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在低温条件下,由硝酸铁催化的生物质基石墨碳的制备及形成机理。

Preparation and formation mechanism of biomass-based graphite carbon catalyzed by iron nitrate under a low-temperature condition.

机构信息

College of Engineering, Huazhong Agricultural University, No. 1, Shizishan Street, Hongshan District, Wuhan, 430070, PR China.

College of Engineering, Huazhong Agricultural University, No. 1, Shizishan Street, Hongshan District, Wuhan, 430070, PR China; Key Laboratory of Agricultural Equipment in the Mid-lower Yangtze River, Ministry of Agriculture, Wuhan, 430070, PR China.

出版信息

J Environ Manage. 2022 Sep 15;318:115555. doi: 10.1016/j.jenvman.2022.115555. Epub 2022 Jun 20.

Abstract

Graphite is a widely used industrial material, which experienced a marked shortage caused by the growing demand for electrode anode material and the increased costs for raw material. Graphitic carbon from biomass is a promising approach that will result in low-cost and efficient preparation. Herein, Fe(NO) was selected as the catalyst for pine sawdust, and the effects of temperature and iron content on the graphitization of biochar were investigated. Additionally, the formation mechanism of the graphitic crystallite structure was explored. Results showed that the formation of pyrolysis gas increased with the increase in the amount of catalyst added or pyrolysis temperature. The change in pyrolysis gas, such as H and CO, was a critical auxiliary factor reflecting the conversion process. As temperature was increased from 600 °C to 800 °C, the solid products showed high graphitization and low solid yield. Graphite structure mainly formed at 700 °C because of the formation of Fe nanoparticles. The increase in the amount of catalyst could provide more reaction sites and promote the contact between Fe and C, showing that amorphous carbon is dissolved on Fe nanoparticles and precipitated into ordered graphitic carbon. On this basis, a mechanism of "carbon dissolution-precipitation" was proposed to explain the formation of graphite structure, and the whole pyrolysis process included the transformation of the iron element were analyzed.

摘要

石墨是一种广泛应用的工业材料,由于对电极阳极材料的需求不断增长以及原材料成本的增加,其经历了明显的短缺。生物质衍生的石墨化碳是一种很有前途的方法,将导致低成本和高效的制备。在此,选择 Fe(NO)作为催化剂用于木屑,研究了温度和铁含量对生物炭石墨化的影响。此外,还探讨了石墨微晶结构的形成机理。结果表明,随着催化剂用量或热解温度的增加,热解气体的形成增加。热解气体(如 H 和 CO)的变化是反映转化过程的关键辅助因素。随着温度从 600°C 升高到 800°C,固体产物表现出高石墨化和低固收率。由于 Fe 纳米颗粒的形成,石墨结构主要在 700°C 形成。催化剂用量的增加可以提供更多的反应位点,并促进 Fe 和 C 之间的接触,表明无定形碳溶解在 Fe 纳米颗粒上,并沉淀成有序的石墨碳。在此基础上,提出了“碳溶解-沉淀”的机理来解释石墨结构的形成,并对整个热解过程中 Fe 元素的转化进行了分析。

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