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Journal of Water Process Engineering · 2024 · IF 6.3

Novel pretreatment technologies for sludge dewatering and dissolution: Humic acid combine with sodium percarbonate and different iron species

Denglong Lu,Shanshan Zhang,Yang Song,Huanying Ge,Zhaoguang Yang,Haipu Li

Large amounts of waste activated sludge are generated daily worldwide, posing significant environmental challenges. A promising sludge management method is urgently needed. This study innovatively introduces humic acid (HA) into a sodium percarbonate (SPC) sludge treatment system to enhance dewatering and dissolution processes. Therein, SPC was activated by dissolved iron (Fe(II) or Fe(III)) or solid phase iron (zero-valent iron or magnetite (Fe 3 O 4 )). Results confirmed that Fe(III)/SPC/HA could improve the dewaterability of sludge without pH adjustment, with the capillary suction time decreasing from 123.6 ± 1.32 s (control) to 58.10 ± 4.35 s, which was comparable with that of the Fe(III)/SPC at pH 3.0. Meanwhile, Fe 3 O 4 /SPC/HA significantly enhanced sludge dissolution, and the released protein and polysaccharide levels were 2.98 and 7.08 times higher than that in the control. Both Fe(III)/SPC/HA and Fe 3 O 4 /SPC/HA reduced heavy metals and pathogens in the sludge while increasing HA content in filtrates, all of which were beneficial for subsequent sludge disposal and HA recycling, offering cost-effective technologies for sludge treatment.

CAS / MDL: 15630-89-4
研究领域: 环境科学 · 污水处理
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ChemCatChem · 2022 ·Vol. 15 ·期 1 ·e202201234 · IF 5.497

Selective Oxidation of Methane into Formic Acid over ZIF-8-Encapsulated Mononuclear Fe Species under Mild Conditions

Lu Lin,Guikai Zhang,Liqun Kang,Tao Yu,Yang Su,Guang Zeng,Shengqi Chu,Wenhao Luo

Graphical Methane oxidation : Highly dispersed mononuclear Fe species encapsulated by ZIF-8 (Fe-ZIF-8) afford an optimal turnover rate of ∼45 mol C1 mol Fe −1 h −1 and a formic acid selectivity of ∼97 % in the direct methane oxidation at 323 K. The direct catalytic oxidation of methane into C1 oxygenates is a promising approach for methane valorization. However, the difficulties in CH 4 activation and inhibition of over-oxidation hinder the development of efficient catalysts for this transformation. Herein, highly dispersed Fe species confined by ZIF-8 are developed for the direct transformation of methane into value-added C1 oxygenates with H 2 O 2 as oxidant at 323 K. The as-obtained Fe-ZIF-8 can afford an optimal turnover rate (TOR) of ∼45 mol C1 mol Fe −1 h −1 . Note that the selectivity to HCOOH is ∼97 %, outstanding among the reported Fe-based heterogeneous catalysts. Combined analysis of X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, ultraviolet-visible diffuse reflectance spectroscopy and 57 Fe Mössbauer spectroscopy suggests that the catalytically active sites in Fe-ZIF-8 are mononuclear six-coordinated Fe 3+ species. The confinement of mononuclear Fe species within a porous metal-organic framework material can provide an exquisite, enzyme-like performance for highly selective oxidation of methane towards formic acid under mild conditions.

CAS / MDL: 14024-18-1 693-98-1
研究领域: 化学 · 催化科学
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Journal of Energy Storage · 2020 · IF 3.762

Tuning nitrogen doping types and pore structures in carbon nanosheets as electrodes for supercapacitor by controlling existence form of iron species

Rui Zhao,Hui Peng,Hailing Wang,Jing Liang,Yaya Lv,Guofu Ma,Ziqiang Lei

Nitrogen-doped hierarchically porous carbon (HPC) with plate-like intertwined nanosheets structures and different distributed pores is fabricated by directly carbonize phenyl polyimide nanosheets with FeCl 3 •6H 2 O as activator and regulator. Inspiringly, the nitrogen doping types, morphologies, pore structures and nitrogen content of HPC can regulate by controlling the existence form of Fe species in HPC under different carbonization temperature. The optimal HPC sample possesses the uniform distributed pores, the high N content (7.8 wt%) and the appropriate specific surface area. Especially, the optimal HPC shows satisfactory specific capacitance of 254 F g −1 at the current density of 0.5 A g −1 in 2 M KOH electrolyte. Moreover, when it comes to both positive and negative electrode materials for two-electrode symmetric cell, the operating voltage window of the symmetric cell can extend up to 1.8 V and provide an energy density of 14.4 W h kg −1 at power density of 225 W kg −1 , as well as an excellent cycling stability of 93% capacitance retention after 15 000 cycles in 0.5 M Na 2 SO 4 electrolyte.

