Mechanochemical synthesis of biochar encapsulated FeMn nanoparticles with strong metal–carbon interactions for efficient degradation of tetracycline via activating peroxymonosulfate

IF 13.2 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Yue Wang, Zhenglong Liu, Pan Huang, Baoliang Lei, Lele Qiao, Tielong Li, Kun-Yi Andrew Lin, Haitao Wang
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Abstract

Transition metal and carbon nanomaterials are well-known for their peroxymonosulfate (PMS) activation capabilities. However, metal-based materials often suffer from ion leakage and poor reusability, while carbon-based materials have limited catalytic efficiency. To overcome these challenges and leverage the strengths of both, we introduce carbon-coated Fe/Mn composites (FeMn@BC), that establish strong interactions between metal components and the carbon substrate. FeMn@BC exhibited exceptional selectivity for 1O2 generation via PMS activation. In practical applications, FeMn@BC efficiently degraded tetracycline by activating PMS, achieving 99 % removal in just 30 min. Importantly, FeMn@BC demonstrated remarkable stability, especially under visible light exposure. XPS analyses revealed strong interactions between FeMn components and the biochar shell, enhancing the electron transfer capacity of FeMn@BC through Fe(III)/Fe(II) and Mn(III)/Mn(II) redox pairs. In-situ attenuated total reflection Fourier-transform infrared (ATR-FTIR) analysis highlighted abundant hydroxyl groups in FeMn@BC as crucial active sites for electron transfer. Quenching experiments and electron paramagnetic resonance (EPR) measurements unveiled that FeMn@BC catalyzed 1O2 generation primarily through the disproportionation of O2Abstract Image and energy transfer from oxygen vacancy to O2. Our work demonstrates the possibility of simple ball milling of biomass in the presence of iron salts for iron-catalyzed mechanochemical synthesis of biochar-based catalysts. This study not only presents a novel strategy for large-scale biochar-encapsulated transition metal catalyst synthesis but also explores the potential use of agricultural waste for value-added applications.

Abstract Image

机械化学合成具有强金属-碳相互作用的生物炭包封FeMn纳米颗粒,通过活化过氧单硫酸盐高效降解四环素
过渡金属和碳纳米材料以其过氧单硫酸盐(PMS)活化能力而闻名。然而,金属基材料经常存在离子泄漏和可重复使用性差的问题,而碳基材料的催化效率有限。为了克服这些挑战并利用两者的优势,我们引入了碳涂层Fe/Mn复合材料(FeMn@BC),该复合材料在金属成分和碳衬底之间建立了强相互作用。FeMn@BC通过PMS活化对1O2的产生表现出特殊的选择性。在实际应用中,FeMn@BC通过激活PMS有效地降解四环素,在30 分钟内达到99% %的去除率。重要的是,FeMn@BC表现出了非凡的稳定性,特别是在可见光照射下。XPS分析显示,FeMn组分与生物炭壳之间存在较强的相互作用,通过Fe(III)/Fe(II)和Mn(III)/Mn(II)氧化还原对增强FeMn@BC的电子传递能力。原位衰减全反射傅里叶变换红外(ATR-FTIR)分析表明,FeMn@BC中丰富的羟基是电子转移的关键活性位点。猝灭实验和电子顺磁共振(EPR)测量表明,FeMn@BC主要通过O2 -歧化和氧空位向O2的能量转移来催化1O2的生成。我们的工作证明了在铁盐存在下对生物质进行简单球磨的可能性,用于铁催化的生物炭基催化剂的机械化学合成。本研究不仅提出了大规模生物炭包封过渡金属催化剂合成的新策略,而且还探索了农业废弃物增值应用的潜在用途。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
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.
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Ferric chloride hexahydrate
¥15.00~¥57619.42
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Sodium carbonate
¥16.00~¥44404.31
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5,5-Dimethyl-1-pyrroline N-oxide
¥50.00~¥27918.00
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Sodium nitrate
¥45.00~¥26204.90
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Sodium hydroxide
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Manganese chloride
¥19.00~¥13568.00
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Sorbic acid
¥16.00~¥10160.90
上海源叶
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¥24.00~¥7557.00
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Tetracycline
¥29.90~¥7479.00
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2,2,6,6-Tetramethyl-4-piperidinol
¥6.00~¥5759.00
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Sodium dihydrogen phosphate
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Manganese (Mn) standard solution
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Iron (Fe) standard solution
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p -Benzoquinone
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tert -Butanol
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Peroxymonosulfate | >47%
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Sorbic acid
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2,2,6,6-Tetramethyl-4-piperidinol (TEMP)
阿拉丁
5,5-Dimethyl-1-pyrroline N-oxide (DMPO)
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Sodium dihydrogen phosphate (NaH?PO?)
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Sodium bicarbonate (NaHCO?)
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Sodium carbonate (Na?CO?)
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Sodium nitrate (NaNO?)
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Sodium chloride (NaCl)
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Sodium sulfate (Na?SO?)
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p-Benzoquinone (p-BQ)
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tert-butanol
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Methanol
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Ethanol (EtOH)
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Sodium hydroxide (NaOH)
阿拉丁
Peroxymonosulfate
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Tetracycline
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Manganese chloride (MnCl?)
阿拉丁
Ferric chloride hexahydrate (FeCl?·6H?O)
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