针对传统净水氧化体系存在的内源性介质传质受限、依赖高能耗或牺牲剂维持催化活性等瓶颈问题,提出利用微量H2O2微调控双反应中心(DRC)催化剂表面增强水自净化的创新策略.研究发现,通过制备表面具有电子极化分布结构的DRC催化剂(FZSO)能有效用于增强水中自然溶解氧与污染物的相互作用,打破二者间传质限制从而强化水体自净.这一过程,使H2O2角色发生根本性的转变—从传统高级氧化过程中的牺牲剂创新性作为微调控剂,极大降低水处理过程能耗.结果表明,在仅1mmol/L H2O2微调控下,FZSO自净增强体系在15min实现对环丙沙星的完全去除,其H2O2的消耗不到10%,且不受水中复杂介质(pH值或盐分离子等)的干扰,具有良好的适应性和稳定性.该策略通过强化水体自净力实现节能增效的突破,为开发应用高效的低能耗净水工艺提供新的思路和技术参考.
Abstract
This study addresses challenges in conventional advanced oxidation processes (AOPs), including mass transfer limitations of endogenous mediators, and reliance on energy-intensive/sacrificial agents’ consumption to maintain the catalytic activity, by proposing an innovative strategy that employs trace H2O2 to micro-regulate dual-reaction center (DRC) catalysts for enhanced water self-purification. DRC catalyst (FZSO) with surface electron-polarized distribution can effectively enhance interactions between naturally dissolved oxygen and pollutants, thereby overcomes mass transfer limitations and obviously enhances water self- purification. This process radically changes the role of H2O2—innovatively repurposed from the sacrificial agent in AOPs to the precision micro-regulator in DRC system, largely reducing consumption in water treatment. Experimental results demonstrate that under micro-regulation with only 1mmol/L H2O2, the FZSO-DRC system achieved complete ciprofloxacin removal within 15min, with less than 10% H2O2 consumption. FZSO system also exhibits strong adaptability and stability for complex water matrices (pH or salinity ions). This study proposes a breakthrough in energy-efficient water purification by amplifying natural water self- purification capacity through the FZSO-DRC system, providing new technical perspective for developing high-efficiency, low- consumption water treatment processes.
关键词
强化水体自净 /
双反应中心 /
微量H2O2 /
活化溶解氧 /
微调控
Key words
water self-purification enhancement /
dual reaction center /
trace H2O2 /
activated dissolved oxygen /
micro-regulation
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参考文献
[1] Marefat A, Asgari S, Badpa R, et al. Geospatial investigation on self-purification capacity of river Estuaries in the Caspian region: reducing heavy metals pollution [J]. npj Clean Water, 2024,7(1):32.
[2] An S Q, Song Y, Fu Q, et al. Reclaimed water use improved polluted water's self-purification capacity--Evidenced by water quality factors and bacterial community structure [J]. Journal of Cleaner Production, 2023,386:135736.
[3] 窦明,贾瑞鹏.基于环境自净能力的龙凤湿地水质改善优化调控模型 [J].环境科学学报, 2018,38(6):2418-2426. Dou M, Jia R P. Optimization of water quality improvement program for Longfeng wetland considering the purification of aquatic plants [J]. Acta Scientiae Circumstantiae, 2018,38(6):2418-2426.
[4] Zhang W L, Fang S Q, Li Y, et al. Optimizing the integration of pollution control and water transfer for contaminated river remediation considering life-cycle concept [J]. Journal of Cleaner Production, 2019,236:117651.
[5] Zhu Z X, Lu W Y, Li N, et al. Pyridyl-containing polymer blends stabilized iron phthalocyanine to degrade sulfonamides by enzyme- like process [J]. Chemical Engineering Journal, 2017,321:58-66.
[6] Cao W R, Hu C, Zhang P, et al. Salinity-mediated water self- purification via bond network distorting of H2O molecules on DRC-surface [J]. Proceedings of the National Academy of Sciences, 2023,120(45):e2311920120.
[7] Lu C, Hu C, Wu J M, et al. Endogenous substances utilization for water self-purification amplification driven by nonexpendable H2O2 over a micro-potential difference surface [J]. Environmental Science & Technology, 2024,58(52):23241-23250.
[8] Hodges B C, Cates E L, Kim J H. Challenges and prospects of advanced oxidation water treatment processes using catalytic nanomaterials [J]. Nature Nanotechnology, 2018,13(8):642-650.
