废铁渣基铁碳填料活化过一硫酸盐降解染料模拟废水

张友真; 吴家宜; 曾小星; 王海洋; 周颖; 万昊俊; 冯斐

doi:10.13205/j.hjgc.202609006

废铁渣基铁碳填料活化过一硫酸盐降解染料模拟废水

doi: 10.13205/j.hjgc.202609006

南昌大学资源与环境学院, 南昌 330031

详细信息

作者简介:
张友真(2000—),男,研究生,主要研究方向为废水处理及资源化。youzhen.zhang@foxmail.com

通讯作者:
冯斐(1978—),男,副教授,主要研究方向为废水处理及资源化。fongfei003@163.com

计量
- 文章访问数: 7
- HTML全文浏览量: 2
- PDF下载量: 0
- 被引次数: 0
出版历程
- 收稿日期: 2025-12-15
- 网络出版日期: 2026-11-05

Activation of peroxymonosulfate by iron-slag-derived iron-carbon filler for degradation of simulated dye wastewater

School of Resources and Environment, Nanchang University, Nanchang 330031, China

摘要

摘要: 为实现工业含铁废渣的高值化利用并发展高效稳定的印染废水处理技术，以制药行业含铁废渣为主要铁源，与活性炭复合制备废铁渣基铁碳填料（ICF），构建了一种低成本的过一硫酸盐（PMS）非均相活化体系。系统考察了铁碳质量比、PMS投加量、初始pH和曝气量对染料降解性能的影响。在最优条件［m（Fe）∶m（C）=1∶1，ρ（PMS）=3 g/L，pH=3，曝气量为0.5 L/min］下，ICF/PMS 体系可在30 min内几乎完全降解 100 mg/L 的橙Ⅱ，并对多种结构不同的染料表现出良好的普适性。机理研究表明：该体系不同于传统自由基主导的铁基 PMS 体系，而是以铁–碳界面形成的Fe—C—PMS* 表面络合物及其转化生成的高价铁Fe（Ⅳ）＝O为核心的非自由基氧化途径为主，¹O₂与·O₂^-起协同作用。结果表明，该方法在实现工业废渣资源化利用的同时，为发展高效、稳定且经济可行的印染废水处理技术提供了新技术路径。
- 过一硫酸盐 /
- 非自由基 /
- 废渣资源利用 /
- 高级氧化技术
Abstract: To realize the high-value utilization of iron-containing industrial wastes and to develop an efficient and stable technology for dye wastewater treatment， iron-containing solid waste from the pharmaceutical industry was used as the primary iron source and composited with activated carbon to prepare a waste iron-slag-derived iron-carbon filler （ICF）. Based on this material， a low-cost heterogeneous peroxymonosulfate （PMS） activation system was constructed. The effects of the Fe/C mass ratio， PMS dosage， initial pH， and aeration rate on dye degradation performance were systematically investigated. Under the optimal conditions ［m（Fe）∶m（C）=1∶1， PMS=3 g/L， pH=3， and aeration rate of 0.5 L/min］， the ICF/PMS system could almost completely degrade 100 mg/L of Orange Ⅱ within 30 min and exhibited good universality toward various dyes with different molecular structures. Mechanistic investigations revealed that， unlike conventional iron-based PMS systems dominated by free-radical pathways， this system primarily follows a non-radical oxidation mechanism centered on Fe-C interfacial Fe—C—PMS* surface complexes and their transformation into high-valent iron species， Fe（Ⅳ）＝O， with singlet oxygen （¹O₂） and superoxide radicals （·O₂^-） playing synergistic roles. These findings demonstrate that this strategy not only enables the resource utilization of industrial solid wastes， but also provides a promising new technical route for efficient， stable， and economically feasible dye wastewater treatment.
- peroxymonosulfate （PMS） /
- non-radical /
- resource utilization of waste slag /
- advanced oxidation processes

HTML全文

参考文献(39)

