2022年 01期

超声辅助脱除煤中的有机硫

Ultrasonic-assisted Removal of Organic Sulfur from Coal


摘要(Abstract):

为了研究超声辅助过氧化氢-乙酸氧化脱除煤中有机硫的机理,选取4种脱灰煤和6种含硫模型化合物作为研究对象,探讨反应温度、反应时间和超声功率对有机硫的脱除影响;采用X射线光电子能谱、傅里叶变换红外光谱、扫描电子显微镜等手段,对脱硫处理前、后的样品进行表征。结果表明:超声辅助过氧化氢-乙酸脱硫时,有机硫化物硫的含量越高,脱硫率越大;煤中以苄硫醇、二苄基二硫和二苄基硫醚形态存在的硫更容易被转化为高价态的SO_4~(2-)而被除去。

关键词(KeyWords): 有机硫;脱硫;超声波;含硫模型化合物

基金项目(Foundation): 国家自然科学基金项目(21666001);; 宁夏自然科学基金项目(2020AAC03208,2019AAC03112);; 北方民族大学研究生创新项目(YCX20137)

作者(Author): 丁宁,金权,李梅,岳劲松,孙功成,程雪云,高彩云

DOI: 10.13349/j.cnki.jdxbn.20211012.001

参考文献(References):

[1] BHATTACHARYA M,RAFIQ S,BHATTACHARYA S.The role of technology on the dynamics of coal consumption-economic growth:new evidence from China[J].Applied Energy,2015,154:686-695.

[2] CHEN L,BHATTACHARYA S.Sulfur emission from Victorian brown coal under pyrolysis,oxy-fuel combustion and gasification conditions[J].Environmental Science & Technology,2013,47(3):1729-1734.

[3] WANG X J,LI F T,LIU J X,et al.Preparation of TiO2 in ionic liquid via microwave radiation and in situ photocatalytic oxidative desulfurization of diesel oil[J].Energy & Fuels,2012,26(11):6777-6782.

[4] LIU X Y,LIN B Q,ZHANG Y J.Sulfur dioxide emission reduction of power plants in China:current policies and implications[J].Journal of Cleaner Production,2016,113:133-143.

[5] LI Z,FU Y H,ZHOU A N,et al.Effect of multi-intensification on the liberation of maceral components in coal[J].Fuel,2019,237:1003-1012.

[6] WAN M J,SHEN Y F,HU Y F,et al.Effect of pre-desulfurization process on the sulfur forms and their transformations during pyrolysis of Yanzhou high sulfur coal[J].Fuel,2020,276:118124.

[7] WANG L Y,JIN G S,XU Y L.Desulfurization of coal using four ionic liquids with [HSO4][J].Fuel,2019,236:1181-1190.

[8] GAUDINO E C,CARNAROGLIO D,BOFFA L,et al.Efficient H2O2/CH3COOH oxidative desulfurization/denitrification of liquid fuels in sonochemical flow-reactors[J].Ultrasonics Sonochemistry,2014,21(1):283-288.

[9] FAN Q,ZHAO D,DAI Y.The research of ultra-deep desulfurization in diesel via ultrasonic irradiation under the catalytic system of H2O2-CH3COOH-FeSO4[J].Petroleum Science and Technology,2009,27(3):302-314.

[10] HARUNA S Y,FARUQ U Z,ZUBAIRU A Y,et al.Comparative studies on reduction of sulphur content of heavy crude oil using KMnO4+H2O2/CH3COOH and KMnO4+H2O2 /HCOOH via oxidative desulphurization (ODS)[J].American Journal of Applied Chemistry,2018,6(1):15-24.

[11] LEVENT M,KAYA ?,KOCAKERIM M,et al.Optimization of desulphurization of Artvin-Yusufeli lignite with acidic hydrogen peroxide solutions[J].Fuel,2006,86(7/8):983-992.

[12] NEMETH L,BARE S R,RATHBUN W,et al.Oxidative desulfurization of sulfur compounds:oxidation of thiophene and derivatives with hydrogen peroxide using Ti-Beta catalyst[J].Studies in Surface Science and Catalysis,2008,174(Part B):1017-1020.

[13] BORAH D,BARUAH M K,HAQUE I.Oxidation of high sulphur coal:3:desulphurisation of organic sulphur by peroxyacetic acid (produced in situ) in presence of metal ions[J].Fuel Processing Technology,2005,86(9):959-976.

[14] 李国良,王西奎,王金刚,等.空化降解水中有机污染物的研究进展[J].济南大学学报(自然科学版),2007,21(1):34-37.

[15] 孙成江,邱立平,王嘉斌,等.低强度超声辐射对活性污泥微生物种群结构及活性的影响[J].济南大学学报(自然科学版),2014,28(5):395-400.

[16] ALBAYRAK A T,GURKAYNAK M A.Sonocatalytic oxidative desulfurization of thiophene and its derivatives[J].Procedia Engineering,2012,42:1711-1719.

[17] SAIKIA B K,DUTTA A M,BARUAH B P.Feasibility studies of de-sulfurization and de-ashing of low grade medium to high sulfur coals by low energy ultrasonication[J].Fuel,2014,123:12-18.

[18] 韩玥.不同脱硫剂脱除煤中硫的研究[J].煤炭转化,2010,33(3):56-58.

[19] TANG L F,FAN H D,GUO J F,et al.Investigation on the mechanism of coal desulfurization by ultrasonic with peroxyacetic acid[J].Energy Sources:Part A:Recovery,Utilization,and Environmental Effects,2018,40(8):999-1009.

[20] ACHOLLA F V,ORR W L.Pyrite removal from kerogen without altering organic matter:the chromous chloride method[J].Energy Fuels,1993,7(3):406-410.

[21] 李梅,金权,孙功成,等.微波辅助脱除煤中有机硫的机理研究[J].燃料化学学报,2019,47(10):1153-1162.

[22] 曾维晨.炼焦煤微波与超声波联合脱硫研究[D].徐州:中国矿业大学,2015.

[23] QIN Z H,ZHANG H F,DAI D J,et al.Study on occurrence of sulfur in different group components in Xinyu clean coking coal[J].燃料化学学报,2014,42(11):1286-1294.

[24] SHAIDA M A,SEN A K,DUTTA R K.Alternate use of sulphur rich coals as solar photo-Fenton agent for degradation of toxic azo dyes[J].Journal of Cleaner Production,2018,195:1003-1014.

[25] 代世峰,任德贻,宋建芳,等.应用XPS研究镜煤中有机硫的存在形态[J].中国矿业大学学报,2002,31(3):225-228.