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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Amino-rich Ag-NWs/NH2-MIL-125(Ti) hybrid heterostructure via LSPR effect for photo-assist uranium extraction from fluorine-containing uranium wastewater without sacrificial agents

Boyuan Tu,Kaifu Yu,Dengjiang Fu,Li Zhou,Ruixiang Wang,Xinying Jiang,Huanhuan Liu,Xin Cao,Xiang Gong,Rong He,Yongjian Tang,Tao Chen,Wenkun Zhu

Photo-assist uranium extraction from fluorine-containing uranium wastewater by building semiconductor-plasma material heterostructure is a forward-looking strategy, which not only effectively accelerates F-U separation via the LSPR effect but also impacts the intensity of binding between U (VI) and site. Here, we developed an amino-rich Ag-NWs/NH 2 -MIL-125(Ti) (AgNW/N-M(Ti)) hybrid nanowires with LSPR effect for photo-assist uranium extraction. Accordingly, the AgNW/N-M(Ti) hybrid nanowires presented 90.4% removal efficiency for U(VI) without a sacrificial agent at the U: F molar ratio of 1:20. By virtue of In-situ KPFM, we identify hot electrons generated over AgNW were transferred to amino-rich N-M(Ti) to efficiently reduce the U(VI) adsorbed on the N-M(Ti), which effectively enhances the excellent uranium removal performance of AgNW/N-M(Ti) hybrid nanowires. This strategy may open a paradigm for the development of advanced heterojunctions with the LSPR effect as catalysts for photo-assisted uranium extraction from fluorine-containing uranium wastewater.

研究领域: 材料科学 · 环境科学
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ENVIRONMENTAL RESEARCH · 2024 · IF 7.7

Experimental and DFT calculation study on the efficient removal of high fluoride wastewater from metallurgical wastewater by kaolinite

Zhen Zeng,Qisheng Huang,Qian Li,Jia Yan,Xiaoyu Zhao,Lei Huang,Sijie Zhao,Hongguo Zhang

Fluoride pollution and water scarcity are urgent issues. Reducing fluoride concentration in water is crucial. Kaolinite has been used to study adsorption and fluoride removal in water and to characterize material properties. The experimental results showed that the adsorption capacity of kaolinite decreased with increasing pH. The highest adsorption of fluoride occurred at pH 2, with a capacity of 11.1 mg/g. The fluoride removal efficiency remained high after four regeneration cycles. The fitting results with the Freundlich isotherm model and the external diffusion model showed that the non-homogeneous adsorption of kaolinite fit the adsorption behavior better. Finally, the adsorption mechanism was analyzed by FT-IR and XPS. The binding energies of various adsorption sites and the chemical adsorption properties of atomic states were discussed in relation to DFT calculations. The results showed that Al and H sites were the main binding sites, and the bonding stability for different forms of fluoride varies, with the size of Al–F (−7.498 eV) > H–F (−6.04 eV) > H–HF (−3.439 eV) > Al–HF (−3.283 eV). Furthermore, the density of states and Mulliken charge distribution revealed that the 2p orbital of F was found to be active in the adsorption process and was the main orbital for charge transfer.

研究领域: 环境科学 · 材料科学
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WATER AIR AND SOIL POLLUTION · 2025 ·Vol. 236 ·期 10 ·1-15 · IF 3

Efficient Removal of Fluoride From Water by Polymeric Aluminum Zirconium Chloride: Performance and Mechanism From Flocculation Aspects

Sun Yongjun,Hu Zhihao,Wang Zihan,Zhang Can,Sun Wenquan

In this work, polymeric aluminum zirconium chloride (PAZC), a defluoridating flocculant, was prepared using calcium aluminate and zirconium tetrachloride as the main materials, and its defluoridation performance was evaluated. At pH 7 and PAZC dosage (Zr) of 50 mg•L −1 , the flocculation and defluorination rates of PAZC in simulated fluorinated wastewater with initial fluoride ion concentrations of 10, 8, and 5 mg•L −1 were 90.90%, 89.38%, and 92.2%, respectively, and the residual fluoride ion concentration in the solution was reduced to 0.91, 0.85, and 0.39 mg•L −1 , respectively. The degree of the effects of the same concentration of anions on the flocculation and fluoride removal performance of PAZC was in the order of SiO 3 2− >PO 4 3− >CO 3 2− >NO 3 − >Cl − >SO 4 2− . Characterization results indicated that PAZC was a polymer containing hydroxyl bonds of zirconium–aluminum metal ions, and the surface of PAZC had a tight, dense, porous nature. Under optimum flocculation conditions, the average particle size of the flocs obtained after fluoride removal by PAZC flocculation was 2.54 μm, and the flocculation mechanism was dominated by adsorption, electro-neutralization, and ion exchange when the dosage of the PAZC was 40–50 mg•L −1 and the pH was 5–7. It is proved that the composite flocculant PAZC has good application prospects and can provide guidance for the treatment of actual fluorine-containing wastewater.