[9] Gao T T, Lu C, Hu C, et al. H2O2inducing dissolved oxygen activation and electron donation of pollutants over Fe-ZnS quantum dots through surface electron-poor/rich microregion construction for water treatment [J]. Journal of Hazardous materials, 2021,420:126579.
[10] 陈怡,何银宁,汪达,等.碳氮掺杂Mn3O4催化臭氧氧化降解水中2,3-二甲基吡嗪 [J].中国环境科学, 2025,45(3):1251-1259. Chen Y, He Y N, Wang D, et al. Catalytic ozonation of 2,3- dimethylpyrazine using CN-doped Mn3O4 [J]. China Environmental Science, 2025,45(3):1251-1259.
[11] Shi Y H, Yang D X, Hu C, et al. Water self-purification via electron donation effect of emerging contaminants arousing oxygen activation over ordered carbon-enhanced CoFe quantum dots [J]. Environmental Science and Ecotechnology, 2023,20:100356.
[12] Wang Y M, Zhang P, Lyu L, et al. Preferential destruction of micropollutants in water through a self-purification process with dissolved organic carbon polar complexation [J]. Environmental Science & Technology, 2022,56(15):10849-10856.
[13] Lyu L, Wang Y M, Lu C, et al. Potential and prospects in molecular orbital level micro-electric field for low energy consumption water purification [J]. National Science Open, 2023,2:20230017.
[14] Liu S Q, Lu C, Liu J M, et al. Anti-NOM interference water purification through natural oxygen activation over DRC-catalyst obtained by pigeon manure recycling [J]. Separation and Purification Technology, 2025,354:129016.
[15] 方谦,杨东旋,孙英涛,等.过氧化物微调控铜铈双反应中心催化剂诱发氧活化驱动水净化 [J].能源环境保护, 2025,39(1):135-144. Fang Q, Yang D X, Sun Y T, et al. Peroxide-micro-modulated dual reaction center catalyst inducing oxygen activation for water purification [J]. Energy Environmental Protection, 2025,39(1):135−144.
[16] Ribeiro J P, Sarinho L, Nunes M I. Application of life cycle assessment to Fenton processes in wastewater treatment-A review [J]. Journal of Water Process Engineering, 2024,57:104692.
[17] Lyu L, Lu C, Sun Y T, et al. Low consumption Fenton-like water purification through pollutants as electron donors substituting H2O2 consumption via twofold cation-π over MoS2 cross-linking g-C3N4 hybrid [J]. Applied Catalysis B: Environmental, 2023,320:121871.
[18] Wang Y M, Zhang P, Lyu L, et al. Efficient destruction of humic acid with a self-purification process in an Fe0-FeyCz/Fex-GZIF-8-rGO aqueous suspension [J]. Chemical Engineering Journal, 2022,446:136625.
[19] Song J Y, Fan H G, Wang Y P, et al. Multifunctional iron selenate sheath of Fe-based anode achieving high-rate capacity-durability combination of aqueous hybrid energy storage devices [J]. Small, 2024,20(23):2309097.
[20] Ruan J F, Zang J H, Hu J M, et al. Respective roles of inner and outer carbon in boosting the K+ storage performance of dual-carbon- confined ZnSe [J]. Advanced Science, 2021,9(5):2104822.
[21] Ning J J, Liu J, Levi-Kalisman Y, et al. Controlling anisotropic growth of colloidal ZnSe nanostructures [J]. Journal of the American Chemical Society, 2018,140(44):14627-14637.
[22] Zhu T, Liu C, Tan X Y, et al. Se-incorporation stabilizes and activates metastable MoS2for efficient and cost-effective water gas shift reaction [J]. ACS Nano, 2019,13(10):11303-11309.
[23] Park S K, Choi J H, Kang Y C. Synthesis of hierarchical structured Fe2O3 rod clusters with numerous empty nanovoids via the Kirkendall effect and their electrochemical properties for lithium-ion storage [J]. Journal of Materials Chemistry A, 2018,6(18):8462-8469.
[24] Hong P, Zhang K, He J, et al. Selenization governs the intrinsic activity of copper-cobalt complexes for enhanced non-radical Fenton- like oxidation toward organic contaminants [J]. Journal of Hazardous materials, 2022,435:128958.
基金
国家自然科学基金项目(52470069);广东省重点领域研发计划项目纳米科技专项(2023B0101200004)
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