfate were ammonium hydrogen sulfate，ammonium pyrosulfate，ammonia，water，nitrogen and sulfur dioxide.The characterization method combined with thermogravimetric analysis showed that the thermal decomposition process of ammonium sulfate was divided into three stages：the decomposition of ammonium sulfate to form ammonium bisulfate and ammonia gas，the dehydration of ammonium bisulfate to form ammonium pyrosulfate，and the decomposition of ammonium pyrosulfate.The Ozawa-Flynn-Wall and Kissinger-Akahira-Sunose model-free methods were used to calculate the activation energy for each stage.The Coats–Redfern method was used to determine the most likely dyna-mic mechanism function for each stage.The results showed that the average activation energy was E=125.21 kJ/mol in the first stage，and ln A=18.46；the average activation energy of the second stage was E=110.21 kJ/mol and ln A=13.94；the average activation energy of the third stage was E=97.70 kJ/mol and ln A=8.44.
| 1 | 韦聚才，石霖，吴旭.膜电极电解器电解脱硫废水制备硫酸铵副产氢［J］.电化学，2022，28（5）：4-12. |
| WEI Jucai， SHI Lin， WU Xu.Simultaneous hydrogen and （NH4）2SO4 productions from desulfurization wastewater electrolysis using MEA electrolyser［J］.Journal of Electrochemistry，2022，28（5）：4-12. | |
| 2 | ALAM T， SURYANTO P， KASTONO D，et al.Interactions of biochar briquette with ammonium sulfate fertilizer for controlled nitrogen loss in soybean intercopping with melaleuca cajuputi［J］.Legume Research，2021，44：339-343. |
| 3 | YIN Shu， ALDAHRI T， ROHANI S，et al.Insights into the roasting kinetics and mechanism of blast furnace slag with ammonium sulfate for CO2 mineralization［J］.Industrial & Engineering Chemistry Research，2019，58：14026-14036. |
| 4 | BATTISTA F， MASALA C， ZAMBONI A，et al.Valorisation of agricultural digestate for the ammonium sulfate recovery and soil improvers production［J］.Waste and Biomass Valorization，2021，12（12）：6903-6916. |
| 5 | SONG Xingfu， ZHAO Jingcai， LI Yunzhao，et al.Thermal decomposition mechanism of ammonium sulfate catalyzed by ferric oxi-de［J］.Frontiers of Chemical Science and Engineering，2013，7（2）：210-217. |
| 6 | KIYOURA R， URANO K.Mechanism，kinetics，and equilibrium of thermal decomposition of ammonium sulfate［J］.Industrial & Engineering Chemistry Process Design and Development，1970，9（4）：489-494. |
| 7 | KUMMER J T.Thermal decomposition of ammonium nitrate［J］.Journal of the American Chemical Society，1947，69（10）.Doi：10.1021/ja01202a507. |
| 8 | DIXON P.Formation of sulphamic acid during the thermal decomposition of ammonium sulphate［J］.Nature，1944，154（3918）：706. |
| 9 | ZHU Zhenping， NIU Hongxian， LIU Zhenyu，et al.Decomposition and reactivity of NH4HSO4 on V2O5/AC catalysts used for NO reduction with ammonia［J］.Journal of Catalysis，2000，195（2）：268-278. |
| 10 | LI Jie， LI Yandong， DUAN Huamei，et al.Experimental and kinetic study of magnesium extraction and leaching from laterite nickel ore by roasting with ammonium sulfate［J］.Russian Journal of Non-Ferrous Metals，2018，59（6）：596-604. |
