APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Xiaoqi Zhao,Yingxiao Li,Xue Zhang,Yanfang Gao,Ling Liu
Surface oxygen vacancy increases active site numbers, and multidimensional cross-linked structure improves the exposure of active sites. Thereby, they can enhance the oxygen reduction reaction (ORR) performance of Fe-N-C catalysts effectively. Herein, Fe(NO 3 ) 3 ·9H 2 O and carbon nanotubes (CNTs) were introduced into zeolitic imidazolate framework nano leaves (ZIF-L) to prepare multidimensional cross-linked Fe-N-CNTs with surface oxygen vacancies through co-pyrolysis at the high-temperature. As expected, the synthesized multidimensional cross-linked Fe-N-CNTs-900-0.2 composite rich in oxygen vacancies increased the conduction band potential and improved the reducing capacity. Thus, Fe-N-CNTs-900-0.2 possessed a better ORR electrochemical performance (half-wave potential = 0.892 V vs. RHE) that surpass the Pt/C catalysts. Moreover, the Al-air batteries containing Fe-N-CNTs-900-0.2 displayed a higher maximum power density than those of Pt/C catalysts. The electronic band structure shows that Fe-N-CNTs-900-0.2 rich in oxygen vacancy concentration has higher conduction band potential and effectively improves the activity of ORR catalysts. This work innovatively proposes that the joint work of multidimensional cross-linked structure and oxygen defects is an effective method to enhance the ORR performance and clarifies its internal reaction mechanism, which provides a new idea to design and preparer Fe-N-C catalysts.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 5
·1-10
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IF 5.7
Wei Chunying,Lin Huiqing,Bai Hehe
Five G-/C-rich single-stranded DNA (ssDNA) with different sequences and lengths were templated to prepare the DNA-Cu, DNA-Fe, and bimetallic DNA-Cu/M nanoclusters (NCs). The peroxidase-like activities of these nanomaterials were studied using H 2 O 2 and 3,3′,5,5′'-tetramethylbenzidine (TMB) as the reaction substrates in HAc-NaAc buffer. It was found that T30-G2-Fe NCs and T30-G2-Cu/Fe NCs, with a size of about 2 nm, exhibit similar and the strongest enzyme-like activity under optimal conditions. Both NCs possess a similarly high affinity to substrates, and the Michaelis–Menten constant ( K m ) values to TMB and H 2 O 2 are about 11 and 2–3 times lower than those of natural horseradish peroxidase (HRP), respectively. The activity of both nanozymes decreases to about 70% after being kept for one week in pH 4.0 buffer at 4 °C, which is comparable with HRP. Hydroxyl radicals (•OH) are the main reactive oxygen species (ROS) produced in the catalytic reaction. Moreover, both NCs can facilitate in situ generation of ROS in HeLa cells using endogenous H 2 O 2 . MTT assays indicate that the T30-G2-Cu/Fe NCs exhibit the strong selective cytotoxicity to HeLa cells over HL-7702 cells. The cellular viability is about 70% and 50% after incubating with 0.6 M NCs for 24 h without or with 2 mM H 2 O 2 , respectively. The current study shows that the T30-G2-Cu/Fe NCs have the potential for chemical dynamic treatment (CDT). Graphical abstract
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2023
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IF 4.3
Yunxin Shi,Liying Wang,Xin Miao,Zhenzhu Cao,Yongfeng Zhang,Lin Cheng,Jucai Yang
A series of donut-like nanostructured heterojunction materials are first synthesized via one-step solvothermal method to improve the photocatalytic efficiency for the environmental pollutants. The unique donut-like Fe-doped-BiOCl@Fe-MOF heterojunction with uniform size guarantees suitable surface area and many active sites for the model pollutant. The optimal photocatalytic efficiency is shown in degradation of RhB (99.0 %, 90 min) and TC (90.4 %, 90 min) solution, which had higher photocatalytic efficiency than a variety of similar materials previously reported. The result revealed that the enhancing photocatalytic activity is mainly depended on the synergistic effect of Fe-MOF and Fe-doped BiOCl. The possible mechanism is further studied, which shown h + and O 2 − are the primary active species in the degradation process of RhB and TC solution. Meantime, Fe-doped BiOCl@Fe-MOF with the excellent reusability and stability. After the fourth cycle, the degradation rate of RhB solution can still be as high as 86.4 %. In this work, we provide a higher efficiency heterojunction photocatalytic material by varying the organic ligand content.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2025
·
IF 6.2
Mingqiang Chen,Quan Wang,Defang Liang,Yishuang Wang,Chang Li,Xuemei Shen,Chunyue cheng,Jun Wang
Herein, a series of Fe-based biochar catalysts (xFe/WSBC) were synthesised via impregnation using wheat straw as a carbon precursor and applied to the Fischer–Tropsch synthesis of olefins (FTO) from syngas. Various characterisations of fresh catalysts demonstrated that Fe content significantly affected the dispersion of iron particles and the surface distribution of Fe 3 + /Fe 2+ . Among the samples, 5Fe/WSBC exhibited the highest surface Fe 3+ /Fe 2+ ratio and thus the lowest surface electron density, which enhanced the adsorption and activation of H 2 . In addition, an appropriate amount of the Fe additive (5 wt%) significantly decreased the Fe 3 O 4 particle size, which promoted the continuous reduction and carbonisation processes during FTO to generate iron carbide phases, which boosted CO activation and the subsequent C–C coupling. Therefore, 5Fe/WSBC exhibited the highest CO conversion (46.9 %) and iron time yield (348.9 μmol CO ·g Fe −1 ·s −1 ) as well as the major enhancement of selectivity to light olefins (C 2 = –C 4 = ). The results for the used catalysts demonstrated that 5 wt% Fe clearly inhibited the sintering of iron particle size and improved the catalytic stability of FTO.
