CaZr_(0.4)Fe_(0.6)O_3的水热合成及其催化热解甘蔗渣木质素制备芳香类化合物
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摘要
采用水热合成法制备CaZr_(0.4)Fe_(0.6)O_3(CZFO)钙钛矿型氧化物,对其在催化热解甘蔗渣木质素(BL)反应中的催化性能进行研究。利用XRD、SEM和Raman等方法对所制备的CZFO进行表征,考察了pH值、晶化温度、晶化时间对其晶型结构的影响。结果表明,pH=12、170℃晶化9 h,制得的CZFO结晶度最高、结构规整、呈球状且粒径均一,形成了稳定的Zr—O、Fe—O。在m(CZFO)∶m(BL)=1∶3、反应温度为550℃条件下反应2 h,液体产物收率可达29.5%。通过GC-MS分析显示出液体产物主要为酚类、苯类、苯醚类、紫丁香酚类、苯二酚类、愈创木酚类,计算得出液体产物中的6种芳香类化合物选择性为43.85%。经过3次反应-再生循环后,液体产物收率仍可达到20.3%。
Preparation of CaZr_(0.4)Fe_(0.6)O_3(CZFO)perovskite oxides by hydrothermal synthesis and their catalytic properties in the catalytic pyrolysis of bagasse lignin(BL)were studied.The prepared CZFO was characterized by XRD,SEM and Raman techniques.The effects of pH,crystallization temperature and crystallization time on the crystal structure were investigated.The results showed that the CZFO prepared at the pH of 12 and at 170 ℃ for 9 h had the highest crystallinity,regular structure,spherical shape and uniform particle size,which formed stable Zr—O and Fe—O.Under the condition of m(CZFO)∶m(BL)=1∶3 and reaction temperature of 550 ℃ for 2 h,the yield of liquid product can reach 29.5%.The GC-MS analysis showed that the liquid products were mainly phenols,benzenes,phenyl ethers,syringols,benzenediols,guaiacols,and the aromatic compound selectivity was 43.85%.After three reaction-regeneration cycles,the liquid product yield can still reach 20.3%.
Preparation of CaZr_(0.4)Fe_(0.6)O_3(CZFO)perovskite oxides by hydrothermal synthesis and their catalytic properties in the catalytic pyrolysis of bagasse lignin(BL)were studied.The prepared CZFO was characterized by XRD,SEM and Raman techniques.The effects of pH,crystallization temperature and crystallization time on the crystal structure were investigated.The results showed that the CZFO prepared at the pH of 12 and at 170 ℃ for 9 h had the highest crystallinity,regular structure,spherical shape and uniform particle size,which formed stable Zr—O and Fe—O.Under the condition of m(CZFO)∶m(BL)=1∶3 and reaction temperature of 550 ℃ for 2 h,the yield of liquid product can reach 29.5%.The GC-MS analysis showed that the liquid products were mainly phenols,benzenes,phenyl ethers,syringols,benzenediols,guaiacols,and the aromatic compound selectivity was 43.85%.After three reaction-regeneration cycles,the liquid product yield can still reach 20.3%.
引文
[1] KAWAMOTO H.Lignin pyrolysis reactions[J].Journal of Wood Science,2017,63(2):117-132.
[2] UPTON B M,KASKO A M.Strategies for the conversion of lignin to high-value polymeric materials:Review and perspective[J].Chemical Review,2015,116(4):2275-2306.
[3] 凌吉廷,陈晓晔,蒋朱克,等.木质纤维素的预处理及应用[J].粮油加工(电子版),2010(3):119-123.
[4] 陈磊,陈汉平,陆强,等.木质素结构及热解特性[J].化工学报,2014,65(9):3626-3633.
[5] LU Y,WEI X Y,ZONG Z M,et al.Structural investigation and application of lignins[J].Progress in Chemistry,2013(25):838-858.
[6] 曹双瑜,胡文冉,范玲.木质素结构及分析方法的研究进展[J].高分子通报,2012(3):8-13.
[7] ZIKELI F,TERS T,FACKLER K,et al.Wheat straw lignin fractionation and characterization as lignin-carbohydrate complexes[J].Industrial Crops and Products,2016,85:309-317.
[8] 武小芬,苏小军,陈亮,等.木质素结构分析方法研究进展[J].可再生能源,2015,33(2):267-274.
[9] 张晓华,李凝,滕俊江,等.掺杂离子的种类对介孔La0.6A0.4NiO3钙钛矿催化剂的结构与催化活性的影响[J].化工进展,2016,35(11):3542-3548.
[10] 晏耀宗,郭谨玮,陈亚中,等.La1-xCaxMnO3+δ钙钛矿催化剂制备及其甲烷催化燃烧性能研究[J].分子催化,2015,29(1):82-89.
[11] 王海,朱永法,谭瑞琴,等.非晶态配合物法制备钙钛矿型纳米粉体催化剂及其CO催化氧化性能[J].化学学报,2003,61(1):13-16.
[12] ORERA V M,PECHARROMAN C,PENA J I,et al.Vibrational spectroscopy of CaZrO3 single crystals[J].Journal of Physics:Condensed Matter,1998,10:7501-7510.
[13] ZHENG H,REANEY I M,DE G D C C,et al.Raman spectroscopy of CaTiO3-based perovskite solid solutions[J].Journal of Materials Research,2004,19(2):488-495.
[2] UPTON B M,KASKO A M.Strategies for the conversion of lignin to high-value polymeric materials:Review and perspective[J].Chemical Review,2015,116(4):2275-2306.
[3] 凌吉廷,陈晓晔,蒋朱克,等.木质纤维素的预处理及应用[J].粮油加工(电子版),2010(3):119-123.
[4] 陈磊,陈汉平,陆强,等.木质素结构及热解特性[J].化工学报,2014,65(9):3626-3633.
[5] LU Y,WEI X Y,ZONG Z M,et al.Structural investigation and application of lignins[J].Progress in Chemistry,2013(25):838-858.
[6] 曹双瑜,胡文冉,范玲.木质素结构及分析方法的研究进展[J].高分子通报,2012(3):8-13.
[7] ZIKELI F,TERS T,FACKLER K,et al.Wheat straw lignin fractionation and characterization as lignin-carbohydrate complexes[J].Industrial Crops and Products,2016,85:309-317.
[8] 武小芬,苏小军,陈亮,等.木质素结构分析方法研究进展[J].可再生能源,2015,33(2):267-274.
[9] 张晓华,李凝,滕俊江,等.掺杂离子的种类对介孔La0.6A0.4NiO3钙钛矿催化剂的结构与催化活性的影响[J].化工进展,2016,35(11):3542-3548.
[10] 晏耀宗,郭谨玮,陈亚中,等.La1-xCaxMnO3+δ钙钛矿催化剂制备及其甲烷催化燃烧性能研究[J].分子催化,2015,29(1):82-89.
[11] 王海,朱永法,谭瑞琴,等.非晶态配合物法制备钙钛矿型纳米粉体催化剂及其CO催化氧化性能[J].化学学报,2003,61(1):13-16.
[12] ORERA V M,PECHARROMAN C,PENA J I,et al.Vibrational spectroscopy of CaZrO3 single crystals[J].Journal of Physics:Condensed Matter,1998,10:7501-7510.
[13] ZHENG H,REANEY I M,DE G D C C,et al.Raman spectroscopy of CaTiO3-based perovskite solid solutions[J].Journal of Materials Research,2004,19(2):488-495.
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