Sustainable catalytic graphitization of biomass to graphitic porous carbon by constructing permeation network with organic ligands

doi:10.1016/j.cjche.2023.06.025

中国化学工程学报 ›› 2023, Vol. 64 ›› Issue (12): 259-270.DOI: 10.1016/j.cjche.2023.06.025

• Full Length Article • 上一篇下一篇

Sustainable catalytic graphitization of biomass to graphitic porous carbon by constructing permeation network with organic ligands

Pengfei Liu, Wenqiao Du, Xiangjing Liu, Long Zhang, Zhimin Chen

Jilin Provincial Engineering Laboratory for the Complex Utilization of Petro-Resources and Biomass, School of Chemical Engineering, Changchun University of Technology, Jilin 130012, China

收稿日期:2023-01-29 修回日期:2023-06-12 出版日期:2023-12-28 发布日期:2024-02-05
通讯作者: Long Zhang,E-mail:zhanglongzhl@163.com;Zhimin Chen,E-mail:chenzhimin-2009@163.com
基金资助:
This work is sponsored by the Science and Technology Research Project of Education Department of Jilin Province (JJKH20220683KJ), Natural Science Foundation of Jilin Province (20220101093JC).

Sustainable catalytic graphitization of biomass to graphitic porous carbon by constructing permeation network with organic ligands

Pengfei Liu, Wenqiao Du, Xiangjing Liu, Long Zhang, Zhimin Chen

Jilin Provincial Engineering Laboratory for the Complex Utilization of Petro-Resources and Biomass, School of Chemical Engineering, Changchun University of Technology, Jilin 130012, China

Received:2023-01-29 Revised:2023-06-12 Online:2023-12-28 Published:2024-02-05
Contact: Long Zhang,E-mail:zhanglongzhl@163.com;Zhimin Chen,E-mail:chenzhimin-2009@163.com
Supported by:
This work is sponsored by the Science and Technology Research Project of Education Department of Jilin Province (JJKH20220683KJ), Natural Science Foundation of Jilin Province (20220101093JC).

摘要/Abstract

摘要： Common strategies for catalytic graphitization of biochar into graphitic porous carbon (GPC) still face great challenges, such as the realization of simple procedures, energy conservation, and green processes. Controlling over the graphitization degree and pore structure of biochar is the key to its structural diversification. Herein, a clean and energy-efficient method is developed to synthesize adjustable graphitic degree and structure porosity GPC from rice husk-based carbon (RHC) at a relatively low temperature of 800–1000 ℃ with environment-benign organometallic catalyst ethylenediaminetetraacetic acid ferric sodium salt (EDTA-iron) and the recovery ratio of catalyst is as high as 97%. The formed by the organic ligands of EDTA-iron facilitates the etching of RHC surface and pore by iron, resulting in highly graphitized and developed porous GPCs. The pore structure and graphitization degree of GPCs can be adjusted by altering the catalyst loading, temperature, and holding time. The catalyst EDTA-iron with a lower concentration mainly plays the role of etching, which promotes the formation of porous carbon with larger surface area (S_BET = 1187.2 m²·g^-1). The catalyst with higher concentration mainly plays the role of catalyzing graphitization and promotes the obtaining of graphitic carbon with high graphitization degree (I_D/I_G = 0.19). The mechanism of EDTA-iron catalyzed graphitization of RHC is explored by the comprehensive analysis of BET, XRD, Raman, TEM and TGA. This research not only provides an efficient method for the preparation of high-quality biomass-based graphite carbon, but also provides a feasible method for the preparation of biomass-based porous carbon.

关键词: Catalytic graphitization, EDTA-iron, Rice husk, Porous carbon, Graphite

Abstract: Common strategies for catalytic graphitization of biochar into graphitic porous carbon (GPC) still face great challenges, such as the realization of simple procedures, energy conservation, and green processes. Controlling over the graphitization degree and pore structure of biochar is the key to its structural diversification. Herein, a clean and energy-efficient method is developed to synthesize adjustable graphitic degree and structure porosity GPC from rice husk-based carbon (RHC) at a relatively low temperature of 800–1000 ℃ with environment-benign organometallic catalyst ethylenediaminetetraacetic acid ferric sodium salt (EDTA-iron) and the recovery ratio of catalyst is as high as 97%. The formed by the organic ligands of EDTA-iron facilitates the etching of RHC surface and pore by iron, resulting in highly graphitized and developed porous GPCs. The pore structure and graphitization degree of GPCs can be adjusted by altering the catalyst loading, temperature, and holding time. The catalyst EDTA-iron with a lower concentration mainly plays the role of etching, which promotes the formation of porous carbon with larger surface area (S_BET = 1187.2 m²·g^-1). The catalyst with higher concentration mainly plays the role of catalyzing graphitization and promotes the obtaining of graphitic carbon with high graphitization degree (I_D/I_G = 0.19). The mechanism of EDTA-iron catalyzed graphitization of RHC is explored by the comprehensive analysis of BET, XRD, Raman, TEM and TGA. This research not only provides an efficient method for the preparation of high-quality biomass-based graphite carbon, but also provides a feasible method for the preparation of biomass-based porous carbon.

Key words: Catalytic graphitization, EDTA-iron, Rice husk, Porous carbon, Graphite

Pengfei Liu, Wenqiao Du, Xiangjing Liu, Long Zhang, Zhimin Chen. Sustainable catalytic graphitization of biomass to graphitic porous carbon by constructing permeation network with organic ligands[J]. 中国化学工程学报, 2023, 64(12): 259-270.

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Sustainable catalytic graphitization of biomass to graphitic porous carbon by constructing permeation network with organic ligands

Sustainable catalytic graphitization of biomass to graphitic porous carbon by constructing permeation network with organic ligands

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