[1]	KHAN S，NOOR T，IQBAL N，et al. Photocatalytic dye degradation from textile wastewater:a review［J］. ACS Omega，2024，9（20）:21751-21767.
[2]	BERRADI M，HSISSOU R，KHUDHAIR M，et al. Textile finishing dyes and their impact on aquatic environs［J］. Heliyon，2019，5（11）:e02711.
[3]	WANG J L，WANG S Z. Activation of persulfate（PS）and peroxymonosulfate（PMS）and application for the degradation of emerging contaminants［J］. Chemical Engineering Journal，2018，334:1502-1517.
[4]	LI Y H，LI M X，ZHU C Q，et al. Main factors for photocatalytic degradation of rhodamine B by MoS₂ activated PMS［J］. Materials Letters，2023，341:134191.
[5]	ZHENG X，NIU X，ZHANG D，et al. Metal-based catalysts for persulfate and peroxymonosulfate activation in heterogeneous ways:a review［J］. Chemical Engineering Journal，2022，429:132323.
[6]	LI S H，NING X E，HAO P Y，et al. Defect-rich MoS₂ piezocatalyst:efficient boosting piezocatalytic activation of PMS activity towards degradation of organic pollutant［J］. Dyes and Pigments，2022，206:110678.
[7]	SU R，LI Z，CHENG F，et al. Advances in the degradation of emerging contaminants by persulfate oxidation technology［J］. Water，Air，& Soil Pollution，2023，234（12）:754.
[8]	CAO Y X，YUAN X Z，ZHAO Y L，et al. In-situ soil remediation via heterogeneous iron-based catalysts activated persulfate process:a review［J］. Chemical Engineering Journal，2022，431:133833.
[9]	HUANG L，ZHU W，WU Y. Advancements in transition metal iron-based catalysts:enhancing catalytic activity through electron transfer［J］. Catalysis Science& Technology，2025，15（13）:3784-3792.
[10]	CUI B，TIAN T，DUAN L，et al. Towards advanced removal of organics in persulfate solution by heterogeneous iron-based catalyst:a review［J］. Journal of Environmental Sciences，2024，146:163-175.
[11]	XIA X Y，WANG L，CHENG F，et al. Research progress of heterogeneous Fenton technology based on carbon/iron-based catalysts and physical field-assisted systems［J］. Environmental Chemistry，2026，45（5）:1941-1951. 夏惜缘，王兰，程飞，等. 基于碳/ 铁基催化剂的非均相芬顿技术及物理场辅助体系的研究进展［J］. 环境化学，2026，45（5）:1941-1951.
[12]	QIAO Q C，SHI J，ZHAO Q，et al. Electro-catalytic oxidation of acid orange Ⅱ by modified γ-Al₂O₃ particle electrodes loaded with metallic oxides［J］. Environmental Engineering，2017，35（7）:86-90. 乔启成，石健，赵勤，等. 金属氧化物负载γ-Al₂O₃粒子电极对酸性橙Ⅱ 的电催化氧化研究［J］. 环境工程，2017，35（7）:86-90.
[13]	MEI Y，ZENG J，SUN M，et al. A novel Fenton-like system of Fe₂O₃ and NaHSO₃ for Orange Ⅱ degradation［J］. Separation and Purification Technology，2020，230:115866.
[14]	GAO Y，ZHOU Y，PANG S Y，et al. New insights into the combination of permanganate and bisulfite as a novel advanced oxidation process:importance of high valent manganese-oxo species and sulfate radical［J］. Environmental Science & Technology，2019，53（7）:3689-3696.
[15]	HUANG Q L，HUANG K，LU Y H，et al. Recovery of iron and aluminum from red mud by oxalic acid leaching and solar photocatalysis［J］. Environmental Engineering，2021，39（12）:199-205. 黄荃莅，黄魁，卢远桓，等. 草酸浸出和太阳光催化回收赤泥中的铁和铝［J］. 环境工程，2021，39（12）:199-205.
[16]	LIANG X F，LIU D F. Biochar supported nanoscale zero-valent iron as an efficient peroxymonosulfate activator to accelerate methylene blue degradation in high-sulfate wastewater［J］. Technology of Water Treatment，2022，48（5）:53-58. 梁啸夫，刘东方. nZVI@BC活化PMS氧化高硫酸盐废水中亚甲基蓝的研究［J］. 水处理技术，2022，48（5）:53-58.
[17]	LONG J，MAO Y，LONG Y，et al. Ru nanoparticles on HZSM-5 with strong metal-support interactions for efficient hydrodeoxygenation of lignin-derived phenols under mild conditions［J］. Bioresource Technology，2026，439:133357.
[18]	HU B，ZHOU M，ZHANG K，et al. The advanced treatment of mature landfill leachate by iron-carbon micro-electrolysis combined with persulfate activated（ICME-PS）process［J］. Journal of Environmental Chemical Engineering，2024，12（5）:113786.
[19]	LI Y，YANG Y J，GONG Z，et al. Electrically driven single-atom Mo enhances support effect for efficient PMS activation to degrade high-concentration sulfanilamide［J］. Chemical Engineering Journal，2025，521:166845.
[20]	SUN Z Z，LIU Z H，HAN L，et al. Study on the treatment of simulated azo dye wastewater by a novel micro-electrolysis filler［J］. Water Science and Technology，2019，79（12）:2279-2288.
