Journal of Water Process Engineering
·
2022
·
IF 7.34
Junjie Su,Han Hao,Jingran Li,Zhilin Yang,Qi Yang
Nanometer zero-valent iron (nZVI), Fe 2+ and H 2 were potential electron donors for CT removal by nZVI. However, the action of these electron donors in CT reduction was often ambiguous. In this study, the actual catalytic activity of Ni 4 /Fe@Fe 3 O 4 under common ions and humic acid (HA) was investigated. The results showed that Na + and K + had no effect on CT removal, Cl ‐ , SO 4 2 ‐ and low concentration of Mg 2+ was beneficial to CT removal, while NO 3 ‐ , HCO 3 ‐ , Ca 2+ and HA exhibited the negative effects. According to the analysis results of gas chromatography (GC) and ion chromatography (IC), a possible dechlorination pathway of CT was proposed. Furthermore, the action mechanism of nZVI, Ni 0 and magnetite (Fe 3 O 4 ) on CT removal were explored. Among the three possible nZVI reducing mechanism, the use of H 2 by Ni 0 for the hydrodechlorination was dominant, while the direct reduction of nZVI was secondary. Fe 2+ , the product of nZVI corrosion, contributed little to CT degradation and required longer reaction time. Ni 0 could not only utilize H 2 but also form galvanic cells with nZVI to accelerate CT dechlorination. In addition, the support Fe 3 O 4 significantly improved the dispersion of Ni/Fe nanoparticles and its corrosion product Fe 2+ also promoted the CT removal. These findings were significant for comprehending the mechanisms of bimetallic nanocomposites in reducing CT, and might guide to the development of nZVI based technology for repairing polluted water or soil with organochlorine pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2020
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IF 10.652
Yong Sun,Muhammad Danish,Meesam Ali,Ali Shan,Ming Li,Yanchen Lyu,Zhaofu Qiu,Qian Sui,Xueke Zang,Shuguang Lyu
The performance of trichloroethene (TCE) degradation was significantly improved with the addition of FeS in nanoscale calcium peroxide (nCP) environment and the enhancement of HO generation in nCP/Fe(II)/FeS system was confirmed by comparison with nCP/Fe(II) and nCP/FeS systems. The role of FeS in nCP/Fe(II)/FeS system demonstrated that the majority of reactive oxygen radicals (ROSs) was generated on the catalyst surface due to the heterogeneous reaction through FeS activated nCP in one hand, and the reductive FeS could promote TCE degradation by regenerating Fe(II) from Fe(III) in the other hand. The probe as well as scavenger test results suggested that the major ROSs was HO rather than O 2 − . Over 91.5% TCE could be degraded at the molar ratio of 2/2/4/1 of nCP/Fe(II)/FeS/TCE, in which more than 95.5% TCE was dechlorinated. The effect of surfactants on TCE degradation was evaluated. In contrast, further investigation found that BTEX removal was inhibited with the addition of FeS. In conclusion, this study revealed the well function and fundamental synergistic mechanism of FeS. Moreover, the degradation of TCE in actual groundwater confirmed that nCP/Fe(II)/FeS technique has a great advantage and potential in TCE contaminated groundwater remediation in ISCO practice.
