揭示废木质素掺氮多孔碳去除六价铬的促进机制。

IF 8.2 1区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Science of the Total Environment Pub Date : 2024-12-15 Epub Date: 2024-11-09 DOI:10.1016/j.scitotenv.2024.177426
Huirong Zhang, Yi Shen, Xiaokai Shi, Jinlei Cui, Baofeng Wang, Yanxia Guo, Dongke Zhang, Fangqin Cheng
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引用次数: 0

摘要

重金属,尤其是六(Cr)的高毒性和生物蓄积性对生态系统和人类健康造成了严重威胁。利用可持续材料开发高性能、高性价比的吸附剂仍是铬 (VI) 修复领域面临的一项严峻挑战。本研究探讨了掺氮分层多孔碳(N-HPC)中吡咯烷酮-N(N-5)对其吸附能力的影响。结果表明,N-5 含量较高的 N-HPC 变体表现出卓越的吸附能力。最佳样品对六价铬的吸附能力高达 386.2 mg/g。即使经过七个再生周期,这种 N-HPC 变体对六价铬的去除率仍高达 77.8%,显示了其强大的稳定性和选择性。对 N-5 和 N-HPC 的物理化学特性之间的关系进行了深入研究,发现 N-5 在吸附过程中起着至关重要的作用。由于氮具有高电负性,在碳框架中掺入氮会产生偶极矩,从而增强 N-HPC 的电负性,改变其局部电子密度和极性,增加比表面积、碳缺陷密度和离子交换能力。这些因素共同促成了 N-HPC 在孔隙填充、离子交换效率和静电吸附方面的显著改善。还原复合机制是吸附过程中的主导因素。N-5 不仅作为电子供体提供还原电子,促进铬 (VI) 不断转化为铬 (III),还作为吸附活性位点将铬络合到 N-HPC 表面。这种协同效应加强了还原络合,提高了吸附性能,改善了再生周期和对铬的吸附选择性。
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Unraveling the promotive mechanism of nitrogen-doped porous carbon from wasted lignin for Cr (VI) removal.

Persistent environmental pollution by heavy metals, particularly Cr (VI), poses significant risks to ecosystems and human health due to its high toxicity and bioaccumulation potential. The development of high-performance, cost-effective adsorbents from sustainable materials remains a critical challenge in the field of Cr (VI) remediation. This study investigates the influence of pyrrolic-N (N-5) within nitrogen-doped hierarchical porous carbon (N-HPC) on its adsorption capacity. Results indicate that N-HPC variants with a higher N-5 content exhibit superior adsorption abilities. The optimal sample demonstrated an exceptional adsorption capacity of 386.2 mg/g for Cr (VI). Even after seven regeneration cycles, this N-HPC variant maintained a remarkable 77.8 % removal efficiency for Cr (VI), highlighting its robust stability and selectivity. The relationship between the physicochemical properties of N-5 and N-HPC was thoroughly examined, revealing that N-5 plays a crucial role in the adsorption process. Due to its high electronegativity, nitrogen-doping into the carbon framework generates a dipole moment, enhancing the electronegativity of N-HPC, altering its local electron density and polarity, increasing specific surface area, carbon defect density, and ion exchange capacity. These factors collectively contribute to significant improvements in pore filling, ion exchange efficiency, and electrostatic adsorption by N-HPC. The reduction complexation mechanism emerges as the dominant factor in the adsorption process. N-5 not only provides reducing electrons as an electron donor, facilitating the continuous conversion of Cr (VI) to Cr (III), but also acts as an adsorption active site, complexing Cr to the surface of N-HPC. This synergistic effect strengthens the reduction complexation, enhances adsorption performance, and improves the regeneration cycle and adsorption selectivity for Cr.

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来源期刊
Science of the Total Environment
Science of the Total Environment 环境科学-环境科学
CiteScore
17.60
自引率
10.20%
发文量
8726
审稿时长
2.4 months
期刊介绍: The Science of the Total Environment is an international journal dedicated to scientific research on the environment and its interaction with humanity. It covers a wide range of disciplines and seeks to publish innovative, hypothesis-driven, and impactful research that explores the entire environment, including the atmosphere, lithosphere, hydrosphere, biosphere, and anthroposphere. The journal's updated Aims & Scope emphasizes the importance of interdisciplinary environmental research with broad impact. Priority is given to studies that advance fundamental understanding and explore the interconnectedness of multiple environmental spheres. Field studies are preferred, while laboratory experiments must demonstrate significant methodological advancements or mechanistic insights with direct relevance to the environment.
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