Parihar Anurag, Vongsvivut Jitraporn, Bhattacharya Sankar
Department of Chemical Engineering, Monash University, Wellington Road, Clayton 3800, Australia.
Infrared Microspectroscopy Beamline, Australian Synchrotron, 800 Blackburn Road, Clayton 3168, Australia.
ACS Omega. 2019 May 23;4(5):8747-8757. doi: 10.1021/acsomega.8b03681. eCollection 2019 May 31.
Thermo-catalytic conversion of cellulosic feedstock, such as lignocellulose, to platform chemicals offers a renewable alternative to fossil-based chemicals. Mechanistic insights behind thermochemical conversion of lignocellulose would facilitate thermo-catalytic process development for bio-based chemicals. This study employed synchrotron-based Fourier transform infrared (FTIR) microspectroscopy to investigate chemical changes in acid-catalyzed cellulose and lignocellulose and glucose during pyrolysis. Major changes in glucose occurred at 200 °C, where it underwent reactions including ring opening and tautomerization. Acid treatment did not change the molecular structure of cellulose but disrupted the lignocellulose network. The observed synchrotron FTIR spectral features provided evidence for acceleration of catalytic dehydration of cellulose and lignocellulose to levoglucosenone and furans. Catalytic passivation of alkali and alkaline earth metals in lignocellulose was also observed at low acid concentration.
将纤维素原料(如木质纤维素)热催化转化为平台化学品,为基于化石的化学品提供了一种可再生的替代方案。木质纤维素热化学转化背后的机理见解将有助于生物基化学品的热催化工艺开发。本研究采用基于同步加速器的傅里叶变换红外(FTIR)显微光谱技术,研究了酸催化的纤维素、木质纤维素和葡萄糖在热解过程中的化学变化。葡萄糖的主要变化发生在200℃,在此温度下它经历了包括开环和互变异构在内的反应。酸处理没有改变纤维素的分子结构,但破坏了木质纤维素网络。观察到的同步加速器FTIR光谱特征为纤维素和木质纤维素催化脱水生成左旋葡萄糖酮和呋喃提供了证据。在低酸浓度下还观察到木质纤维素中碱金属和碱土金属的催化钝化。