Insights into the Crucial Role of Electron and Spin Structures in Heteroatom-Doped Covalent Triazine Frameworks for Removing Organic Micropollutants

Zhu Chao; Fang Qile; Liu RenlanDong WenSong ShuangShen Yi

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Insights into the Crucial Role of Electron and Spin Structures in Heteroatom-Doped Covalent Triazine Frameworks for Removing Organic Micropollutants

机译：Insights into the Crucial Role of Electron and Spin Structures in Heteroatom-Doped Covalent Triazine Frameworks for Removing Organic Micropollutants

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摘要

The water shortage crisis, characterized by organic micropollutants (OMPs), urgently requires new materials and methods to deal with it. Although heteroatom doping has been developed into an effective method to modify carbon nanomaterials for various heterogeneous adsorption and catalytic oxidation systems, the active source regulated by intrinsic electron and spin structures is still obscure. Here, a series of nonmetallic element-doped (such as P, S, and Se) covalent triazine frameworks (CTFs) were constructed and applied to remove organic pollutants using the adsorption-photocatalysis process. The external mass transfer model (EMTM) and the homogeneous surface diffusion model (HSDM) were employed to describe the adsorption process. It was found that sulfur-doped CTF (S-CTF-1) showed a 25.6-fold increase in saturated adsorption capacity (554.7 mu mol/g) and a 169.0-fold surge in photocatalytic kinetics (5.07 h(-1)), respectively, compared with the pristine CTF-1. A positive correlation between electron accumulation at the active site (N1 atom) and adsorption energy was further demonstrated with experimental results and theoretical calculations. Meanwhile, the photocatalytic degradation rates were greatly enhanced by forming a built-in electric field driven by spin polarization. In addition, S-CTF-1 still maintained a 98.3% removal of 2,2 ',4,4 '-tetrahydroxybenzophenone (BP-2) micropollutants and 97.6% regeneration after six-cycle sequencing batch treatment in real water matrices. This work established a relation between electron and spin structures for adsorption and photocatalysis, paving a new way to design modified carbon nanomaterials to control OMPs.

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《Environmental Science & Technology: ES&T》 |2022年第10期|6699-6709|共11页
作者
Zhu Chao; Fang Qile; Liu RenlanDong WenSong ShuangShen Yi;
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作者单位

Zhejiang Univ Technol;

Beijing Normal Univ Zhuhais;

Wenzhou Univ;

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收录信息美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
原文格式 PDF
正文语种英语
中图分类环境科学、安全科学;
关键词
adsorption; photocatalysis; electron accumulation; spin polarization; micropollutants removal; METAL; EFFICIENT; HYDROGEN; DEGRADATION; ADSORPTION; ADSORBENT; OXIDE;

Insights into the Crucial Role of Electron and Spin Structures in Heteroatom-Doped Covalent Triazine Frameworks for Removing Organic Micropollutants

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