从纤维素中设计用于CO2吸附的杂原子掺杂生物炭:N和S的竞争行为和相互作用的新视角

IF 13.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Biochar Pub Date : 2023-11-22 DOI:10.1007/s42773-023-00275-1
Yuxuan Sun, Jixiu Jia, Zhidan Liu, Ziyun Liu, Lili Huo, Lixin Zhao, Yanan Zhao, Zonglu Yao
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摘要

生物炭作为一种潜在的CO2吸附剂,对解决全球变暖问题具有重要意义。已有研究表明,通过氮和硫掺杂可以提高生物炭的CO2吸附性能。共掺杂可以将两种元素的结构和功能结合起来。然而,在共掺杂生物炭中,氮和硫在掺杂过程中的物理化学相互作用以及CO2吸附过程尚不清楚。本研究采用水热炭化法制备了不同添加剂(尿素、硫代硫酸钠和硫脲)的杂原子掺杂生物炭,并对共掺杂生物炭中氮和硫的物理化学相互作用进行了广泛的研究。结果表明,在共掺杂过程中,氮和硫在碳骨架上竞争有限的掺杂活性位点。有趣的是,硫脲在很大程度上保留了生物炭表面的氨基,这是由于碳硫双键的断裂和成键,促进了活化过程中孔隙的形成。氮和硫掺杂对生物炭的CO2吸附性能分别提高了11.9%和8.5%,但共掺杂对生物炭的改善效果不显著。共掺杂生物炭中的含氮官能团和含硫官能团在CO2吸附过程中表现出相互抑制作用。本研究结果将对氮/硫共掺杂生物炭在CO2吸附中的应用具有重要意义。图形抽象
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Heteroatom-doped biochar devised from cellulose for CO2 adsorption: a new vision on competitive behavior and interactions of N and S

Biochar, as a potential CO2 adsorbent, is of great significance in addressing the problem of global warming. Previous studies have demonstrated that the CO2 adsorption performance of biochar can be improved by nitrogen and sulfur doping. Co-doping can integrate the structure and function of two elements. However, the physicochemical interaction of nitrogen and sulfur during doping and the CO2 adsorption process remains unclear in co-doped biochar. In this study, the heteroatom-doped biochar was prepared with different additives (urea, sodium thiosulfate, and thiourea) via hydrothermal carbonization, and the physicochemical interaction of nitrogen and sulfur in co-doped biochar was investigated extensively. The findings revealed that nitrogen and sulfur competed for limited doped active sites on the carbon skeleton during the co-doping process. Interestingly, thiourea retained the amino group on the surface of biochar to a great extent due to carbon–sulfur double bond breaking and bonding, which facilitated the formation of pore in the activation process. Significantly, co-doping had no significant improvement effect although nitrogen and sulfur doping separately enhanced the CO2 adsorption performance of biochar by 11.9% and 8.5%. The nitrogen-containing and sulfur-containing functional groups in co-doped biochar exhibited mutual inhibition in the process of CO2 adsorption. The findings of this study will have pertinent implications in the application of N/S co-doped biochar for CO2 adsorption.

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来源期刊
Biochar
Biochar Multiple-
CiteScore
18.60
自引率
10.20%
发文量
61
期刊介绍: Biochar stands as a distinguished academic journal delving into multidisciplinary subjects such as agronomy, environmental science, and materials science. Its pages showcase innovative articles spanning the preparation and processing of biochar, exploring its diverse applications, including but not limited to bioenergy production, biochar-based materials for environmental use, soil enhancement, climate change mitigation, contaminated-environment remediation, water purification, new analytical techniques, life cycle assessment, and crucially, rural and regional development. Biochar publishes various article types, including reviews, original research, rapid reports, commentaries, and perspectives, with the overarching goal of reporting significant research achievements, critical reviews fostering a deeper mechanistic understanding of the science, and facilitating academic exchange to drive scientific and technological development.
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