研究领域: 材料科学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Removal of Microcystis aeruginosa by natural pyrite-activated persulfate: Performance and the significance of iron species

Xiaoxian Zheng,Xiaojun Niu,Dongqing Zhang,Xingyao Ye,Jinling Ma,Mengyu Lv,Zhang Lin

In this study, the feasibility of removing Microcystis aeruginosa by heterogeneous persulfate activation using ubiquitous natural pyrite was investigated. The results indicated the significant degradation efficiency of chlorophyll-a (over 90%) was obtained in pyrite/persulfate (PS) system, which was influenced by various experimental parameters, including pyrite loading, PS dosage, the initial pH and coexisting common anions. The EPR, SEM, TEM, XPS and zeta potential analysis indicated that the reactive oxygen species ( ∙ S O 4 - , ·OH, · O 2 - and 1 O 2 ) generated during PS activation using pyrite played an essential role in facilitate the destabilization of algae cells to further destroyed them, while the continuous formation of oxidation layer consisting of FeOOH and Fe 2 O 3 on pyrite surface and dissolved Fe(III) could favor coagulation of algae. Furthermore, pyrite/PS system was not only effective in destructing the cellular morphology and reducing the viability of algae, but also able to control algal organic matter, which could avoid yielding serious secondary pollution. This study highlighted the dual role of iron species as both catalyst and coagulant for M. aeruginosa removal and demonstrated that it is highly advantageous to employ pyrite/persulfate system with high-efficiency and cost-effectiveness to eliminate algae.

研究领域: 环境科学 · 水处理技术
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Science China-Chemistry · 2021 ·Vol. 64 ·期 7 ·1088-1095 · IF 9.445

The selective deposition of Fe species inside ZSM-5 for the oxidation of cyclohexane to cyclohexanone

Zhai Liming,Zhang Bin,Liang Haojie,Wu Huibin,Yang Xinchun,Luo Gen,Zhao Shichao,Qin Yong

The design of efficient iron-based catalysts remains a great challenge for selective cyclohexane oxidation to cyclohexanone under mild conditions. Because of the complex distribution of iron location on the support, the selectivity is always low. Here, we report a general strategy to selectively deposit highly-dispersed FeO x into the micropore of ZSM-5 by atomic layer deposition (ALD). The framework of ZSM-5 and the Brønsted acid sites are intact during ALD, and the Fe species are selectively deposited onto the defect and Lewis acid sites of ZSM-5. Besides, more Fe-O-Si bonds are formed over FeO x /ZSM-5 with a low loading of Fe, while FeO x nanoparticles are generated at high Fe loading. They cannot be realized by the traditional solution method. The obtained FeO x /ZSM-5 catalysts perform high selectivity of cyclohexanone (92%–97%), and ALD cycle numbers of FeO x control the activity. Compared with the Fe nanoparticles, the Fe-O-Si species performs higher turnover frequency and stability in the oxidation reaction.

研究领域: 催化化学 · 材料科学
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MICROCHIMICA ACTA · 2017 ·Vol. 185 ·期 1 ·1-7 · IF 4.58

Amperometric determination of hydroquinone and catechol using a glassy carbon electrode modified with a porous carbon material doped with an iron species

Huang Wei,Zhang Ting,Hu Xiaoya,Wang Yang,Wang Jianmin

A porous carbon material doped with an iron species (Fe/PC) was prepared by carbonizing a mixture of zeolitic imidazolate framework-8 in the presence of iron(II) ions. The resulting material was characterized by X-ray diffraction, nitrogen adsorption isotherms, transmission electron microscopy, and by Raman and X-ray photoelectron spectroscopy. Fe/PC was the deposited on the surface of glassy carbon electrode (GCE) to obtain a sensor for amperometric determination of phenolic compounds. The unique catalytic activity, good electrical conductivity and hierarchical structure of the Fe/PC composite results in good electrooxidative activity towards hydroquinone (HQ; typically at 44 mV) and catechol (CC; typically at 160 mV). Under optimal conditions, the amperometric responses are linear in the range from 0.1 to 120 μmol · L −1 for HQ, and from 1.0 to 120 μmol · L −1 for CC. The respective detection limits are 14 and 33 nmol · L −1 . The sensor is highly selective against potential interferents and was successfully applied to the determination of HQ and CC contents in (spiked) water samples. An amperometric sensor for phenolic compounds was constructed by using a metal-organic framework derived iron doped porous carbon material.

