DESALINATION
·
2026
·
IF 9.9
Linkai He,Xingqiang Wu,Yun Tian,Yixin Pan,Faquan Wu
The release and dispersion of uranium during mining activities and fuel/waste management processes in nuclear power plants pose serious environmental risks, particularly in aqueous systems. In such environments, uranium exhibits high solubility and strong mobility, leading to severe radioactive contamination of groundwater, soil, and ecosystems. Therefore, remediating uranium-contaminated environments remains a significant scientific and technological challenge. To address this issue, the present study exploits the high specific surface area and tunable pore architectures/functional sites of metal-organic frameworks (MOFs). Using a controlled synthesis strategy, a core-shell (Fe-Ni) galvanic cell structure was constructed and integrated with MIL-100(Fe) to fabricate the Ni-Fe-MIL-100(Fe) composite, enabling highly efficient and synergistic removal of U(VI) via an “adsorption-reduction-complexation” mechanism. Experimental results demonstrate that the maximum uranium uptake capacity reached 3038.19 mg·g −1 at 303 K and pH = 5, with a significantly enhanced removal efficiency. The kinetic analysis indicates that the uranium adsorption process is well described by the pseudo-second-order model. Combined with density functional theory (DFT) calculations, the electronic transfer channels of the structure were elucidated, revealing that they drive the reduction of U(VI) and facilitate its coordination and immobilization at multi-metal and oxygen-containing sites. These findings confirm that U(VI) removal by the composite material proceeds via a coupled chemical reduction and complexation process, thereby clarifying the underlying adsorption mechanism. Moreover, in mixed-ion solutions and real seawater, the composite maintains high adsorption capacity and excellent selectivity, demonstrating strong potential for uranium immobilization and recovery in the remediation of radioactive wastewater.
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Advanced Sustainable Systems
·
2022
·Vol. 7
·期 2
·2200378
·
IF 6.737
Ziying Xiong,Hai Hu,Ziqi Cao,Yaxin Hu,Di Sun,Hengfei Qin,Shifei Kang
Photocatalysis water treatment without artificial energy is cost-effective, waste-free and sustainable. Coventional powder photocatalysts have tiny contact surfaces, low catalytic efficiency, and are difficult to recycle and reuse, restricting their usage. Herein, a Lignin@t-FeC 2 O 4 /g-C 3 N 4 material is developed by engineering hollow quadrangle t-FeC 2 O 4 and g-C 3 N 4 nanosheets on lignin membranes through facile impregnation coating and precipitation reaction. Fast mass transport, catalytic activity and accessibility characterize hollow tetragonal FeC 2 O 4 · 2H 2 O. TEM, SEM and FTIR show that lignin binds t-FeC 2 O 4 and g-C 3 N 4 . The g-C 3 N 4 nanosheets are uniformly wrapped on the surface of lignin fibers, and t-FeC 2 O 4 is loaded between them. This structure increases visible light absorption and active site-contaminant contact. The chain reaction produces extremely active hydroxyl radicals from hydrogen peroxide because the Lignin@t-FeC 2 O 4 /g-C 3 N 4 modules are rich inFe II , according to XPS. Transient photocurrent response curves and electrochemical impedance spectroscopy suggest a promoted charge migration and isolation at the redox reaction interface in the Lignin@t-FeC 2 O 4 /g-C 3 N 4 system. As a result, Lignin@t-FeC 2 O 4 /g-C 3 N 4 degrades 99% Rhodamine B within 40 minutes, and this performance is stable even under difficult conditions, such as low hydrogen peroxide concentration and high pH. This study combines lignin membranes with the photo-Fenton reaction, and thus provides new concept for the development and application of membranes and photocatalysis.
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CHEMOSPHERE
·
2022
·
IF 8.943
Lina Wang,Hanpei Yang,Li Kang,Mi Wu,Yuankun Yang
In this work, Ag/AgCl/FeOCl (Ag–Fe) catalysts were successfully prepared via multistep routes in which Ag was uniformly anchored to the enriched Cl sites provided by exfoliated FeOCl nanosheets. Among these Ag–Fe catalysts, 5% Ag–Fe exhibited the highest pseudo first-order kinetic constant 0.1056 min −1 for photo-Fenton degradation of Rhodamine B (RhB), which was 11 times higher than that of FeOCl (0.0096 min −1 ). Ag–Fe catalysts exposed more coordinatively unsaturated Fe active sites to coordinate with H 2 O 2 due to the cleavage of Fe–Cl bond. The exposed coordinatively unsaturated Fe(III) active sites could capture the photoinduced electrons and reduce them to Fe(II), which boosted the separation efficiency of photogenerated charge carriers. Meanwhile, the photogenerated electrons of Ag 0 transferred to the FeOCl, promoting the reduction of Fe(III) to Fe(II). In addition, the intensified visible light adsorption (SPR effect) was achieved after introducing Ag/AgCl nanoparticles on exfoliated FeOCl. Hydroxyl radicals (·OH) and holes (h + ) were determined as the main reactive oxidative species (ROS) in the photo-Fenton degradation process.