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RSC Advances
·
2019
·Vol. 9
·期 72
·42236-42244
·
IF 3.049
Limeng Yang,Zhigang Shao
The development of low-cost, efficient and stable electrocatalysts for the oxygen reduction reaction (ORR) is desirable but remains a great challenge. We report a convenient and efficient synthesis approach of highly dispersed Fe–Nx catalysts for ORR. Typically, Fe–Zn-ZIF (zeolitic imidazolate frameworks) nanocrystals cast as precursor and graphene as supports, highly dispersed Fe–Nx species were fabricated with PVP (polyvinyl pyrrolidone) as surfactant via pyrolysis. With the help of graphene and surfactant, the agglomeration of iron particles has been avoided during pyrolysis, and the size and morphology of ZIF particles intercalating into the graphene layers can be regulated precisely as well. The amount of Fe–Nx active sites in C-rGO-ZIF catalyst arrived 4.29%, which is obviously higher than most monodispersed non-precious metal catalysts reported. The obtained C-rGO-ZIF catalyst exhibits a high onset potential of 0.89 V and a half-wave potential of 0.77 V, which is only 30 mV away from Pt/C in acidic media. The active sites of the catalyst was characterized and found to be the highly dispersed Fe–Nx species, large and accessible specific surface area of graphene and abundant active nitrogen atoms. When the C-rGO-ZIF catalyst was applied in the cathode of fuel cell, the power density can reach up to 301 mW cm−2, which highlights a practical application potential on small power supplies.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Zigui Luo,Xi’an Fan,Wentao Hu,Fan Luo,Jian Wang,Zhaoyang Wu,Xin Liu,Guangqiang Li,Yawei Li
In this work, Fe–Si/Fe 2 SiO 4 soft magnetic composites (SMCs) are prepared successfully via sintering Fe-6.5 wt%Si/α-Fe 2 O 3 core-shell composite powders obtained by ball milling. The transformation mechanism from Fe-6.5 wt%Si/α-Fe 2 O 3 to Fe–Si/Fe 2 SiO 4 is revealed in detail. The effect of α-Fe 2 O 3 coating content on microstructure and magnetic properties for the Fe–Si/Fe 2 SiO 4 SMCs is also investigated. During the high temperature sintering process, α-Fe 2 O 3 coating will in situ react with diffused Si from Fe–Si alloy cores, and result in the generation of Fe 2 SiO 4 insulating layer and Fe atoms. When the α-Fe 2 O 3 coating content increases from 0.0 wt% to 7.5 wt%, the insulating layer becomes thicker. Nevertheless, with further increasing the α-Fe 2 O 3 coating content from 7.5 wt% to 12.5 wt%, the generation of excessive Fe breaks the continuity of the insulation layer. As a result, the saturation magnetization decreases gradually, while the coercivity exhibits an opposite trend. The core loss decreases firstly and then increases. Therefore, the Fe–Si/Fe 2 SiO 4 SMCs coated with 7.5 wt% α-Fe 2 O 3 exhibit superior comprehensive performance such as very low core loss (39.6 mW/cm 3 at 50 kHz), very high saturation magnetization (191.4 emu/g) and stable permeability (44) from 50 Hz to 200 kHz.
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WATER RESEARCH
·
2023
·
IF 12.8
Bin Liu,Yin Jun,Changrong Zhao,Chu Zhou,Tingting Zhu,Senlin Shao
Ultrafiltration (UF) is a technology commonly used to treat secondary effluents in wastewater reuse; however, it faces two main challenges: 1) membrane fouling and 2) inadequate nitrogen (N), phosphorus (P), and organic micropollutants (OMPs) removal. To address these two issues, in this study, we applied peracetic acid (PAA), Fe(VI)/PAA, and Fe(II)/PAA as UF pretreatments. The results showed that the most effective pretreatment was Fe(II)/200 μM PAA, which reduced the total fouling resistance by 90.2%. In comparison, the reduction was only 29.7% with 200 μM PAA alone and 64.3% with Fe(VI)/200 μM PAA. Fe(II)/200 μM PAA could effectively remove fluorescent components and hydrophobic organics in effluent organic matter (EfOM), and enhance the repulsive force between foulants and membrane (according to XDLVO analysis), and consequently, mitigate pore blocking and delay cake layer formation. Regarding pollutant removal, Fe(II)/200 μM PAA effectively degraded OMPs (>85%) and improved P removal by 58.2% via in-situ Fe(Ⅲ) co-precipitation. The quencher and probe experiments indicated that Fe IV O 2+ , •OH, and CH 3 C(O)OO•/CH 3 C(O)O• all played important roles in micropollutant degradation with Fe(II)/PAA. Interestingly, PAA oxidation produced highly biodegradable products such as acetic acid, which significantly elevated the BOD 5 level and increased the BOD 5 /total nitrogen (BOD 5 /TN) ratio from 0.8 to 8.6, benefiting N removal with subsequent denitrification. Overall, the Fe(II)/PAA process exhibits great potential as a UF pretreatment to control membrane fouling and improve water quality during secondary effluent treatment.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 8
·2066-2076
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IF 7.3
Jiahui Zhou,Xuesong Li,Qiuying Yi,Zhiwei Wang
