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过硫酸盐和可见光存在下双功能聚合碳氮化物/生物炭杂化体中双酚 A 的多路径消除。

Multipath elimination of bisphenol A over bifunctional polymeric carbon nitride/biochar hybrids in the presence of persulfate and visible light.

机构信息

State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, China.

State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, China.

出版信息

J Hazard Mater. 2021 Sep 5;417:126008. doi: 10.1016/j.jhazmat.2021.126008. Epub 2021 May 5.

Abstract

Polymeric carbon nitride (PCN) has become a star material either in photocatalysis or in persulfate (PS) activation. In this work, we synthesized bifunctional biochar (BC)-doped PCN through a facile one-pot thermal treatment process. The PCN/BC hybrid (CNBC) with an optimized proportion could not only activate PS directly, but also possessed improved optical properties. Amorphous BC domains generated from the carbonization of external corncob provided attachments for the in-situ growth of PCN and upgraded its catalytic ability including electron transport property, visible light (VIS) utilization, and oxidation power. Mechanism studies demonstrated that in the CNBC/PS system without VIS, a nonradical electron transfer route was responsible for the degradation of bisphenol A (BPA), while in the CNBC/PS/VIS system, radical/nonradical mixing mechanisms including mediated electron transfer, radical oxidation, and hole oxidation were unveiled. Degradation pathways of BPA were deduced including direct oxidation at the aromatic ring, β-scission of isopropyl, and ring cleavage. Most of the intermediates were less toxic than BPA as assessed by the ECOSAR software. The CNBC/PS/VIS system showed satisfactory resistance to environmental interferences except for HCO. This work provides a simple but effective strategy for the synthesis of PCN-based bifunctional catalysts and deepens mechanistic insights into hybrid advanced oxidation technologies.

摘要

聚合物氮化碳(PCN)在光催化或过硫酸盐(PS)活化中已经成为一种明星材料。在这项工作中,我们通过简便的一锅热处理工艺合成了双功能生物炭(BC)掺杂的 PCN。具有最佳比例的 PCN/BC 杂化体(CNBC)不仅可以直接激活 PS,而且还具有改善的光学性质。来自外部玉米芯碳化的无定形 BC 域为 PCN 的原位生长提供了附着点,并提高了其催化能力,包括电子传输性能、可见光(VIS)利用和氧化能力。机理研究表明,在没有 VIS 的 CNBC/PS 体系中,非自由基电子转移途径负责双酚 A(BPA)的降解,而在 CNBC/PS/VIS 体系中,揭示了包括介导电子转移、自由基氧化和空穴氧化在内的自由基/非自由基混合机制。通过 ECOSAR 软件评估,推断出 BPA 的降解途径包括芳环的直接氧化、异丙基的β断裂和环裂解。除了 HCO 之外,CNBC/PS/VIS 体系对环境干扰具有令人满意的抵抗力。这项工作为基于 PCN 的双功能催化剂的合成提供了一种简单但有效的策略,并深化了对混合高级氧化技术的机理认识。

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