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 51
·77851-77863
·
IF 5.19
Jiang Changjin,Zhang Ting,Li Shuhui,Yang Zhaoguang
Fe(III)-chitosan and Fe(III)-chitosan-CTAB composites were prepared using an ionotropic gelation method. Various techniques were used to analyze the morphology, structure, and property of the adsorbents, including SEM, EDS, FT-IR, XPS, and zeta potential. Compared with Fe(III)-chitosan, Fe(III)-chitosan-CTAB was more effective for As(V) adsorption at a wide range of pH (3.0–8.0). The adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB could reach equilibrium in 20 min, and their maximum adsorption capacities were 33.85 and 31.69 mg g ‒1 , respectively. The adsorption kinetics was best described by the pseudo-second-order model ( R 2 = 0.998 and 0.992), whereas the adsorption isotherm was fitted well by the Freundlich model ( R 2 = 0.963 and 0.987). The presence of H 2 PO 4 – significantly inhibited the adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB, and humic acid also led to a slight decrease in As(V) adsorption by Fe(III)-chitosan-CTAB. Over 94% of As(V) at the initial concentration of no more than 5 mg L –1 was removed from real water by the two adsorbents. 1% (w/v) NaOH solution was determined to be the most suitable desorption agent. Fe(III)-chitosan and Fe(III)-chitosan-CTAB still maintained their initial adsorption capacities after five adsorption–desorption cycles. Based on different characterization results, both electrostatic attraction and surface complexation mechanisms played important roles in As(V) adsorption on Fe(III)-chitosan and Fe(III)-chitosan-CTAB.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Fengxian Zhang,Ye Chen,Yang Liu,Xupo Liu,Shuyan Gao
Constructing highly efficient and durable non-noble metal modified carbon catalysts for oxygen reduction reaction (ORR) in the whole pH range is essential for energy conversion devices but still remains a challenge. Herein, the Fe/Fe 3 C nanoparticles and Fe-N X species anchored on the interconnected mesoporous carbon materials are fabricated through an economical and facile template-assisted polymerization-pyrolysis strategy. The catalyst exhibits unique features with the electronic interaction between Fe/Fe 3 C and Fe−N X , large specific surface area and high mesoporous structure as well as nitrogen doping in porous carbon skeletons, which can effectively catalyze ORR over the full pH range. In an alkaline electrolyte , the optimized catalyst displays favorable ORR performance with positive onset potential ( E onset = 0.91 V), half-wave potential ( E 1/2 = 0.83 V), long-term cycles stability and methanol tolerance, exceeding those for the commercial Pt/C. Furthermore, the prepared catalyst could be directly assembled into the alkaline Zn−air battery that exhibits the open-circuit voltage of 1.44 V, high power density of 96.0 mW cm −2 and long-term durability. Therefore, the template-assisted polymerization-pyrolysis strategy provides a promising route for designing high-performance non-noble metal decorated ORR electrocatalysts .