Heterogeneous Fenton-like processes based on Fe-based catalysts are effective technology to degrade emerging organic pollutants in water and wastewater such as tetracycline (TC). However, the kinetically limited redox cycling between Fe2+ and Fe3+ is still a persistent challenge for their widespread application. To address this issue, we designed a novel Fe-based catalyst by coating reduced iron powder (RIP) with ferroferric oxide nanoparticles (FONP@RIP) using a simple chemical co-precipitation method. The reduced iron could rapidly reduce Fe(III) to Fe(II) and accelerate the cycle of Fe(II)/Fe(III) in the heterogeneous Fenton-like system. Benefiting from the accelerated cycle of Fe(II)/Fe(III), TC could be efficiently degraded in the FONP@RIP/H2O2 system over a wide pH range of 3–6, with a removal efficiency of 94.5% within 60 min (TC0 = 150 ppm). The predominant reactive oxygen species were identified as ˙OH and HO2˙. Based on the identified intermediates, the possible pathway of TC degradation was deduced and the toxicity of pollutants could also be significantly reduced during the degradation process. Moreover, FONP@RIP exhibited stable catalytic performance during multiple cyclic tests with only a marginal loss of catalytic components. This study presents a new catalyst design strategy for heterogeneous Fenton-like processes, which provides a promising way for the degradation of residual antibiotics in water and wastewater.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 19
·11792-11801
·
IF 10.733
Xiang Ao,Wei Zhang,Zhishan Li,Lin Lv,Yunjun Ruan,Hong-Hui Wu,Wei-Hung Chiang,Chundong Wang,Meilin Liu,Xiao Cheng Zeng
The scarcity and weak durability of precious metal catalysts are among the biggest obstacles to achieving cost-effective electrocatalysts in fuel cells and metal–air batteries. Hence, it is imperative to develop low-cost non-precious metal catalysts with comparable oxygen reduction reaction (ORR) activity to precious metal catalysts. Herein, we report a highly effective strategy for the facile synthesis of Fe/N-functionalized 3D porous carbon networks. A major advantage of the newly designed catalyst is that ultrafine Fe4N nanoparticles are grown and uniformly mounted on the carbon framework upon pyrolysis treatment at 800 °C, and co-exist with numerous in situ formed Fe–N4 moieties in the carbon matrix, being evidenced by using X-ray absorption and photoelectron spectroscopy. The new electrocatalysts exhibit high ORR activity, comparable/superior to that of the state-of-the-art Fe/N–carbon based catalysts reported to date. Specifically, the catalysts show a half-wave potential of 0.890 V (vs. RHE) and a limited current density of 6.18 mA cm−2. By resorting to experimental measurements and density-functional theory (DFT) calculations, the synergistic effects between Fe–N4 moieties and the Fe4N support are identified for the first time, which play a key role in boosting the catalytic performance of the Fe/N-functionalized porous carbon networks.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Xuechao Cai,Xiaoran Deng,Zhongxi Xie,Yanshu Shi,Maolin Pang,Jun Lin
Nanoscale metal-organic frameworks (NMOFs) are promising porous nanomaterials for various applications, such as catalysis, biomedical imaging, drug delivery and cancer therapy etc . Especially when it comes to medical applications, downsizing of MOFs into nanoscale is the crucial requirement. Herein, liquid-solid-solution (LSS) method was used to prepare nano Fe- soc -MOF for the first time, and then we integrated the as-synthesized nanoscale Fe- soc -MOF with polypyrrole (PPy) to construct a multifunctional theranostic platform. The novel Fe- soc -MOF@PPy core-shell nanohybrids can be triggered by the 808 nm laser irradiation to produce photothermal effect for cancer therapy. The photothermal therapy (PTT) was performed both in vitro and in vivo . This work demonstrates the great potential of the MOF nanocomposites for cancer diagnosis and treatment.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Maolin Wang,Mi Deng,Gang Zhao,Yanchun Fan,Tianwen Liu,Ying Huang,Lan Peng,Haoyang Fu,Shengqiong Fang
The remediation of organic-contaminated water is a critical environmental challenge, and iron-based persulfate (PS) activation processes have emerged as a promising solution. However, the introduction of reductive sulfur species, while accelerating the Fe(III)/Fe(II) redox cycle, may also quench reactive species, potentially compromising the efficiency of Fenton-like systems. Here we systematically investigate the trade-off between accelerated Fe(III)/Fe(II) cycling and quenching effects in the zerovalent iron/PS (ZVI/PS) system using thiosulfate (TSF) as an activator. Our results show that low-level TSF (0.03–1.00 mmol/L) effectively facilitated the removal of naphthalene (Nap) and atrazine (ATZ), respectively. This enhancement is attributed to accelerated ZVI dissolution and FeS x formation, which promote the Fe(III)/Fe(II) cycle, with Fe(IV) was identified as the primary active species. However, high-level TSF (>1.0 mmol/L) drastically reduced Nap removal due to PS consumption and active species elimination. The optimal TSF dosage of 0.20 mmol/L (TSF/PS molar ratio of 1:10) demonstrated robust organic pollutant degradation, achieving a 22-fold increase in the rate constant ( k obs ) for Nap removal and 0.47–7.5-fold increases for ATZ removal. These findings highlight the potential of the TSF-ZVI/PS system as a versatile and efficient solution for degrading a wide range of organic pollutants, including PAHs and herbicides, in water treatment applications.
