Nature Communications
·
2020
·Vol. 11
·期 1
·1-12
·
IF 12.121
Long Xiangdong,Li Zelong,Gao Guang,Sun Peng,Wang Jia,Zhang Bingsen,Zhong Jun,Jiang Zheng,Li Fuwei
Single-atom metal-nitrogen-carbon (M-N-C) catalysts have sparked intensive interests, however, the development of an atomically dispersed metal-phosphorus-carbon (M-P-C) catalyst has not been achieved, although molecular metal-phosphine complexes have found tremendous applications in homogeneous catalysis. Herein, we successfully construct graphitic phosphorus species coordinated single-atom Fe on P-doped carbon, which display outstanding catalytic performance and reaction generality in the heterogeneous hydrogenation of N-heterocycles, functionalized nitroarenes, and reductive amination reactions, while the corresponding atomically dispersed Fe atoms embedded on N-doped carbon are almost inactive under the same reaction conditions. Furthermore, we find that the catalytic activity of graphitic phosphorus coordinated single-atom Fe sharply decreased when Fe atoms were transformed to Fe clusters/nanoparticles by post-impregnation Fe species. This work can be of fundamental interest for the design of single-atom catalysts by utilizing P atoms as coordination sites as well as of practical use for the application of M-P-C catalysts in heterogeneous catalysis.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Liyun Zhang,Yi He,Pingya Luo,Lan Ma,Shuangshuang Li,Yiling Nie,Fei Zhong,Yuqi Wang,Li Chen
Developing the high-efficient and robust antifouling membranes for oily emulsions to achieve the purpose of prolonging the service life of the membrane shows great demand because of the restriction of hydration anti-fouling mechanism strategy to against pollution. Herein, a hydrophilic photo-Fenton-like catalyst – GO/Fe-MOF assembled stabilized polyacrylonitrile (SPAN) nanofibrous membrane with underwater superoleophobicity, robust mechanical strength and photo-Fenton self-cleaning performance was firstly designed and fabricated via ultrasonic assistance, mussel-inspired fixation and low temperature hydrothermal synthesis methods. In this work, benefiting by the regulable amounts of GO nanosheets on the SPAN@GO/M88A membrane surface, the obtained membrane possessed sub-micrometer skin layer, which guarantees the balance of fast permeation flux (920–7083 ± 47 L m −2 h −1 ) and separation efficiency (>99.2%) for diesel/water emulsion with small emulsified oils. Moreover, introduced hydrophilic Metal-organic frame nanoparticles (MIL-88A (Fe)) into modified membrane endowed underwater anti-oil-fouling and photo-Fenton catalytic degradation performance for organic contaminants. Meanwhile, the charged GO/M88A heterostructure can assist to achieve demulsification for separation of surfactant-stabilized emulsions by strong electrostatic force. More importantly, attached and irremovable contaminants on the membrane can be quickly removed by photo-Fenton self-cleaning method, and achieved over 96% of recovery flux recovery ratio, which effectively prolonged the service life of the membrane. We believe the newly designed SPAN@GO/M88A membrane with hydration antifouling and photo-Fenton self-cleaning properties can stimulate more studies on revivable separation membranes for multifunctional applications.
