无烟煤的溶胀行为及对其电解液化的影响
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摘要
本文系统地研究了无烟煤的溶胀行为,及其对无烟煤电催化加氢液化的促进效果.研究结果表明,作为高阶煤的无烟煤,其溶胀行为和低阶煤(褐煤)不同,非极性溶剂的溶胀效果优于极性溶剂.在所研究的多种有机溶胀剂中,苯对无烟煤的溶胀效果最佳,60℃下溶胀度可达4.01.研究发现,在溶胀过程中溶胀剂分子在煤大分子网络结构中的渗入可使无烟煤体积膨胀,促进煤结构疏松化以及使煤颗粒变小;同时溶胀剂分子与煤大分子的相互作用力可以破坏原煤中的部分化学键结构并产生小分子物种,进一步削弱了煤大分子的网络结构,促进煤的溶胀度提高.研究还表明,引入溶胀促进剂Fe(NO3)3可与有机溶胀剂产生协同溶胀作用从而进一步促进煤的溶胀,提高煤的溶胀度.对于无烟煤的溶胀处理,有利于其电催化加氢液化反应的活性,大大提高了无烟煤的电解液化率,使其电解液化率由原煤的32.04%提高到63.19%.
Swelling behavior of anthracite and its effect on the electrochemical hydrogenation of the coal has been studied.It has been found that,different from low rank coal such as lignite,the swelling effect of high rank coal anthracite by using nonpolar solvent is better than that of polar solvent.Among several solvents employed in this study,benzene presents the best swelling effect for anthracite,i.e.the swelling ratio is up to 4.01 at 60℃.During the swelling process,the permeation of swelling solvent into the macromolecular network of anthracite leads to the expansion of coal particle,resulting in loose and porous,even fragmentized coal particles.Moreover,the interaction between swelling solvent and coal macromolecule can partially break the chemical bonds in anthracite and release small molecules,which can further damage the network structure of coal and promote the swelling degree of coal.Furthermore,the synergistic swelling effect between Fe(NO3)3and swelling solvent can further promote the swelling of anthracite,and then improve the following electrochemical reaction activity.The swelling of anthracite can improve the electrolysis liquefaction reactivity of anthracite and benefit to the liquefaction yield,which is increased from 32.04%to 63.19%.
Swelling behavior of anthracite and its effect on the electrochemical hydrogenation of the coal has been studied.It has been found that,different from low rank coal such as lignite,the swelling effect of high rank coal anthracite by using nonpolar solvent is better than that of polar solvent.Among several solvents employed in this study,benzene presents the best swelling effect for anthracite,i.e.the swelling ratio is up to 4.01 at 60℃.During the swelling process,the permeation of swelling solvent into the macromolecular network of anthracite leads to the expansion of coal particle,resulting in loose and porous,even fragmentized coal particles.Moreover,the interaction between swelling solvent and coal macromolecule can partially break the chemical bonds in anthracite and release small molecules,which can further damage the network structure of coal and promote the swelling degree of coal.Furthermore,the synergistic swelling effect between Fe(NO3)3and swelling solvent can further promote the swelling of anthracite,and then improve the following electrochemical reaction activity.The swelling of anthracite can improve the electrolysis liquefaction reactivity of anthracite and benefit to the liquefaction yield,which is increased from 32.04%to 63.19%.
引文
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[27] LI X,HU S X,JIN L J,et al.Role of iron-based catalyst and hydrogen transfer in direct coal liquefaction[J].Energy&Fuels,2008,22(2):1126-1129.
[28]王知彩.神华煤的预处理及其新型固体酸催化液化研究[D].上海:华东理工大学,2007.
[29]刘缠民,宗志敏,贾吉仙,等.N-甲基-2-吡咯烷酮与3种国产烟煤中某些有机物的强烈缔合作用[J].科学通报,2008,53(2):183-190.
[30] SUN B L,YU J L,TAHMASEBI A,et al.An experimental study on binderless briquetting of Chinese lignite:Effects of briquetting conditions[J].Fuel Processing Technology,2014,124:243-248.
[2] LIU S,ZHOU W,TANG F,et al.Pretreatment of coal by ionic liquids towards coal electrolysis liquefaction[J].Fuel,2015,160:495-501.
[3] LIU S,ZHOU W,YU T,et al.Preparation of layered nanoporous Ti/TiO2/Ni-W-B electrode for electrocatalytic reduction of coal[J].Fuel,2014,134:151-158.
[4] LIU Y L,ZHOU W,FAN C Q,et al.Electrochemical hydrogenation of coal on Ni-based catalysts[J].Fuel,2014,122:54-59.
