基于生物质基碳纳米片的水污染物氧化脱除

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摘要通过在熔融盐辅助热解法中加入含氧酸盐(K₂CO₃或KNO₃),并以葡萄糖为碳源成功合成了高石墨化和多缺陷位点的多孔二维碳纳米片M-C和M-N.含氧酸盐显著提高了纳米片的比表面积,特别是KNO₃还促进氮掺杂,使M-N对酸性橙7(AO7)的最大吸附容量达到480.77mg/g,远高于直接热解生物炭BC和无含氧酸盐的熔融盐热解炭M-BC.碳材料对AO7去除的吸附和催化降解过程具有协同效应,M-N活化过一硫酸盐(PMS)的活性分别为M-BC的22.64倍和BC的33.48倍.此外,通过密度泛函理论(DFT)初步计算了氮掺杂和不同缺陷对非自由基主导的催化过程的影响.本研究发现含氧酸盐可以明显降低碳纳米片制备过程中熔融盐添加量,也为开发有机污染物高效吸附和PMS高效活化的生物质基双功能碳材料提供了理论指导.

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	郝熔江
	顾翔宇
	李松庚

关键词 ：碳纳米片, 热解, 吸附, 催化剂, 高级氧化

Abstract：The porous two-dimensional carbon nanosheets with high graphitization and defect sites, designated M-C and M-N, were successfully synthesized via molten salt-assisted pyrolysis of glucose, with oxysalts (K₂CO₃ or KNO₃) as additives, respectively. The oxysalts significantly enhanced the specific surface area of the carbon nanosheets. Particularly, KNO₃ promoted nitrogen doping in M-N, resulting in a maximum adsorption capacity for acid orange 7 (AO7) of 480.77mg/g, surpassing that of biochar (BC) from direct pyrolysis and M-BC from molten salt-assisted pyrolysis without oxysalts. The adsorption and catalytic degradation of AO7 removal over carbon materials exhibited a synergistic effect. The catalytic activity of M-N in peroxymonosulfate (PMS) activation was 22.64times that of M-BC and 33.48times that of BC. Additionally, the impact of nitrogen doping and other structural defects on the non-radical pathway-dominated catalytic processes was preliminarily assessed using density functional theory (DFT) calculations. This study indicates that oxysalts can significantly reduce the amount of molten salt required in the preparation of carbon nanosheets, and also provides theoretical guidance for developing bifunctional biomass-based carbon materials for highly efficient organic pollutants adsorption and PMS activation.

Key words： carbon nanosheet pyrolysis adsorption catalyst advanced oxidation

收稿日期: 2024-06-13

PACS:

X703.5

基金资助:国家重点研发项目(2018YFC1901300)

通讯作者: 李松庚,研究员,sgli@ipe.ac.cn E-mail: sgli@ipe.ac.cn

作者简介: 郝熔江(1996-),男,山西忻州人,中国科学院大学博士研究生,主要从事碳纳米材料催化高级氧化研究.发表论文4篇.haorongjiang@qq.com.

引用本文:

郝熔江, 顾翔宇, 李松庚. 基于生物质基碳纳米片的水污染物氧化脱除[J]. 中国环境科学, 2025, 45(1): 144-157. HAO Rong-jiang, GU Xiang-yu, LI Song-geng. Oxidative removal of water pollutants based on biomass-derived carbon nanosheets. CHINA ENVIRONMENTAL SCIENCECE, 2025, 45(1): 144-157.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2025/V45/I1/144

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