Template-assisted synthesis of CaCO3-stabilized cobalt silicate nanoflowers for efficient peroxymonosulfate activation with minimized cobalt leaching.

IF 2.9 4区 材料科学 Q3 MATERIALS SCIENCE, MULTIDISCIPLINARY
Qing Sun, Lu Yang, Yutao Zhou, Jian Zhang, Jiawei Sheng
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引用次数: 0

Abstract

Cobalt-based catalysts demonstrate significant activity in activating peroxymonosulfate (PMS) for the degradation of water pollutants. Nevertheless, their practical application remains constrained due to concerns regarding potential cobalt leaching, associated toxicity risks, and overall stability under operational conditions. A novel CoCa-SBA-600 catalyst was synthesized via a hydrothermal-assisted SBA-15 sacrificial templating strategy, where the zeolite simultaneously served as a silicate precursor and structural scaffold. Comprehensive characterization (XRD, FTIR, SEM, TEM and XPS) confirmed the co-existence of CaCO3-stabilized cobalt silicate nanoflowers with ultrathin two-dimensional layered morphology. The CaCO3 incorporation remarkably enhanced PMS activation efficiency while suppressing Co²⁺ leaching (≤0.51 mg/L), achieving 99.29% metronidazole (MNZ) degradation within 10 min at 500 mg/L catalyst dosage. The system demonstrated exceptional universality, degrading multiple antibiotics (≥96.97% efficiency within 10 min) across diverse aqueous matrices (tap/lake/river water) and maintained >98% MNZ removal after four cycles, highlighting robust stability. Mechanistic studies verified singlet oxygen (¹O₂) as the dominant reactive species via quenching experiments and EPR analysis, with proposed MNZ degradation pathways aligned with LC-MS data. Notably, seed germination assays confirmed the low biotoxicity of degradation intermediates. The calcium carbonate-mediated stabilization strategy proposed in this study achieves efficient stabilization of cobalt silicate materials. The insights gained not only advance the development of environmentally friendly advanced oxidation processes (AOPs) but also provide a new paradigm for designing long-lasting catalysts for environmental remediation applications.

模板辅助合成caco3稳定的硅酸钴纳米花,用于高效过氧单硫酸盐活化和最小化钴浸出。
钴基催化剂在激活过氧单硫酸盐(PMS)降解水污染物方面表现出显著的活性。然而,由于担心潜在的钴浸出、相关的毒性风险和操作条件下的整体稳定性,它们的实际应用仍然受到限制。通过水热辅助SBA-15牺牲模板策略合成了一种新型的CoCa-SBA-600催化剂,其中沸石同时作为硅酸盐前驱体和结构支架。综合表征(XRD, FTIR, SEM, TEM和XPS)证实caco3稳定的硅酸钴纳米花具有超薄的二维层状形貌。CaCO3的掺入显著提高了PMS的活化效率,同时抑制了Co 2⁺的浸出(≤0.51 mg/L),在500 mg/L的催化剂用量下,10 min内甲硝唑(MNZ)的降解率达到99.29%。该系统表现出卓越的通用性,在不同的水基质(自来水/湖水/河水)中降解多种抗生素(10分钟内效率≥96.97%),并在4个循环后保持98%的MNZ去除率,突出了强大的稳定性。机理研究通过淬火实验和EPR分析验证了单线态氧(¹O₂)是主要的反应物质,所提出的MNZ降解途径与LC-MS数据一致。值得注意的是,种子萌发试验证实了降解中间体的低生物毒性。本研究提出的碳酸钙介导的稳定策略实现了硅酸钴材料的高效稳定。这些见解不仅推动了环境友好型高级氧化工艺(AOPs)的发展,而且为设计用于环境修复应用的长效催化剂提供了新的范例。
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来源期刊
Nanotechnology
Nanotechnology 工程技术-材料科学:综合
CiteScore
7.10
自引率
5.70%
发文量
820
审稿时长
2.5 months
期刊介绍: The journal aims to publish papers at the forefront of nanoscale science and technology and especially those of an interdisciplinary nature. Here, nanotechnology is taken to include the ability to individually address, control, and modify structures, materials and devices with nanometre precision, and the synthesis of such structures into systems of micro- and macroscopic dimensions such as MEMS based devices. It encompasses the understanding of the fundamental physics, chemistry, biology and technology of nanometre-scale objects and how such objects can be used in the areas of computation, sensors, nanostructured materials and nano-biotechnology.
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