Synthesis of N-doped porous carbon derived from biomass waste for activating peroxymonosulfate in water decontamination: Mechanism insight and biotoxicity assessment

IF 5.8 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Environmental Science: Nano Pub Date : 2024-07-10 DOI:10.1039/d4en00481g
Shun Ding, FANGYU FU, Huibin Niu, Jiaying Yan, Yanfen Fang, Xiang Liu
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Abstract

N-doping is a widely used strategy for the synthesis of highly efficient carbon nanocatalysts, however, an in-depth understanding of the effect of nitrogen source on the intrinsic structure and catalytic performance is highly desired. Therefore, to kill two birds with one stone, a series of N-doped carbon nanomaterials were synthesized from the pyrolysis of biomass waste (dealkali lignin) and various nitrogen sources (including melamine, dicyandiamide, and urea). Even though N-doping nanocatalysts showed better catalytic activity than the HCNs (pyrolysis form only dealkali lignin) for sulfamethoxazole (SMX) degradation via peroxymonosulfate (PMS) activation, NCN-1 and NCN-2 presented contractive and small spherical structures when melamine and dicyandiamide with high nitrogen content were added, showing relatively low catalytic efficiency. NPCN derived from dealkali lignin and urea led to the formation of a porous cluster structure with abundant active species of graphitic C/N and C-OH, which showed the best catalytic performance for SMX degradation. Significantly, NPCN exhibited excellent universality, adaptability, and reusability. Moreover, the possible mechanism was proposed based on the quenching study, EPR analysis, electronic quenching experiment, DFT calculation, and HR-MS, confirming that e−, 1O2, •OH, SO4•−, and O2•− were the active species, of which 1O2 was the dominating one in NPCN/PMS system. In addition, the biotoxicity of SMX was evaluated by the ECOSAR analysis and germination tests of wheat seeds. This work provides how the nitrogen source would affect the microstructure-dependent catalytic activity of metal-free carbon nanocatalysts for water decontamination.
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从生物质废弃物中合成掺杂 N 的多孔碳,用于活化水污染中的过硫酸盐:机理研究与生物毒性评估
氮掺杂是合成高效碳纳米催化剂的一种广泛应用的策略,然而,深入了解氮源对其内在结构和催化性能的影响是非常必要的。因此,为了一石二鸟,研究人员利用生物质废料(脱碱木质素)热解和各种氮源(包括三聚氰胺、双氰胺和尿素)合成了一系列氮掺杂碳纳米材料。在通过过一硫酸盐(PMS)活化降解磺胺甲噁唑(SMX)方面,尽管掺杂氮的纳米催化剂比 HCN(热解形式仅为脱碱木质素)显示出更好的催化活性,但当添加含氮量较高的三聚氰胺和双氰胺时,NCN-1 和 NCN-2 出现收缩和小球形结构,显示出相对较低的催化效率。从脱碱木质素和尿素中提取的 NPCN 可形成多孔团簇结构,其中含有丰富的石墨 C/N 和 C-OH 活性物种,对 SMX 降解具有最佳催化性能。值得注意的是,NPCN 具有优异的通用性、适应性和可重复使用性。此外,根据淬灭研究、EPR分析、电子淬灭实验、DFT计算和HR-MS,提出了可能的机理,证实了e-、1O2、-OH、SO4-和O2-是活性物种,其中1O2在NPCN/PMS体系中占主导地位。此外,还通过 ECOSAR 分析和小麦种子发芽试验评估了 SMX 的生物毒性。这项研究提供了氮源如何影响用于水净化的无金属碳纳米催化剂的微结构催化活性。
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来源期刊
Environmental Science: Nano
Environmental Science: Nano CHEMISTRY, MULTIDISCIPLINARY-ENVIRONMENTAL SCIENCES
CiteScore
12.20
自引率
5.50%
发文量
290
审稿时长
2.1 months
期刊介绍: Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas: Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability Nanomaterial interactions with biological systems and nanotoxicology Environmental fate, reactivity, and transformations of nanoscale materials Nanoscale processes in the environment Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis
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