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Multipath elimination of bisphenol A over bifunctional polymeric carbon nitride/biochar hybrids in the presence of persulfate and visible light
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-05-05 , DOI: 10.1016/j.jhazmat.2021.126008
Huazhe Wang 1 , Wanqian Guo 1 , Qishi Si 1 , Banghai Liu 1 , Qi Zhao 1 , Haichao Luo 1 , Nanqi Ren 1
Affiliation  

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 HCO3. 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.



中文翻译:

在过硫酸盐和可见光存在下,双功能聚合双氮化碳/生物炭杂化物对双酚A的多径消除

聚合氮化碳(PCN)在光催化或过硫酸盐(PS)活化中已成为明星材料。在这项工作中,我们通过简便的一锅式热处理工艺合成了掺有双功能生物炭(BC)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能。由外部玉米芯碳化产生的非晶BC域为PCN的原位生长提供了附件,并提高了其催化能力,包括电子传输性能,可见光(VIS)利用率和氧化能力。机理研究表明,在没有VIS的CNBC / PS系统中,非自由基电子转移途径是导致双酚A(BPA)降解的原因,而在CNBC / PS / VIS系统中,揭示了自由基/非自由基混合机制,包括介导的电子转移,自由基氧化和空穴氧化。推导了BPA的降解途径,包括芳环上的直接氧化,异丙基的β-断裂和环的裂解。根据ECOSAR软件评估,大多数中间体的毒性均低于BPA。CNBC / PS / VIS系统显示出令人满意的抗环境干扰能力,除了HCO3。这项工作为合成基于PCN的双功能催化剂提供了一个简单而有效的策略,并加深了对混合高级氧化技术的机械洞察力。

更新日期:2021-05-09
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