[5] MOCHIDA I,OKUMA O,YOON S H.Chemicals from direct coal liquefaction[J].Chemical reviews,2014,114(3):1637-1672.
[6]汤芳,周尉,曹为民,等.二元溶剂[Bmim]Cl+NMP对褐煤的溶胀及电解液化的影响[J].复旦学报(自然科学版),2016,55(6):725-731.
[7] NISHIOKA M,LARSEN J.Association of aromatic structures in coals[J].Energy&Fuels,1990,4(1):100-106.
[8] TAKANOHASHI T,IINO M,NISHIOKA M.Investigation of associated structure of Upper Freeport coal by solvent swelling[J].Energy&Fuels,1995,9(5):788-793.
[9] OTAKE Y,SUUBERG E M.Temperature dependence of solvent swelling and diffusion processes in coals[J].Energy&fuels,1997,11(6):1155-1164.
[10] OTAKE Y,SUUBERG E M.Solvent swelling rates of low rank coals and implications regarding their structure[J].Fuel,1998,77:901-904.
[11] SAKANISHI K,WATANABE I,NONAKA T,et al.Effects of organic acid pretreatment on the structure and pyrolysis reactivity of coals[J].Fuel,2001,8:273-281.
[12] PANDE S,SHARMA D.Studies of kinetics of diffusion of N-methyl-2-pyrrolidone(NMP),ethylenediamine(EDA),and NMP+EDA(1∶1,vol/vol)mixed solvent system in chinakuri coal by solvent swelling techniques[J].Energy&Fuels,2001,15(5):1063-1068.
[13] MATHEWS J P,BURGESS-CLIFFORD C,PAINTER P,.Interactions of Illinois No.6bituminous coal with solvents:A review of solvent swelling and extraction literature[J].Energy&Fuels,2015,29(3):1279-1294.
[14]常鸿雁,张德祥,韩文煜,等.不同温度下煤在溶剂中的溶胀行为[J].华东理工大学学报,2004,30(4):406-409.
[15]陈茺,许学敏,高晋生,等.氢键在煤大分子溶胀行为中的作用[J].燃料化学学报,1997,25(6):45-48.
[16]常鸿雁,韩文煜,张德祥,等.神华煤在有机溶剂中溶胀动力学的研究[J].煤炭转化,2005,28(2):25-28.
[17]王敬空.溶剂处理对低阶煤的溶胀与扩散性能的影响研究[D].马鞍山:安徽工业大学,2017.
[18]柳厚田,梁海河,杨炯,等.阳极Pb(Ⅱ)氧化物膜的阴极还原[J].化学学报,2002,60(3):427-431.
[19]王勇.溶胀预处理对煤结构及煤液化性能的影响[D].大连:大连理工大学,2000.
[20]戈军,郭龙德,郭智慧,等.溶剂与溶胀促进剂对神华煤溶胀行为的影响[J].化工进展,2010,29(10):1885-1889.
[21]李沙沙,侯丽红,刘惠青,等.煤溶胀影响因素及溶胀技术的应用[J].洁净煤技术,2012,18(2):31-34,59.
[22]李沙沙.两种低阶烟煤溶胀特性和分子量研究[D].太原:太原理工大学,2013.
[23]张晓娟,盛清涛,申峻,等.煤溶胀动力学与热力学的研究[J].洁净煤技术,2013,19(5):77-81,91.
[24]李沙沙,盛清涛,范济民,等.鑫源煤在有机溶剂中的溶胀特性研究[J].煤炭转化,2014,37(1):11-14,22.
[25] YIN J N,HANG F T,AN L H,et al.Research progress of organic solvent extraction of low rank coal[J].Clean Coal Technology,2014,20(6):100-103.
[26] LI X,HU H Q,ZHU,S W,et al.Kinetics of coal liquefaction during heating-up and isothermal stages[J].Fuel,2008,87:508-513.
[27] LI X,HU S X,JIN L J,et al.Role of iron-based catalyst and hydrogen transfer in direct coal liquefaction[J].Energy&Fuels,2008,22(2):1126-1129.
[28]王知彩.神华煤的预处理及其新型固体酸催化液化研究[D].上海:华东理工大学,2007.
[29]刘缠民,宗志敏,贾吉仙,等.N-甲基-2-吡咯烷酮与3种国产烟煤中某些有机物的强烈缔合作用[J].科学通报,2008,53(2):183-190.
[30] SUN B L,YU J L,TAHMASEBI A,et al.An experimental study on binderless briquetting of Chinese lignite:Effects of briquetting conditions[J].Fuel Processing Technology,2014,124:243-248.
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