Zhang Xurui, Chen Zezhou, Cheng Long, Xu Linlin, Bi Xiaotao, Liu Qingya
Clean Energy Research Center, Department of Chemical and Biological Engineering, The University of British Columbia, BC V6T 1Z3, Canada; State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
College of Engineering, Huzhou University, Huzhou 313000, China.
J Hazard Mater. 2022 Feb 15;424(Pt A):127297. doi: 10.1016/j.jhazmat.2021.127297. Epub 2021 Sep 24.
Large volumes of waste petroleum coke stockpiled in open yard not only represent a huge loss of valuable material but also pose a significant risk to the environment. This work proposed an innovative strategy for waste petroleum coke valorization by exploring its catalytic performance of biomass gasification tar destruction. Waste petroleum coke was firstly activated by potassium hydroxide (KOH) to obtain high specific surface area as well as low sulfur and ash contents. Petroleum coke derived catalyst showed superior performance than a commercial activated carbon derived catalyst for destruction of naphthalene as the tar model compound. The petroleum coke derived catalyst exhibited 99.1% naphthalene destruction efficiency at 800 °C but deactivated quickly under N atmosphere. Under H and steam atmospheres, the catalytic activities were 98.6% and 96.5% for 8 h, respectively. To study the correlation between catalytic performance and the structure of carbon catalyst, elemental analysis, scanning electron microscope (SEM) analysis, transmission electron microscope (TEM) analysis, X-ray powder diffraction (XRD) analysis, Brunauer-Emmett-Teller method (BET) analysis, Fourier transform infrared (FTIR) spectroscopy, temperature programmed oxidation (TPO) analysis and Raman spectroscopy were performed on both fresh and spent catalysts. Results demonstrated that the hydrogen-rich groups (small rings and amorphous carbon) and oxygen-containing groups may account for the good resistance to coke deposition under H and steam atmospheres.
大量露天堆放的废石油焦不仅意味着宝贵材料的巨大损失，还对环境构成重大风险。这项工作通过探索废石油焦对生物质气化焦油的催化破坏性能，提出了一种创新的废石油焦增值策略。首先用氢氧化钾（KOH）对废石油焦进行活化，以获得高比表面积以及低硫和低灰分含量。以萘作为焦油模型化合物，石油焦衍生的催化剂在破坏萘方面表现出比商业活性炭衍生的催化剂更优异的性能。该石油焦衍生的催化剂在800℃时萘的破坏效率为99.1%，但在氮气气氛下会迅速失活。在氢气和蒸汽气氛下，催化活性分别在8小时内保持为98.6%和96.5%。为了研究催化性能与碳催化剂结构之间的相关性，对新鲜催化剂和失活催化剂都进行了元素分析、扫描电子显微镜（SEM）分析、透射电子显微镜（TEM）分析、X射线粉末衍射（XRD）分析、布鲁诺尔-埃米特-泰勒法（BET）分析、傅里叶变换红外（FTIR）光谱、程序升温氧化（TPO）分析和拉曼光谱分析。结果表明，富含氢的基团（小环和无定形碳）以及含氧基团可能是在氢气和蒸汽气氛下对焦炭沉积具有良好抗性的原因。