CAS / MDL: 7758-94-3 693-98-1
研究领域: 分析化学 · 材料科学 · 环境科学
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Journal of Cleaner Production · 2019 · IF 6.395

Carbothermal reduction for preparing nZVI/BC to extract uranium: Insight into the iron species dependent uranium adsorption behavior

Huimin Zhang,Yang Ruan,Aiping Liang,Kaimin Shih,Zenghui Diao,Minhua Su,Li'an Hou,Diyun Chen,Hui Lu,Lingjun Kong

Currently, a lot of uranium containing wastewater was generated in China, which required efficient treatment before being discharged. Immobilization of uranium on ZVI has attracted many concerns from researchers in the world wide. Surface oxidation and agglomeration limited the efficiency of nano zero-valent iron (nZVI) in remediation of uranium pollution. In this work, a green carbothermal reduction process was conducted to prepare environmental friendly biochar-supported ZVI (nZVI/BC). Immobilization behavior of uranium on nZVI/Cs, oxidized nZVI/Cs and Fe 3 O 4 from wastewater were investigated. The iron salt was converted into iron oxides at 700 °C, further being reduced into nZVI in the presence of ferric chloride and ferric nitrate being carbonization of starch at 800 and 900 °C. The uranium adsorption capacities were different from the carbonization temperature and iron sources, which depended on the transformation of iron species. The maximum adsorption capacities of nano-flake Fe Cl /C (1:4–900) and nanoparticles Fe N /C (1:4–900) for U(VI) were 34.82 and 55.14 mg/g. The removal efficiencies of Fe Cl /C (1:4–900) and nanoparticles Fe N /C (1:4–900) were higher than that of 44% for C–Fe 3 O 4 . The SEM-mapping and XPS analysis of nZVI/Cs after U(VI) adsorption indicated that the immobilization of U(VI) was ascribed to simultaneous adsorption and reduction.

研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2024 · IF 10.8

Insights into the Roles of Different Iron Species on Zeolites for N2O Selective Catalytic Reduction by CO

Yunshuo Wu,Xuanhao Wu,Jie Fan,Haiqiang Wang,Zhongbiao Wu

Iron zeolites are promising candidates for mitigating nitrous oxide (N2O), a potent greenhouse gas and contributor to stratospheric ozone destruction. However, the atomic-level mechanisms by which different iron species, including isolated sites, clusters, and particles, participate in N2O decomposition in the presence of CO still remain poorly understood, which hinders the application of the reaction in practical technology. Herein, through experiments and density functional theory (DFT) calculations, we identified that isolated iron sites were active for N2O activation to generate adsorbed O* species, which readily reacted with CO following the Eley–Rideal (E-R) mechanism. In contrast, Fe2O3 particles exhibited a different reaction pathway, directly reacting with CO to generate oxygen vacancies (Ov), which could efficiently dissociate N2O following the Mars-van Krevelen (MvK) mechanism. Moreover, the transformation of iron oxide clusters into undercoordinated FeOx species by CO was also revealed through various techniques, such as CO-temperature-programmed reduction (TPR), and ab initio molecular dynamics (AIMD) simulations. Our study provides deeper insights into the roles of different iron species in N2O-SCR by CO, and is anticipated to facilitate the understanding of multicomponent catalysis and the design of efficient iron-containing catalysts for practical applications.

研究领域: 催化化学 · 环境科学 · 材料科学
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Journal of Cleaner Production · 2019 · IF 6.395

An easily applicable and recyclable Fenton-like catalyst produced without wastewater emission and its performance evaluation

Lu Liu,Shiquan Liu,Shivani Bhardwaj Mishra,Liping Sheng

A thin disc-shaped Fenton-like catalyst sized 28.59*1.39 mm in diameter and thickness was produced by ball milling a hemi-dried silica xerogel with iron (III) acetylacetonate, followed by mold pressing and calcination. The developed compact catalyst facilitated its application and recovery. The whole fabrication process was free of wastewater emission. Plasticizers or binders indispensable for shaping commercial powders into compact green bodies were not necessary in the present method. The bulky catalyst was mesoporous and had a large surface area of 580 m 2 /g, providing access to the activation of H 2 O 2 by the active iron sites inside the sample. It removed 100% of methylene blue (MB) in solution with a total TOC reduction by 92.13% mainly via the Fenton degradation. No washing, chemical elution of the adsorbed dye before the next application was applied. After five cycles, ca. 93% of the removal efficiency was maintained. The TOC reduction increased from the 1st to 3rd cycle and ca.88% of the initial capacity was kept after the 5th cycle, while the iron leaching was only 0.021% of the applied catalyst. The excellent performance of the bulky catalyst was due to its large surface area, uniformly distributed and chemically bonded iron species. The present work provides a scalable and green way to produce Fenton-like catalysts for environmental application.

