He Zhisen, Liu Shanjian, Zhao Wenjing, Yin Mengqian, Jiang Mei, Bi Dongmei
School of Agricultural Engineering and Food Science, Shandong University of Technology, Zibo255049, China.
ACS Omega. 2022 Dec 19;8(1):1232-1239. doi: 10.1021/acsomega.2c06643. eCollection 2023 Jan 10.
This study aimed to investigate the effect of the urea content on the characteristics and distribution of nitrogen-rich bio-oil and nitrogen-doped biochar. Cellulose, cellobiose, and glucose were used as feedstock. Urea was used as the exogenous nitrogen source in nitrogen-rich pyrolysis at 500 °C. The order of the nitrogen increase in the nitrogen-doped biochar was cellulose < cellobiose < glucose. Nitrogen-doped biochar consisted of abundant nitrogen and nitrogenous functional groups, and the stability of biochar was optimal. The nitrogen-doped biochar obtained from cellulose showed the optimal adsorption performance for diethyl phthalate with 50% urea addition. When the proportion of urea was 20%, the content of anhydro-sugars in bio-oil reached the maximum value (61.86%). Furans and other small-molecule oxygenates were intermediates to produce nitrogenous heterocyclic compounds (NHCs) from cellulose. When the proportion of urea was 40%, the bio-oil had the highest selectivity (91.63%) of NHCs. The NHCs in the obtained bio-oil mainly consisted of pyrroles, pyrimidines, pyridines, imidazoles, and pyrazines. Therefore, the excellent proportion of urea in the blend could promote the generation of high-value NHCs and nitrogen-doped biochar from the nitrogen-rich pyrolysis of cellulose (and its model compounds).
本研究旨在探究尿素含量对富氮生物油和氮掺杂生物炭的特性及分布的影响。以纤维素、纤维二糖和葡萄糖作为原料。在500℃的富氮热解过程中,使用尿素作为外源氮源。氮掺杂生物炭中氮含量的增加顺序为纤维素<纤维二糖<葡萄糖。氮掺杂生物炭含有丰富的氮和含氮官能团,且生物炭的稳定性最佳。由纤维素制得的氮掺杂生物炭在添加50%尿素时对邻苯二甲酸二乙酯表现出最佳吸附性能。当尿素比例为20%时,生物油中脱水糖的含量达到最大值(61.86%)。呋喃和其他小分子含氧化合物是纤维素生成含氮杂环化合物(NHCs)的中间体。当尿素比例为40%时,生物油对NHCs的选择性最高(91.63%)。所得生物油中的NHCs主要由吡咯、嘧啶、吡啶、咪唑和吡嗪组成。因此,混合体系中尿素的适宜比例能够促进纤维素(及其模型化合物)富氮热解生成高价值的NHCs和氮掺杂生物炭。