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Advanced Energy Materials
·
2025
·Vol. 15
·期 36
·e02595
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IF 26
Xiang Ji,Yi Li,Yanlong Wang,Jian Jiang,Maowen Xu,Jianhui Zhu
Rechargeable Fe-ion batteries with overwhelming cost/environmental benign superiorities hold great promise in large-scale charge-storage applications. However, there is still a lack of competitive cathodes with prominent capacity and long-term cyclability. To overcome these constraints, a unique Fe 2+ /NH 4 + co-insertion strategy is proposed, enabling both doubled reversible capacity and cyclic life of Berlin green (FeHCF) cathodes. The Fe 2+ insertion proves to induce FeHCF lattice contractions, alter ligand environment/activation energies of low-spin Fe III, and hence boost the redox conversion depth, while NH 4 + co-insertions help to elevate the cathode capacities by utilizing Fe 2+ -unoccupied reaction sites. Besides, they generate hydrogen bonds between inserted NH 4 + ions and N atoms in FeHCF, capable of vastly strengthening the cathode's cyclic durability. Cathodes in such collaborative dual-cation electrolytes exhibit a remarkable capacity of 162 mAh g −1 (4 A g −1 ) and far prolonged operation lifespan (over 1000 cycles) when compared to single-cation cases. The assembled full cells demonstrate impressive energy densities up to 70.4 Wh kg −1 , and far superior capacity retention of 88% after all the cycling. This work may offer a simple/feasible, and effective route to render high-capacity and long-lasting cathodes for future/practical Fe-ion battery systems.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Kangpeng Jin,Haonan Nie,Fengxian Gao,Jiang-Jiang Ma,Mingfang Shu,Xi Yan,Zhen-Hua Ge,Xiao Gao,Weiyun Zhao,Ming Liu,Yuan Yu,Jie Ma,Biao Xu,Liangwei Fu
Mg 3 (Sb,Bi) 2 alloys offer exceptional near-room temperature thermoelectric (TE) performance comparable to Bi 2 Te 3 . However, the low carrier mobility due to Mg vacancies and relatively high lattice thermal conductivity adversely affect overall TE performance. Herein, carrier mobility and thermal conductivity of Mg 3 (Sb,Bi) 2 are decoupled by modulating both the phase interface and grain boundaries through incorporating different sizes of iron (Fe). Ferromagnetic micrometer-sized Fe particles enhance the figure of merit ( ZT ) more than superparamagnetic nano-sized counterparts. Magnetic moments of Fe induce the charge density overlap near phase boundaries and ≈1 nm Fe interfacial layer lowers grain-boundary barriers, leading to sharply increased carrier mobility. Moreover, the additional magnon-phonon scattering reduces lattice thermal conductivity by over 40%. Consequently, Fe/Mg 3 (Sb,Bi) 2 composite achieves a high average ZT of 1.4 over room temperature to 573 K. The fabricated Mg 3 (Sb,Bi) 2 -CdSb module demonstrates a high conversion efficiency of 8.4% under a 275 K temperature gradient, among the best for Mg 3 (Sb,Bi) 2 -based modules. This work uncovers the role of thermo-electro-magnetic interactions in bolstering TE performance and inspires the development of low-cost, high-efficiency TE modules for low-grade heat recovery.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Qiang Zhang,Ranxiao Ao,Ruijie Gao,Huaming Yang
Transition metals with 3d unoccupied orbitals have superior catalytic activity, but inherent high spin suppresses their adsorption capability, leading to sluggish polysulfide conversion kinetics for Li–S batteries. Herein, we provide Fe–O–Si bridge bonds to manipulate eg filling and induce a high-to-medium spin transition of Fe3+ sites, which enhances polysulfide adsorption and facilitates sulfur redox reaction kinetics. The resultant cathodes exhibit outstanding performances under high sulfur loading, which can deliver a high battery specific energy of 1061 mA h·g–1 even after 100 cycles in Li–S pouch batteries. This work provides new insights into the kinetic and multi-step conversion mechanism of the sulfur redox reaction process, helping in the understanding and design of spin-dependent catalysts.
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