[21]	LIU M X，WU H B，XIE Y Q，et al. Unraveling the role of oxygen in aeration-driven piezoelectric PMS activation process using oxygen vacancy engineered BTO［J］. Separation and Purification Technology，2025，376:133950.
[22]	CHEN S，HUANG J，FANG H L，et al. Chitosan hydrogel catalyst shifts PMS activation towards a singlet oxygen-dominated non-radical pathway for efficient pollutant degradation［J］. Chemical Engineering Journal，2025，525:170553.
[23]	ZHANG Q K，LI G Q，MA Z F，et al. Visible light-induced activation of persulfates in MgFe-LDH and toluidine blue system［J］. Journal of Water Process Engineering，2024，59:105014.
[24]	LI W，NIE C，WANG X，et al. Alkaline lignin-derived N-doped biochars as peroxymonosulfate activators for acetaminophen degradation:performance and catalytic bridging mediated electron-transfer mechanism［J］. Separation and Purification Technology，2023，323:124418.
[25]	LI H，QIU R L，TANG Y T，et al. Formation of Fe（Ⅳ）over a wide pH range via iron-carbon composite-catalyzed persulfate activation［J］. Chemical Engineering Journal，2023，461:141951.
[26]	LIANG J，DUAN X，XU X，et al. Persulfate oxidation of sulfamethoxazole by magnetic iron-char composites via nonradical pathways:Fe（Ⅳ）versus surface-mediated electron transfer［J］. Environmental Science& Technology，2021，55（14）:10077-10086.
[27]	CHENG C，REN W，MIAO F，et al. Generation of Fe（Ⅳ）＝ O and its contribution to Fenton-like reactions on a single-atom iron-N-C catalyst［J］. Angewandte Chemie International Edition，2023，62（10）:e202218510.
[28]	ZHANG Y，CUI M，CUI J，et al. Identification of reactive species and functional groups determining the selective oxidation of organic contaminants in bismuth ferrate/peroxymonosulfate system［J］. Applied Catalysis B:Environment and Energy，2025，376:125447.
[29]	YANG M，HOU Z，ZHANG X，et al. Unveiling the origins of selective oxidation in single-atom catalysis via Co-N₄-C intensified radical and nonradical pathways［J］. Environmental Science& Technology，2022，56（16）:11635-11645.
[30]	KUANG Z，LIU S，LI X，et al. Topotactically constructed nickel-iron（oxy）hydroxide with abundant in-situ produced high-valent iron species for efficient water oxidation［J］. Journal of Energy Chemistry，2021，57:212-218.
[31]	LIN T，ZHOU H，ZHAO L，et al. Direct generation of high-valent iron-oxo species to eliminate oxytetracycline at circumneutral pH via paper mill sludge ash activating peroxymonosulfate［J］. Chemical Engineering Journal，2024，484:150021.
[32]	LI C，KANG L，WANG S，et al. Enhanced PFOA degradation via non-radical PMS pathway through synergistic Fe single-atoms and Fe nanoparticles in Fe-N-C catalysts［J］. Chemical Engineering Journal，2025，512:162424.
[33]	KANG H，LEE D，LEE K M，et al. Nonradical activation of peroxymonosulfate by hematite for oxidation of organic compounds:a novel mechanism involving high-valent iron species［J］. Chemical Engineering Journal，2021，426:130743.
[34]	FENG Y，LI Y，YANG B，et al. Mechanistic insight into the generation of high-valent iron-oxo species via peroxymonosulfate activation:an experimental and density functional theory study［J］. Chemical Engineering Journal，2021，420:130477.
[35]	LI B，WANG Z，SUN L，et al. Breaking through the oxygen hindrance effect in Fenton-like reactions to promote the generation of high-valent iron-oxo species within Fe-N_xB/GCN single-atom catalysts［J］. Applied Catalysis B:Environment and Energy，2025，372:125280.
[36]	YANG T，FAN S，LI Y，et al. Fe-N/C single-atom catalysts with high density of Fe-N_x sites toward peroxymonosulfate activation for high-efficient oxidation of bisphenol A:electron-transfer mechanism［J］. Chemical Engineering Journal，2021，419:129590.
[37]	ZOU Y，FU S，XU Z，et al. Unveiling the long-range interaction of sulfur in the second shell of Fe-N₄ single-atom sites for highly selective generation of high-valent iron-oxo species in peroxymonosulfate activation［J］. Chemical Engineering Journal，2025，505:159684.
[38]	WEI T，ZHU X S，WANG Q X，et al. Prussian blue analogues-derived zero valent iron to efficiently activate peroxymonosulfate for phenol degradation triggered via reactive oxygen species and high-valent iron-oxo complexes［J］. Environmental Research，2023，237:116962.
[39]	Government Singapore. Environmental pollution control（trade effluent）regulations 1999［R］. 1999.