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Huimin Hu,Qiwu Zhang,Chao Wang,Min Chen,Mengfei Chen
Iron manganese oxide resources are widely derived from the geological structure , and their combinations play an important role in the migration and transformation of arsenic. Iron oxide and manganese oxide exist generally in a mixed state in Fe-Mn oxides synthesized via the well studied co-precipitation methods using potassium permanganate and manganese/iron sulfates. Herein, a newly designed Fe-Mn-O compositing oxide with Fe-MnO 2 , Mn-Fe 2 O 3 , (Fe 0.67 Mn 0.33 )OOH solid solution and FeOOH as the main components, simply through solvent-free mechanical ball milling pyrolusite (MnO 2 ) and ferrihydrite (FeOOH) together has been reported. Atomic-scale integrations by doping Fe and Mn with each other were detected and an adsorption-oxidation bifunctionality was achieved, where Fe-doped MnO 2 served as oxidizer for As(III) and amorphous/ground FeOOH acted as adsorbent first for As(III) and then As(V) from the oxidization. The maximal adsorption for As(III) could reach 44.99 mg/g and over 82.5% of As(III) was converted to As(V). More importantly, high removal ability of arsenic worked in a wide pH range of 2–10.5%, and 87.2% of its initial adsorption-oxidation capacity could be kept even after 5-cycles reuse for treating 20 mg/L As(III) with a dosage at 1 g/L. Together with the enhanced adsorption capacity by the milled FeOOH, surface electron transfer efficiency of the developed Fe-MnO 2 surrounded with Mn-Fe 2 O 3 has been studied for the first time to understand the oxidization effect to As(V). Besides the environment-friendliness of ball milling method, the prepared sample is quite stable without noticeable metal release into solution. Mechanism studies of arsenic removal by the as-prepared Fe-Mn-O oxide provide a new direction for improving the oxidation efficiency of MnO 2 to As(III) based on the widely available cheap Mn and Fe oxides, contributing to the development of advanced oxidization process in the treatment of waste water.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2020
·
IF 3.99
Qingwen Long,Feng Liu,Yanjie Yuan,Yuting Dai,Chunli Wang,Xuheng Li,Jing Zhang
In this study, heterogeneous Fenton-like catalyst, nano-Fe° encapsulated in hydrothermal carbon (Fe°/HTCC), was prepared via a green chemistry route, aiming at increasing the degradation efficiency of p-chlorophenol (4-CP) by controlling the stability of the catalyst and Fe(III)/Fe(II) cycling in the advanced oxidation process. The degradation of 4-CP by heterogeneous Fenton reactions was conducted with the assistance of visible light, which was monitored with the aid of the HPLC and total organic carbon analysis. The results revealed that Fe°/HTCC composite markedly enhanced both the degradation (100 %) and the mineralization efficiency (∼73.9 %) for 100 mg/L 4-CP within 60 min at pH 4.0. More importantly, the catalyst presented a high stability to resist the side oxidation, where the removal efficiency was maintained even after 5 successive cycling experiments. Electron spin resonance confirmed that in the presence of both HTCC and visible light irradiation greatly enhanced the production of •OH for the degradation and mineralization of 4-CP, which can be attributed to the enhancement of Fe(III)/Fe(II) cycling. This study paves a new way toward the rational design of Fe°–carbon composites as heterogeneous Fenton-like catalysts for potential applications into wastewater treatment.
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FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Qin Wen,Dongxu Tian,Zequan Zeng,Fei Qi,Zhanggen Huang
Fe-N-C catalysts with magnetism were successfully synthesized through one-step heat treatment of ferrosoferric oxide and covalent organic frameworks composite (Fe 3 O 4 @COF) as heterogeneous catalysts for persulfate (PS) activation and 2,4-dichlorophenol (2,4-DCP) degradation. The morphologies, compositions and active sites were adjusted by changing the pyrolysis temperature. The catalyst prepared at 900 °C showed excellent activity with 2,4-DCP removal of 90% in 60 min, recycling convenience and regeneration stability. Large surface area (342 m 2 g −1 ) and hierarchical porous structure benefited PS activation. It was proved that the radical and non-radical mechanisms coexisted in Fe-N-C-900/PS system with the results of quenching and electrochemical experiments. Roles of graphitic N and Fe-N X were distinguished. Graphitic N and Fe-N X sites palyed an prominent part in the non-radical activation process , in which Fe-N X was closely related to the electron transfer activation mechanism. Density functional theory (DFT) calculation further verified that the Fe N 2 was the key site for PS activation. 2,4-DCP degradation was proved to be a toxicity-attenuation process according to the biotoxicity analysis. The effects of several operating parameters and degradation of different model pollutants were also systematically evaluated, and possible activation mechanism was proposed.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2017
·
IF 3.615
Bo Xu,Xuejiao Li,Zhiming Chen,Tao Zhang,Cuncheng Li
Pd@MIL-100(Fe) composite nanoparticles were synthesized and characterized by high-resolution transmission electron microscopy (HRTEM), powder X-ray diffraction analysis, nitrogen adsorption-desorption analysis, X-ray photoelectron spectroscopic (XPS) analysis, energy-dispersive X-ray spectroscopy (EDS) and element mapping. Due to the local restriction or confinement effect of the unique pore/surface structure within the MIL-100(Fe) nanospheres , small Pd nanoparticle (4–6 nm) were obtained with high stability without using any surfactant as stabilizer . The as-synthesized Pd@MIL-100(Fe) composite nanoparticles were then employed for the catalytic reduction of 2/3/4-nitrophenol, which exhibiting high catalytic activity and recyclability attributed to the synergistic effect between Pd nanoparticles and MIL-100(Fe) nanospheres.