CAS / MDL: 109-73-9 14024-18-1
研究领域: 环境科学 · 材料科学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Feasibility of reduced iron species for promoting Li and Co recovery from spent LiCoO2 batteries using a mixed-culture bioleaching process

Xiaojian Liao,Maoyou Ye,Jialin Liang,Zhijie Guan,Shoupeng Li,Yanghong Deng,Qiaowei Gan,Zihang Liu,Xiaodi Fang,Shuiyu Sun

The recovery of metals from spent LiCoO 2 batteries (SLBs) is essential to avoid resource wastage and the production of hazardous waste . However, the major challenge in regard to recovering metals from SLBs using traditional bioleaching is the low Co yield. To overcome this issue, a mixed culture of Acidithiobacillus caldus and Sulfobacillus thermosulfidooxidans was designed for use in SLBs leaching in this study. With the assistance of Fe 2+ as a reductant, 99% of Co and 100% of Li were leached using the above mixed-culture bioleaching (MCB) process, thus solving the problem of low metal leaching efficiency from SLBs. Analysis of the underlying mechanism revealed that the effective extraction of metals from SLBs by the Fe 2+ -MCB process relied on Fe 2+ -releasing electrons to reduce refractory Co(III) to Co(II) that can be easily bioleached. Finally, the hazardous SLBs was transformed into a non-toxic material after treatment utilizing the Fe 2+ -MCB process. However, effective SLBs leaching was not achieved by the addition of Fe 0 to the MCB system. Only 25% Co and 31% Li yields were obtained, as the addition of Fe 0 caused acid consumption and bacterial apoptosis. Overall, this study revealed that reductants that cause acid consumption and harm bacteria should be ruled out for use in reductant-assisted bioleaching processes for extracting metals from SLBs.

CAS / MDL: 7782-63-0 7439-89-6
研究领域: 环境科学 · 微生物学
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CARBON · 2014 · IF 6.16

Hierarchically porous N-doped carbon nanoflakes: Large-scale facile synthesis and application as an oxygen reduction reaction electrocatalyst with high activity

Rui Ning,Chenjiao Ge,Qian Liu,Jingqi Tian,Abdullah M. Asiri,Khalid A. Alamry,Chang Ming Li,Xuping Sun

Hierarchically porous N-doped carbon nanoflakes (HPNCNFs) were facilely synthesized on a large scale via pyrolysis of 1,8-diaminonaphthalene (DAN)/FeCl 3 ·6H 2 O mixture under Ar followed by acid leaching. Both pyrolysis temperature and the amount of Fe species have strong influence on catalyst activity. It suggests that the presence of large excess Fe species not only is key to nanoflake formation but also serves as a mesopore-forming agent. The HPNCNF-900 catalyst, obtained at 900   °C with a mass ratio 1:5 of DAN to FeCl 3 ·6H 2 O, was found to exhibit superhigh oxygen reduction reaction activity and excellent durability in alkaline media outperforming the state-of-the-art Pt/C catalyst at a moderate loading.

CAS / MDL: 771-97-1
研究领域: 材料科学 · 电化学
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JOURNAL OF CATALYSIS · 2021 · IF 7.92

Single-Atom Fe-N4 sites promote the triplet-energy transfer process of g-C3N4 for the photooxidation

Junhui Wang,Shimin Yin,Qinhua Zhang,Fengliang Cao,Yicheng Xing,Qingshan Zhao,Yang Wang,Wengang Xu,Wenting Wu,Mingbo Wu

Polymeric carbon nitride materials show intriguing prospects in numerous light-to-energy conversion applications, but seldom studies focus on their triplet energy transfer, leading to the insufficient lifetime for the photochemical process. Inspired by the porphyrin molecular photocatalyst, single-atom sites (Fe-N 4 ) as triplet sensitizing sites were fabricated in g-C 3 N 4 for the preparation of Fe-g-C 3 N 4 , which processes a long-lived triplet emissive state (τ PH  = 4.93 μs). But under realistic condition for the large-scale production of catalyst, single atoms are inevitable to sinter, resulting in the formation of other metal species. Therefore, the photooxidation of 1,5-dihydroxynaphthalene (1,5-DHN) and the photocatalytic E-Z Isomerization of stilbene were selected as the model reactions to evaluate the influence of various Fe species on the triplet energy transfer. It was found that Fe-N 4 sites promote the triplet energy transfer process, while Fe nanoclusters (Fe 0 ) promote the electron transfer and inhibit triplet energy transfer. This finding provides guidance for the rational design of photocatalysts to efficiently improve triplet energy transfer process and its application.

CAS / MDL: 461-58-5 7705-08-0
研究领域: 材料科学 · 光化学
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