研究领域:
材料科学
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环境工程
·
化学工程
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GREEN CHEMISTRY
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2022
·Vol. 24
·期 6
·2613-2623
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IF 11.034
Zhao Sun,Hanpeng Liu,Sam Toan,Weizhi Shi,Dongfang Cheng,Zhiqiang Sun
Biomass to hydrogen production has been regarded as a potential approach for green hydrogen synthesis. However, carbon dioxide and bio-tar are inevitably produced, which critically restricts the refinement of biomass-derived syngas. In this study, deoxygenation-enhanced chemical looping biomass gasification (DE-CLBG) is proposed for hydrogen-rich syngas production together with CO2/H2O deoxygenation and catalytic bio-tar removal using the composite Fe/CaO as the deoxidizer. The DE-CLBG process is comprised of a deoxygenated gasification stage and a regeneration stage. During the deoxygenated gasification stage, the deoxidizer is converted under steam gasification via CaO + Fe + O2− → Ca2Fe2O5 with biochar generation; at the regeneration stage, biochar is further gasified with the achievement of deoxidizer reduction via Ca2Fe2O5 + C → CaO + Fe + COx. Experimental results show that the hydrogen production and maximum concentration upon applying 0.300 g of deoxidizer per g of biomass are 6.70 mmol and 89.61 vol%, which was increased by 287% and 27%, respectively, compared with the non-deoxygenated process. Results from the Mössbauer spectrum show that Fe0 is finally transformed into Fe3+ in the form of Ca2Fe2O5 and a small amount of Fe3O4, corresponding to the deoxygenation efficiency of 99.21%. The NMR results imply that aromatic carbon is the main form in biochar whether introducing deoxidizer or not, and deoxygenation can promote the removal of O-alkyl C.
研究领域:
能源科学
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化学工程
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环境科学
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KINETICS AND CATALYSIS
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2018
·Vol. 58
·期 6
·758-762
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IF 0.926
Shao Linjun,Chen Qiuling,Qi Chenze
Metal-Salen (M = Fe, Co, Ni, Cu, Zn) complexes were synthesized to catalyze the oxidation of benzoin to benzil with air as the “green” oxidizing reagent. The effects of temperature, base and solvent on M-Salen catalyzed oxidation of benzoin had been examined and optimized. The catalysis results showed that Co-Salen and Fe-Salen complexes were efficient to catalyze the oxidation reaction with yields over 80% while the catalytic activities of other three M-Salen complexes were poor. Moreover, the Co-Salen catalysis system could be reused three times with satisfied yield.
研究领域:
有机化学
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催化化学
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Catalysis Science & Technology
·
2015
·Vol. 6
·期 4
·1222-1232
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IF 5.426
Yunus Ahmed,Zahira Yaakob,Parul Akhtar
A SiO2-supported Fe and Ni bimetallic catalyst has been synthesized, characterized and, for the first time, tested as a heterogeneous photo-Fenton catalyst for the degradation and mineralization of methylene blue (MB) dye. The morphological, structural, and optical properties of this catalyst were analyzed using FESEM, XRD, FTIR and UV–vis spectroscopy. The photocatalytic degradation of MB has been investigated using Fe–Ni/SiO2 catalysts under visible and solar light irradiation in aqueous solutions. The effects of solution pH, H2O2 concentration, initial MB concentration, catalyst dosage and light intensity on the degradation of MB have been systematically investigated. An almost complete degradation was achieved within 60 min with a solution pH of 3.00, a H2O2 concentration of 3.0 mM L−1 and a catalyst dose of 0.85 g L−1. The degradation and total organic carbon (TOC) removal efficiencies were 99.80% and 86.19%, respectively, for sunlight. However, the values were only 99.01% and 75.71% for visible light. These results suggested that Fe–Ni/SiO2 possesses significant catalytic activity, and the solar-Fenton process is a feasible method for degrading and mineralizing the MB dye compared with artificial visible light. The catalytic action is attributed to H2O2 and the formation of hydroxyl radicals (˙OH) by Fe(III) in Fe–Ni/SiO2via the photo-Fenton reactions. Furthermore, we determined that the catalyst activity can be replicated in successive experiments without a significant decline in the Fe–Ni/SiO2 and H2O2 processing efficiency under light irradiation. Our results will be useful for future improvement of active heterogeneous photo-Fenton catalysts for developing organic dye-containing wastewater treatments.
研究领域:
环境科学
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催化化学
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DESALINATION
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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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FUEL PROCESSING TECHNOLOGY
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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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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 29
·期 51
·77851-77863
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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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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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JOURNAL OF HAZARDOUS MATERIALS
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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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