PCDD/F adsorption enhancement over nitrogen-doped biochar: A DFT-D study

Shijian Xiong; Minghui Tang; Wenqian Jiang; Jiamin Ding; Juan Qiu; Shengyong Lu; Jianhua Yan

doi:10.1016/j.jenvman.2023.118611

PCDD/F adsorption enhancement over nitrogen-doped biochar: A DFT-D study

J Environ Manage. 2023 Oct 15:344:118611. doi: 10.1016/j.jenvman.2023.118611. Epub 2023 Jul 13.

Authors

Shijian Xiong¹, Minghui Tang², Wenqian Jiang¹, Jiamin Ding³, Juan Qiu³, Shengyong Lu⁴, Jianhua Yan¹

Affiliations

¹ State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027, PR China.
² State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027, PR China. Electronic address: lytmh1214@zju.edu.cn.
³ Research Institute of Zhejiang University-Taizhou, Taizhou, 318012, Zhejiang, China.
⁴ State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027, PR China; Research Institute of Zhejiang University-Taizhou, Taizhou, 318012, Zhejiang, China.

PMID: 37453301
DOI: 10.1016/j.jenvman.2023.118611

Abstract

Polychlorinated dibenzo-p-dioxin/furans (PCDD/F) have a great threat to the environment and human health, resulting in controlling PCDD/F emissions to regulation far important for emission source. Considering 2,3,4,7,8-pentachlorodibenzo-p-furan (PeCDF) identified as the most contributor to international toxic equivalent, 2,3,4,7,8-PeCDF can be considered as the target molecule for the adsorption of PCDD/F emission from industries. With the aim to in-depth elucidate how different types of nitrogen (N) species enhance 2,3,4,7,8-PeCDF on the biochar and guide the specific carbon materials design for industries, systematic computational investigations by density functional theory calculations were conducted. The results indicate pristine biochar intrinsically interacts with 2,3,4,7,8-PeCDF by π-π electron donor and acceptor (EDA) interaction, six-membered carbon rings of PeCDF parallel to the biochar surface as the strongest adsorption configuration. Moreover, by comparison of adsorption energy (-150.16 kJ mol^-1) and interaction distance (3.593 Å) of pristine biochar, environment friendly N doping can enhance the adsorption of 2,3,4,7,8-PeCDF on biochar. Compared with graphitic N doping and pyridinic N doping, pyrrolic N doping biochar presents the strongest interaction toward 2,3,4,7,8-PeCDF molecule due to the highest adsorption energy (-155.56 kJ mol^-1) and shortest interaction distance (3.532 Å). Specially, the enhancing adsorption of PeCDF over N doped biochar attributes to the enhancing π-π electron EDA interaction and electrostatic interaction. In addition, the effect of N doping species on PeCDF adsorbed on the biochar is more than that of N doping content. Specially, the adsorption capacity of N doping biochar for PCDD/F can be improved by adding pyrrolic N group most efficiently. Furthermore, pyrrolic N and pyridinic N doping result in the entropy increase, and electrons transform from pyrrolic N and pyridinic N doped biochar to 2,3,4,7,8-PeCDF molecule. A complete understanding of the research would supply crucial information for applying N-doped biochar to effectively remove PCDD/F for industries.

Keywords: 2,3,4,7,8-Pentachlorodibenzo-p-furan; Adsorption; Biochar; Density functional theory; N-doping.

MeSH terms

Adsorption
Carbon
Humans
Nitrogen*
Polychlorinated Dibenzodioxins*

Substances

biochar
Nitrogen
Carbon
Polychlorinated Dibenzodioxins