ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Zhiwen Xu,Lanlu Lu,Weiwei Chen,Fei Yang,Guimei Liu,Yan Sun,Xiaoyi Qiu,M. Danny Gu,Ping Gao,Dong Su,Minhua Shao
Although zinc-air batteries (ZABs) have made great progress in recent years, there still a great challenge to develop low-cost bifunctional electrocatalysts with high catalytic activity and stability. Herein, we report a bifunctional oxygen electrocatalyst consisting of ZIF-derived carbon-anchored Fe/Fe 3 C nanoparticles and Fe single atoms, which are crosslinked by carbon nanotubes (denoted as CNT@Fe/Fe 3 C||FeNC). Benefiting from the synergetic effect of Fe/Fe 3 C nanoparticles, Fe-N 4 active sites, and the 3D interpenetrating network structure, CNT@Fe/Fe 3 C||FeNC shows excellent bifunctional catalytic activities with a low ΔE of 0.671 V. Furthermore, the assembled rechargeable ZAB demonstrates a high peak power density of 187 mW cm –2 and shows excellent cycling stability up to 600 h This work provides new ideas for constructing non-precious metal bifunctional catalysts for practical applications in ZABs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jingjing Tang,Hongchao Li,Xuan Zhang,Jieshu Qian,Bingcai Pan
Fe-based metal–organic frameworks (MOFs) have garnered significant attention as catalysts for heterogeneous Fenton reactions, while the limited efficiency of the Fe(III)/Fe(II) redox cycle hinders their widespread use in wastewater treatment. Herein, we successfully incorporated carbon nanotubes (CNTs) into MIL-101(Fe) to modulate the coordination environment of Fe for achieving better catalytic activity. The MIL-101(Fe)/CNTs/H 2 O 2 system shows outstanding performance in degrading various pollutants, with the catalytic activity of the MIL-101(Fe)/CNTs composites (98.8%) significantly surpassing that of MIL-101(Fe) alone (26.4%) or CNTs alone (3.5%). Multiple experimental findings suggest that this synergistic effect is primarily attributed to the C-O-Fe bridge bonds resulting from the interaction of surface carboxyl groups on CNTs with Fe in MIL-101(Fe). This unique coordination structure accelerates the redox cycle of Fe(III)/Fe(II), thereby promoting the generation of hydroxyl radicals (HO • ). Furthermore, the MIL-101(Fe)/CNTs composites demonstrate excellent reusability and stability, maintaining effectiveness over a wide pH range from 3.0 to 6.5. This study provides new insights into regulating the microstructure of Fe-based MOFs to enhance their Fenton catalytic activity.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Yujia Han,Teng Zong,Yuehan Wang,Ming Tian,Chaojie Wang,Nanxin Wang,Xiaodong Wang
Chemical looping H 2 O splitting is considered as a promising approach to produce hydrogen thanks to its lower energy consumption and carbon footprint compared with traditional steam reforming. Fe-based oxides have been paid much attention but suffer from inferior H 2 production rate and stability due to insufficient activation for H 2 O. Herein, it was found that the introduction of Cr into MgFe spinel oxides (MgFe x Cr 2-x O 4 , MFCO) could greatly increase the performance of H 2 O splitting driven by CH 4 reduction with the highest peak H 2 production rate of about 4.65 mmol min −1 g −1 , H 2 productivity of about 2.88 mmol g −1 and good stability during multiple redox cycles for MFCO-46 (the atomic ratio of Fe and Cr of 2:3), which exceeded most of the state-of-the-art Fe-based oxides. This originated from the Cr doping promoting Fe 0 nanoparticles exsolution by activating CH 4 and Fe-O v -Cr species formation which relay catalyzed H 2 O splitting and was favorable for the fast recovery of lattice oxygen converted.
