Boosting the Conversion of CO2 with Biochar to Clean CO in an Atmospheric Plasmatron: A Synergy of Plasma Chemistry and Thermochemistry

等离子管 生物炭 热化学 化学 热解 一氧化碳 甲烷 分析化学(期刊) 化学工程 等离子体 无机化学 环境化学 有机化学 催化作用 量子力学 物理 工程类
作者
Hao Zhang,Qinhuai Tan,Qunxing Huang,Kaiyi Wang,Xin Tu,Xiaotong Zhao,Chunfei Wu,Jianhua Yan,Xiaodong Li
出处
期刊:ACS Sustainable Chemistry & Engineering [American Chemical Society]
卷期号:10 (23): 7712-7725 被引量:69
标识
DOI:10.1021/acssuschemeng.2c01778
摘要

In this work, the conversion of CO 2 into O 2 -free CO has been investigated in an atmospheric plasmatron via the reaction with biochar. The effects of the biochar source, pyrolysis temperature for biochar preparation, and gas–solid reaction patterns (fixed bed and fluidized bed) on the reaction performance were evaluated under different feed flow rates. The underlying mechanisms were explored using in situ optical emission spectroscopy focusing on understanding the role of plasma chemistry and thermochemistry in CO 2 conversion. The results revealed that the presence of both biochar and plasma significantly facilitate CO 2 conversion. In comparison to thermal CO 2 splitting, the plasmatron CO 2 + C process dramatically enhanced the CO 2 conversion from 0 to 27.1%. Walnut shell biochar prepared at relatively high pyrolysis temperatures favored CO 2 conversion due to a high carbon content. A fixed bed surprisingly provided remarkably better performance than a fluidized bed for the CO 2 + C reaction, benefiting from a prompt consumption of the generated O 2 by biochar. The high electron density achieved in the plasmatron (10 15 cm –3 ) allows for a high processing capacity, and the moderate electron temperature (1.1–1.5 eV) with enhanced vibrational energy (6300–8200 K) obtained stimulates the most efficient CO 2 activation routes through vibrational excitation. The relatively high rotational (gas) temperatures in the core plasma area (2100–2400 K) and in the gas–solid reaction region (<1573 K) detrimentally drive the reverse reactions of CO 2 splitting and advantageously boost the biochar-involved reactions, respectively, by thermochemistry. The synergy of plasma-chemistry-dominated CO 2 dissociation and the thermochemistry-dominated CO 2 + C and O 2 + C reactions accounts for the high CO 2 conversion obtained in the plasmatron CO 2 + C process. The immediate study provides a novel route for efficient CO 2 conversion by coupling plasma chemistry and thermochemistry.
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