Periodate activation with polyaniline-derived carbon for bisphenol A degradation: Insight into the roles of nitrogen dopants and non-radical species formation
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引用次数: 0
Abstract
Periodate-based advanced oxidation processes (PI-AOPs) activated by carbon catalysts have shown promising application prospects in the removal of emerging contaminants. Herein, a series of N-doped carbon catalysts (NC) were prepared by in-situ pyrolysis of N-containing polymers (polyaniline) to unveil the potential mechanism of N dopants on PI activation. The optimized sample NC700 showed a satisfying degradation performance, achieving 100 % removal of bisphenol A (BPA) at a concentration of 10 mg/L within 90 min in the presence of 0.1 mM PI. The impacts of various N types on PI activation were systematically investigated by dynamic fitting and density functional theory computations. These analyses highlighted the crucial role of graphitic N configuration on carbon surface, which exhibited the highest adsorption energy and a positive correlation with the normalized degradation efficiency. The chemical quenching experiments and electrochemical experiments confirmed that the BPA oxidation mechanism was primarily mediated electron transfer by [NC-PI]* complex, with singlet oxygen (1O2) /superoxide radicals (O2•–) playing a supplementary role. In situ ATR-SERAS measurement strengthened the understanding of PI activation by carbon catalyst based on electron transfer pathway. Owing to the non-radical oxidation mechanism, the NC/PI system had a broad pH adaptability and great anti-interference ability against typical wastewater components. This study provides mechanistic insights into the carbon-driven PI activation process for wastewater treatment, advancing the practical application of PI-AOPs.
由碳催化剂激活的基于高碘酸盐的高级氧化过程(PI-AOPs)在去除新兴污染物方面具有广阔的应用前景。本文通过原位热解含氮聚合物(聚苯胺)制备了一系列掺杂氮的碳催化剂(NC),以揭示掺杂氮对高碘酸钾活化的潜在机理。优化样品 NC700 的降解性能令人满意,在 0.1 mM PI 存在下,90 分钟内对浓度为 10 mg/L 的双酚 A(BPA)的去除率达到 100%。通过动态拟合和密度泛函理论计算,系统地研究了各种 N 类型对 PI 活化的影响。这些分析凸显了碳表面石墨化 N 构型的关键作用,它表现出最高的吸附能,并与归一化降解效率呈正相关。化学淬灭实验和电化学实验证实,双酚 A 的氧化机理主要是[NC-PI]* 复合物介导的电子转移,单线态氧(1O2)/超氧自由基(O2--)起辅助作用。原位 ATR-SERAS 测量加深了人们对基于电子传递途径的碳催化剂活化 PI 的理解。由于其非自由基氧化机理,NC/PI 系统具有广泛的 pH 适应性,对典型废水成分具有很强的抗干扰能力。该研究从机理上揭示了碳驱动的 PI 活化过程在废水处理中的应用,推动了 PI-AOPs 的实际应用。
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.