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ACS Omega
·
2024
·
IF 3.7
Junhong Liu,Zhitao Liu,Jing Yang,Bin Xu,Feiyun Chen,Xin Liao
The incorporation of nanomaterials generated from Prussian blue (PB) derivatives has emerged as a promising strategy to significantly improve the properties of energetic materials. In this study, we comprehensively investigated the influence of nanomaterials derived from PB on the thermal decomposition characteristics of energetic materials. To achieve this goal, we prepared nanomaterials using coprecipitation and heat treatment methods with PB derivatives as catalysts. Advanced techniques such as X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Brunauer–Emmett–Teller (BET) analysis for specific surface area and pore size, and X-ray photoelectron spectroscopy were employed to thoroughly characterize these nanomaterials. Differential scanning calorimetry was used to assess the thermal behavior of nitrocellulose (NC), and the relevant kinetic parameters were determined through thermal decomposition kinetics calculations and analysis. This work revealed the influence of catalysts on the NC decomposition process and provided comprehensive insights into the effect of integrating nanomaterials derived from PB derivatives on the thermal decomposition performance of NC. The results of this work demonstrated the possibility of using nanomaterials generated from PB derivatives as effective catalysts to enhance the thermal decomposition characteristics of NC, offering interesting opportunities for their application in the field of high-energy materials.
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PubMed
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yuan Qin,Zihao Ou,Chaozhong Guo,Yao Liu,Rong Jin,Chuanlan Xu,Haifeng Chen,Yujun Si,Honglin Li
Regulating the electronic structure by phosphor-doping is a preferred strategy to boost the performance of carbon-based catalysts for oxygen reduction reaction (ORR). Here, a porous Fe, P, N-codoped carbon catalyst (PCF-FeTz-900) is designed by a phytic acid-assisted thermal etching strategy, in which P atoms are first doped into the carbon matrix to form a stable P C bond, and then FeN 4 sites are produced from Fe-2,4,6-Tris(2-pyridyl)-s-triazine complex (Fe-TPTz). Theoretical calculations suggest that the electrons are transferred from the doped P atom to the neighboring FeN 4 sites, which facilitates the ORR at the Fe sites by reducing the energy barrier and the adsorption energy of intermediates. Additionally, the P-doped FeN 4 (FeN 4 P) structure manifests a lower free energy difference than that of FeN 4 and the d -band center of Fe is also lowered, which further ensures its higher ORR catalytic ability. As a result, the PCF-FeTz-900 catalyst exhibits superior ORR activity and stability in alkaline electrolyte, and the assembled primary zinc-air battery shows greater performances compared to the commercial Pt/C catalyst. This work can provide an effective pathway for modulating the performance of doped-carbon materials in energy conversion devices.
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CHEMICAL GEOLOGY
·
2024
·
IF 3.6
Kuan Cheng,Yunlu Yin,Ying Wang,Guoyong Huang,Dandan Pan,Milan Wang,Xuxin Song,Tongxu Liu,Xiaomin Li
Microbial Fe(II) oxidation is mainly mediated by the outer-membrane proteins that contain c -type cytochromes ( c- Cyts), and the widespread Fe(II)-oxidizing bacteria are usually subjected to fluctuations between oxic and anoxic conditions. However, it remains unclear how oxygen affects the redox dynamics of c- Cyts by Fe(II), particularly in the presence of organic ligands that are widely distributed in the environment. Here, the reduction of a model heme-containing c- Cyts by Fe(II) was investigated in the absence and presence of organic ligands (i.e., citrate and acetate) at pH 5.5 under anoxic and oxic conditions . The kinetic results showed that c- Cyts reduction was enhanced by citrate and acetate under anoxic conditions, and the enhancement by citrate was more pronounced than that by acetate. The speciation calculation and cyclic voltammetry results suggested that the proportions of Fe(II)-Citrate complexes were much higher than those of Fe(II)-Acetate complex, but the addition of acetate and citrate caused minor changes in redox potential of Fe(II)/Fe(III) species. Further analysis using quantum chemical computation demonstrated that the formation of Fe(II)-Heme complexes via lateral binding to the carboxyl group of c- Cyts was more stable than those via replacing the S-linked axial ligand of heme, with the recombination