CAS / MDL: 1344-09-8
研究领域: 环境科学 · 水处理技术 · 化学工程 · 材料科学 · 环境工程
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Journal of Water Process Engineering · 2025 · IF 6.7

Synergistic Co-pyrolysis of Fenton sludge biochar for fluoride removal: Strategy optimization and cooperative adsorption mechanisms

Siqi Tong,Lei Zhang,Xuemin Yu,Guangbing Liu,Haibo Xu,Weijing Liu,Jinyou Shen,Yi Wang

Fluoride-containing wastewater posed significant environmental and health risks, and the high costs of current defluoridation adsorbents highlight the pressing need for cost-effective solutions. To achieve the advanced treatment of fluoride-containing wastewater and the resource utilization of solid waste, a pyrolytic-hydrothermal carbon adsorbent was developed from Fenton sludge (FS) and rice straw (RS). FS/RS-1:2BC, synthesized at 600 °C pyrolysis and 200 °C hydrothermal treatment with a 1:2 mass ratio, exhibited the highest fluoride ions (F − ) adsorption capacity of 10.57 mg g −1 . Physicochemical characterization revealed FS/RS-1:2BC consisted of porous graphitic carbon from RS and α-Fe₂O₃ from FS, with abundant oxygen-containing groups and a large surface area for F − adsorption. Adsorption kinetics and thermodynamic fitting indicated the adsorption of F − was primarily relied on chemical interactions (chemical precipitation, ligand complexation, ion exchange, electrostatic attraction) between F − and the homogeneous monolayer surface, with physical adsorption and intraparticle diffusion as secondary mechanisms. FS/RS-1:2BC exhibited excellent stability and applicability, with a broad pH acceptance range (pH 3.5–8). It maintained 9.58 mg g −1 adsorption capacity under weakly alkaline and achieved around 90 % adsorption efficiency in coexisting anions. Regeneration experiments indicated that FS/RS-1:2BC retained 81.9 % adsorption capacity after five regeneration cycles. The development of FS/RS-1:2BC not only provided a cost-effective adsorbent for low-concentration fluoride removal from tailwater but also established a new approach for resource utilization of solid wastes.

研究领域: 环境科学 · 材料科学 · 化学工程 · 废物管理 · 水处理
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Fabricating ultrafine zirconium oxide based composite sorbents in “soft confined space” for efficiently removing fluoride from environmental water

Danqing Shen,Yulin Song,Xuping Chen,Yongquan Zhou,Hao Li,Jianming Pan

The fluoride pollution in environmental water can cause serious health problems, and the fluoride removal by sorbent is an effective strategy, and challenges by its poor selectivity and low capacity. Herein, we reported a new insight into the fabricating ultrafine zirconium oxide (ZrO 2 ) based composite sorbents (E-ELP-Zr) in “soft confined space” and efficient fluoride removal from water. It relies on the confined aqueous phase of Oil-in-Water (O/W) high internal phase emulsions (HIPEs) as droplet reactor, and ultrafine ZrO 2 particles (<10 nm) were achieved via the controllable in situ growth onto lipase immobilized poly(styrene-co-glycidyl methacrylate) nanospheres. E-ELP-Zr exhibited outstanding capacity for defluorination (135.8 mg g −1 at 298 K), quick adsorption rate in the first 10 min, and the superior selectivity against co-occurring anions (Cl - , SO 4 2− , NO 3 – and CO 3 2– ). The adsorption mechanism of fluoride on E-ELP-Zr was strong electrostatic attraction as well as the specific affinity of zirconium. After five regeneration cycles, the adsorption capacity of E-ELP-Zr slightly decreases to 88.55% of the initial value, and the excellent interfacial stability was benefited from covalently attached lipases. More importantly, this hybrid sorbent can be successfully applied for low level (7.15 mg L -1 ) of fluoride decontamination from actual sample of fluorinated wastewater, which endowed a distribution coefficient ( K d ) as high as 6.3 L g −1 .

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理
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