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Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Guiyuan Yang,Fangyuan Hu,Li-Li Cui,Meihong Fan,Xin Ge,Xingquan He,Wei Zhang,Tewodros Asefa
Sustainable electrochemical energy conversion and storage systems are expected to alleviate the energy shortages and environmental crisis that are currently facing the world. To bring the large-scale deployment of these energy systems to reality, the development of highly efficient, sustainable, and stable electrocatalysts is key. In this work, an electrocatalyst composed of homonuclear paired Fe sites coordinated onto N-doped carbon, labelled as Fe2–N–C-900, is reported. The material is synthesized by preparing, and then pyrolyzing at 900 °C, Fe(III)-tetrapyridinylporphyrin-modified zeolitic imidazolate framework-8 (ZIF-8). The electrocatalyst displays excellent activity for the oxygen reduction reaction (ORR), with an onset potential of 0.990 V vs. RHE, a positive half-wave potential of 0.869 V vs. RHE, and a limiting current density of 6.7 mA cm−2, which are all superior to those of the benchmark noble metal-based ORR catalyst Pt/C. This is attributed to its high-density of catalytically active Fe2–N6 sites, large electrochemically active surface area, and small charge transfer resistance. The electrocatalyst also functions well for the ORR on an air electrode in an aqueous zinc–air battery while showing high catalytic activity, remaining stable, and giving a peak power density of 166.3 mW cm−2. Its performance here, too, exceeds that of a Pt/C-based zinc–air battery.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Leiduo Lai,Peng Zhou,Hongyu Zhou,Minglu Sun,Yue Yuan,Yang Liu,Gang Yao,Bo Lai
Coupling dithionite (DNT) with FeVO 4 induced PMS activation (FeVO 4 /PMS/DNT) effectuates fast heterogeneous Fe(III) reduction to generate multitudinous reactive oxygen species (ROS) for fast degradation of carbamazepine (2.5 mg/L, >90 % degradation efficiency within 300 s) in batch mode. The Fe(III)/Fe(II) circulation propelled by DNT and reduced V species experiences two stages. DNT induces SO 2 − generation, which is a highly active species with strong reducibility for Fe and V reduction. The reduced V species donate electrons to ≡Fe(III) via Fe-O-V bond rather than directly react with PMS, implying introducing polyvalent V to modulate Fe-based materials intensifies DNT utilization and alleviates ROS quenching effects. Moreover, FeVO 4 crystalline form regains after reaction, and FeVO 4 /PMS/DNT system has an excellent reutilization and strong resistance to natural waters. Our discovery sheds new light on acceleration of heterogenous Fe(III)/Fe(II) circulation to promote Fenton-like oxidation , it may be a long-lasting strategy for water remediation.
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Energy Storage Materials
·
2024
·
IF 18.9
Jing Peng,Bihua Hu,Zhitong Li,Xiongwei Zhong,Junwei Shi,Shuyu Cui,Xingzhu Wang,Baomin Xu
Dual-metal single-atom catalysts with heteronuclear active sites exhibit superior oxygen catalysis performance than their single-atom counterparts, facilitating the practical applications in advanced electrochemical energy devices. Herein, a Fe-Cu dual-metal single-atom catalyst with Fe-N 6 and Cu-N 1 S 2 coordination environment (FeCu-DSAs/NSC) is reported. Due to the synergism of bimetallic active sites and asymmetric heteroatom coordination, the resultant FeCu-DSAs/NSC displays better bifunctional catalytic performance (a small potential gap between the E η10 and E 1/2 , ΔE=0.647 V) when compared with the counterparts (Pt/C+IrO 2 and Cu-ISAs/NSC), as well as surpassing most of bifunctional metal atom-based catalysts reported to date. As expected, FeCu-DSAs/NSC based rechargeable zinc-air battery shows remarkable superiority than commercial Pt/C+IrO 2 benchmark, resulting in a high peak power density (230.66 mW cm −2 ), open-circuit voltage (1.464 V) and long-term cycling stability (up to 350 h at 10 mA cm −2 ).
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