energy with Heme ranking as Fe(II)-Citrate < Fe(II)-Acetate < Fe(II). Therefore, the stronger complexation of Fe(II)-Citrate and its lower recombination energy with c- Cyts drive the enhanced c- Cyts reduction under anoxic conditions. By contrast, the c- Cyts reduction by Fe(II) and Fe(II)-ligand was inhibited under oxic conditions. The electron spin resonance characterization indicated that both O 2 − • and OH• radicals were produced in the system of c- Cyts with Fe(II) or Fe(II)-ligand under oxic conditions and the signals were higher with Fe(II)-ligand than those with Fe(II). These reactive oxygen species were proposed to enable a re-oxidation of the c- Cyts that was reduced by Fe(II) or Fe(II)-ligand, causing an inhibitory effect on the observed c- Cyts reduction and forming more reactive oxygen species . Our findings shed light on the important roles of Fe(II)-ligand-heme complexation and reactive oxygen species in the interaction between Fe(II) and c- Cyts, which deepen the understanding of microbial/enzymatic Fe(II) oxidation under oxic conditions at the molecular level.
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JOURNAL OF GEOPHYSICAL RESEARCH-PLANETS
·
2020
·Vol. 125
·期 12
·e2020JE006590
·
IF 3.717
Peixin Du,Peng Yuan,Jiacheng Liu,Yixuan Yang,Hongling Bu,Shun Wang,Junming Zhou,Hongzhe Song,Dong Liu,Joseph R. Michalski,Chengshuai Liu
Allophane, a common component on Earth and a probable constituent of the amorphous component on Mars, is closely associated with Fe in the form of structural Fe and/or iron (oxyhydr)oxide coatings. However, until now, the formation and evolution of allophane as products of environmental Fe concentrations have rarely been studied. We investigated allophane precipitation from gels with different Fe/(Fe + Al) molar ratios ( n , 0 ≤ n ≤ 1.0). X-ray diffraction patterns and Fourier transform infrared spectra of the products showed that allophane was nearly the only product at n ≤ 0.2 and that the crystallinity of Fe-rich allophane decreased with increasing n . Combined with the results of transmission electron microscopy and Mössbauer spectroscopy, Fe was found to be mainly incorporated into the gibbsite-like sheet of allophane, forming clusters; the highest Fe-for-Al substitution content was roughly estimated to be 20 mol.%. As n increased further, the formation of allophane was increasingly suppressed, and the Fe phases began to separate from the Al-Si phases, resulting in mixtures of incipient allophane and incipient akaganeite and finally akaganeite. The near-infrared spectroscopic data (1.2–2.6 μ m) of the products showed incapability in identifying poorly ordered minerals in Al-Si-Fe systems, while the features in the range of 0.4–1.2 μ m were powerful for studying iron occurrence in the products. These findings not only offer insights into the formation, evolution and geological role of allophane in Al-Si-Fe systems on Earth but also help constrain the paleoenvironment of locations where allophane and akaganeite co-occur on Mars. Key Points Environmental Fe concentrations control the formation and evolution of allophane in Al-Si-Fe systems Near-infrared spectra (1.2–2.6 μ m) show incapability in identifying short-range ordered minerals in Al-Si-Fe systems Co-occurrence of allophane and akaganeite would constrain the local palaeoenvironment on Mars
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Journal of Physical Chemistry Letters
·
2024
·
IF 4.8
Yanchang Wang,Yao Xiao,Jiangnan Huang,Chunxiao Zhang,Kentaro Yamamoto,Yoshiharu Uchimoto,Weifeng Wei,Hongshuai Hou,Datong Zhang,Xiaobo Ji
For cathode materials of sodium-ion batteries, O3-type Ni/Fe/Mn-based (Na-NFM) layered oxides have garnered extensive attention because of high economic viability, environmental friendliness, and the potential for high energy density. Among them, Fe-rich compositions exhibit higher initial charge capacity and lower bill-of-material costs, while they fade rapidly and exhibit low initial coulombic efficiency, hindering their commercialization prospects. In this work, we investigate the failure of Fe-rich Na-NFM materials through X-ray absorption spectroscopy methods. The results reveal a combined failure mechanism that encompasses not only the conventional theory of Fe migration but also an abnormal Ni-redox deterioration, which has not yet been reported. More factors related to the failure of Fe-rich Na-NFM layered oxides are discussed in detail. These findings are expected to inspire targeted research efforts toward Fe-rich Na-NFM materials, thereby accelerating the practical application of sodium-ion batteries.