| 11 | WU Yan， XIN Haixia， XU Yujun，et al.Preparation of ultrafine α-Al2O3 powder from fly ash by ammonium sulfate roasting technology［J］.Journal of Physics：Conference Series，2019，1347（1）.Doi：10.1088/1742-6596/1347/1/012111. |
| 12 | ZHANG Xianghui， HE Chuan， WANG Ling，et al.Non-isothermal kinetic analysis of thermal dehydration of La2（CO3）3·3.4H2O in air［J］.Transactions of Nonferrous Metals Society of China，2014，24（10）：3378-3385. |
| 13 | LIAN Jingbao， LIU Fan， ZHANG Jing，et al.Template-free hydrothermal synthesis of Gd2O2SO4：Eu3+ hollow spheres based on urea-ammonium sulfate （UAS） system［J］.Optik，2016，127（20）：8621-8628. |
| 14 | KIEFER W.Recent advances in linear and nonlinear Raman spectroscopy I［J］.Journal of Raman Spectroscopy，2007，38（12）：1538-1553. |
| 15 | ANTO P L， ANTO R J， VARGHESE H T，et al.FT-IR，FT-Raman and SERS spectra of anilinium sulfate［J］.Journal of Raman Spectroscopy，2009，40（12）：1810-1815. |
| 16 | ZAIRI I， GARCíA-GRANDA S， LITAIEM H.Optical，thermal，vibrational and structural investigation to characterize phase transitions in the ammonium sulfate tellurate［J］.Journal of Molecular Structure，2021，1242.Doi：10.1016/J.MOLSTRUC.2021.130816. |
| 17 | JAYARAMAN K， K?K M V， G?KALP I.Combustion mechanism and model free kinetics of different origin coal samples：Thermal analysis approach［J］.Energy，2020，204.Doi：10.1016/j.energy.2020.117905. |
| 18 | ZHANG Wei， WANG Chang'an， LI Guangyu，et al.TG analysis and kinetic study of organic constituents in wastewater from coal-gasification process［J］.Asia-Pacific Journal of Chemical Engineering，2017，12（3）：406-414. |
| 19 | 赵鹏达，倪珊梅，宋小文，等.可见光诱导8-氨基喹啉衍生物二氟烷基化反应［J］.精细化工，2020，37（8）：1678-1683. |
| ZHAO Pengda， NI Shanmei， SONG Xiaowen，et al.Visible light induced difluoroalkylation of 8-aminoquinoline derivatives［J］.Fine Chemicals，2020，37（8）：1678-1683. | |
| 20 | SBIRRAZZUOLI N.Determination of pre-exponential factor and reaction mechanism in a model-free way［J］.Thermochimica Acta，2020，691.Doi：10.1016/j.tca.2020.178707. |
| 21 | 阎杰，谢军，宋丽华，等.煤与焦油、秸秆混合压球共热解的动力学［J］.煤炭学报，2018，43（7）：2052-2060. |
| YAN Jie， XIE Jun， SONG Lihua，et al.Kinetics of co-pyrolysis of coal，tar and straw mixed briquette［J］.Journal of China Coal Society，2018，43（7）：2052-2060. | |
| 22 | SINGH S， PATIL T， TEKADE S P，et al.Studies on individual pyrolysis and co-pyrolysis of corn cob and polyethylene：Thermal degradation behavior，possible synergism，kinetics，and thermodynamic analysis［J］.Science of the Total Environment，2021，783.Doi：10.1016/j.scitotenv.2021.147004. |
| 23 | ASHRAF A， SATTAR H， MUNIR S.A comparative applicability study of model-fitting and model-free kinetic analysis approaches to non-isothermal pyrolysis of coal and agricultural residues［J］.Fuel，2019，240：326-333. |
| 24 | HU Jinghui， GONG Li， HE Jiyu，et al.Studies on multistep thermal decomposition behavior of polytriazole polyethylene oxide-tetrahydrofuran elastomer［J］.Polymers for Advanced Technologies，2020，31（4）：749-758. |
| 25 | 周绿山.硫酸铵与硫酸氢铵混合物催化热分解过程研究［D］.昆明：昆明理工大学，2014. |
/
| 〈 |
|
〉 |