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Heliyon
·
2023
·
IF 4
T. Widjaja,N. Hendrianie,S. Nurkhamidah,A. Altway,Bayu Yusuf,Fakhrizal F,Aisyah Alifatul Zahidah Rohma,Atha Pahlevi
LASC catalyst synthesis process was carried out using iron metal (Fe) and its characterization properties were tested. There are five stages carried out, namely, the manufacture of the LASC Fe(DS)3 catalyst, lactic acid dehydration, polycondensation of lactic acid into l -lactic acid oligomers (OLLA), depolymerization of oligomers into l -lactide, and the ROP process to convert l -lactide into Polymers. l -lactic acid (PLLA). The analysis used is as follows, Karl-Fisher; Spectroscopy Fourier Transform Infrared (FTIR); and Nuclear Magnetic Resonance (HNMR); Gel Permeation Chromatography (GPC); Thermogravimetry Gravity Analysis (TGA) and X-Ray Diffraction (XRD). Based on the experimental results, the catalyst Fe(DS) 3 has a crystallinity value of 24% which indicates an amorphous nature and is easy to react. The value of the thermal stability of the catalyst is at 180 °C where the catalyst is able to process up to a temperature of 180 ° C. Each step of the ROP is validated by FTIR analysis which shows that the components of the group are in accordance with the expected product. The comparison of the crystallinity values of PLA produced with FeCl 3 and Fe(DS) 3 were 37.5 and 49%, respectively. Melting temperature (Tm) values are 111 and 107 ° C, respectively, Td values are 327 and 352 °C, and the resulting molecular weights are 23,720 and 20,232 g/mol. Based on the results obtained, it can be seen that the use of a LASC catalyst in the form of Fe(DS) 3 is more effective than without using a LASC catalyst.
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PubMed
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ACS Applied Electronic Materials
·
2026
·Vol. 8
·期 15
·6545-6553
·
IF 4.7
Liu Qianzuo,Sun Sifan,Li Jiawei,Yang Haoran,Xiang Xinyue,Hao Ying,Yan Xuehua,Zhang Ting,Li Tie
Hydrogen peroxide (H 2 O 2 ), a key reactive oxygen species in physiological and pathological processes, demands highly sensitive detection for biological and biomedical research, yet developing electrocatalytic materials with high sensitivity, low detection limit, and excellent stability remains a challenge. Herein, a Fe−C@Fe/Ce−C bilayer heterojunction composite was fabricated for H 2 O 2 detection. Benefiting from its unique heterojunction architecture and synergistic Fe/Ce/carbon interactions, the as-prepared nanocomposite exhibits the exceptional H 2 O 2 sensing performance, with a wide linear range of 0.5−6000 µM, a high sensitivity of 490.5 μA·mM −1 ·cm −2 , a low detection limit of 0.12 µM, excellent anti-interference selectivity against common biological interferents, and outstanding long-term stability with no obvious performance variation after 11 days of continuous testing. The robust built-in electric field arising from the heterojunction facilitates interfacial charge transfer and accelerates H 2 O 2 activation, boosting sensing behavior. Furthermore, the flexible electrochemical sensor was fabricated via the screen-printing technology, which enables reliable real-time monitoring of intracellular H 2 O 2 released from HeLa cells, showing great potential for biological sensing. This work provides a promising design strategy for high-performance flexible electrochemical sensors and deepens the understanding of heterojunction and built-in electric field roles in electrocatalytic sensing systems.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122408
·
IF 7.5
Shan Huang,Jiangxue Luo,Tianren Zhan,Yubo Wu,Jiankun Li,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Iron-based catalysts have been widely used to activate peroxymonosulfate (PMS) for the treatment of carbamazepine (CBZ) wastewater. However, the development of efficient and stable pyrite (FeS 2 )-based catalysts to mitigate the consumption of Fe 3 + /Fe 2+ and S 2 2– is still challenging. Herein, FeS 2 /nitrogen-doped carbon (FeS 2 /NC) composite was synthesized using hydrothermal combined with pyrolytic strategy, wherein FeS 2 and NC connected by Fe−N x and Fe−C x bonds. In the photo-PMS system, FeS 2 /NC achieved a removal rate of 98.2 % for CBZ within 6 min, and the total organic carbon (TOC) removal was 83.4 %, which exceeded FeS 2 and most of the results reported in the previous literature. The electron paramagnetic resonance results and quenching experiments confirmed that 1 O 2 played a critical role in the FeS 2 /NC + PMS + visible light system, while h + , SO 4 • − , and •O 2 − were secondary. The excellent performance stemmed from that the Fe−N x and Fe−C x bonds between FeS 2 and NC enhanced the photogenerated electron transport efficiency, resulting in efficiently circulating Fe 3+ to Fe 2+ and minimizing the S 2 2– consumption. Meanwhile, the electron-deficient graphitic-N could facilitate the 1 O 2 generation. Moreover, FeS 2 /NC exhibited good stability and satisfactory universality, providing the potential for actual wastewater treatment. This work offers a novel strategy for enhancing the Fe 3+ /Fe 2+ cycle and reducing the S 2 2– consumption of FeS 2 -based catalyst for the effective treatment of CBZ wastewater.
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RSC Advances
·
2026
·Vol. 16
·期 18
·16505-16511
·
IF 6.1
Cong Gao,Houfen Li,Jize Liu,Wenchao Yang,Hong Chen,Jianbo Han
The heterogeneous Fenton-like reaction is a promissing technology for removing organic pollutants in water. The reduction of Fe(III) to Fe(II), as the rate-limiting step for generating ˙OH, is crucial in heterogeneous Fenton-like reactions and may be improved using organic pollutants with lower redox potential than that of Fe(III)/Fe(II). In this work, the rapid reduction of Fe(III) to Fe(II) on the MIL-100-Fe catalyst was achieved by degrading methylene blue (MB, E0 = 0.01 V), which has the desired lower redox potential than that of MIL-100-Fe(III)/Fe(II) (E0 = 0.76 V). By contrast, organic pollutants with higher redox potentials than that of MIL-100-Fe, such as phenol (E0 = 0.97 V) and p-nitrophenol (E0 = 1.23 V), were incapable of reducing Fe(III) to Fe(II). As a result, the degradation rate constant of MB was one order of magnitude higher than those of phenol and p-nitrophenol. Notably, MB could also promote the reduction of Fe(III) to Fe(II) in the presence of phenol or p-nitrophenol; thus, the degradation rate constants of phenol and p-nitrophenol were significantly enhanced by 50 and 30 times, respectively. The results revealed that organic pollutants with lower redox potential than that of Fe(III)/Fe(II) could facilitate the reduction of Fe(III) to Fe(II), which is beneficial for producing more ˙OH, thus improving the heterogeneous Fenton-like catalytic performance.
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