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ACS Nano
·
2024
·
IF 15.8
Qing Luo,Qian Ma,Taoxia Liu,Yiting Luo,Lianying Wang,Chang Guo,Leyu Wang
We developed an intrinsic hydrophilic single-atom iron nanobowl (Fe-SANB) for magnetic resonance imaging (MRI)-guided tumor microenvironment-triggered cancer therapy. Benefiting from the sufficient exposure of Fe single atoms and the intrinsic hydrophilicity of the bowl-shaped structure, the Fe-SANBs exhibited a superior performance for T1-weighted MRI with an r1 value of 11.48 mM–1 s–1, which is 3-fold higher than that of the commercial Gd-DTPA (r1 = 3.72 mM–1 s–1). After further coembedding Gd single atoms in the nanobowls, the r1 value can be greatly improved to 19.54 mM–1 s–1. In tumor microenvironment (TME), the Fe-SANBs can trigger pH-induced Fenton-like activity to generate highly toxic hydroxyl radicals for high-efficiency chemodynamic therapy (CDT). Both the MRI and CDT efficiency of these nanobowls can be optimized by tuning the ratio of Fe(II)/Fe(III) in the Fe-SANBs via controlling the calcination temperature. Furthermore, the generation of •OH at the tumor site can be accelerated via the photothermal effect of Fe-SANBs, thus promoting CDT efficacy. Both in vitro and in vivo results confirmed that our nanoplatform exhibited high T1-weighted MRI contrast, robust biocompatibility, and satisfactory tumor treatment, providing a potential nanoplatform for MRI-guided TME-triggered precise cancer therapy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jiaojiao Sun,Mengxia Shen,A.jun Chang,Jianfeng Huang,Pengbo Wang,Yonghao Ni
Conventional metal-nitrogen-carbon single-atom catalysts (M-N-C SACs) are plagued by electron localization effects arising from symmetric coordination geometries and the absence of synergistic interactions among isolated active sites, both of which critically undermine oxygen reduction reaction (ORR) catalytic performance. To address these limitations, this study introduces a multiscale synergistic engineering strategy that integrates asymmetric coordination design with bioinspired structural innovation. Specifically, the symmetry of the Fe-N 4 coordination is disrupted to generate Fe-N 3 Se sites, which facilitate charge density redistribution; while Fe atomic clusters (FeACs) are strategically integrated to construct asymmetric catalytic centers that activate O 2 and promote O-O bond cleavage. A hierarchical porous carbon submicronspheres architecture, inspired by alveolar structures and featuring gradient-distributed micropores and mesopores, has been developed to enhance the mass transport efficiency at triple-phase interface. Overall, we have developed FeSAs and FeACs anchored on alveolar-inspired hierarchically porous nitrogen/selenium co-doped carbon submicronspheres (Fe SA+AC -N/Se-AHCs), which exhibits outstanding ORR activity (E o =0.99 V, E 1/2 =0.90 V) and long-term durability. Theoretical analyses further demonstrate that the electronic coupling between Fe-N 3 Se sites and FeAC synergistically optimizes the adsorption free energies of critical *OOH and *O intermediates, thereby accelerating O-O bond dissociation. This work presents a comprehensive cathode catalyst platform for developing high-energy-density and long-cycle-life Zinc-air batteries.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Jiangfu Zheng,Xiaoming Li,Jinglin Ding,Xingong Li
Research on peroxymonosulfate (PMS) activation via catalytic processes for degrading trace organic pollutants in aquatic environments has attracted considerable interest. Although iron is widely used in homogeneous advanced oxidation processes (AOPs), its effectiveness in activating PMS remains suboptimal. This study demonstrates that the environmentally benign chelating agent ethylenediamine- N , N ′-dibutyldicarboxylate (EDDS) markedly enhances iron-mediated PMS activation. With six coordination sites, EDDS forms stable five- and six-membered chelate rings with Fe(III)/Fe(II) ions, facilitating efficient PMS activation and leading to complete degradation of NTP. Beyond improving iron's catalytic performance, EDDS also inhibits iron disproportionation, thereby promoting PMS activation and facilitating NTP mineralization. Moreover, the system achieved removal efficiencies exceeding 96 % for tetracycline (TC), ciprofloxacin (CIP), sulfamethoxazole (SMX), and methylene blue (MB) within 35 min. Systematic experiments elucidated the critical role of the Fe(III)/Fe(II) redox cycle in the HeLDH/EDDS/PMS system, highlighting the central involvement of Fe(III) species in the regeneration of Fe(II). Multiple reactive oxygen species, including •OH, SO₄• − , RO•, O₂• − , and 1 O₂, were identified as contributors to NTP degradation. Transformation pathways and mechanistic details of NTP degradation were revealed via mass spectrometry, and toxicity evaluations confirmed a significant reduction in the ecotoxicity of oxidation products. The system also exhibited strong resistance to humic acid interference and effectively degraded multiple organic contaminants, underscoring its potential for sustainable water purification applications.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Lei Dong,Yangyang Yuan,Shengjie Zhu,Peidong Li,Xiaomin Zhang,Yanping Chen,Lei Xu
Direct synthesis of dimethyl carbonate (DMC) using CO2 and methanol as raw materials is an environmentally friendly and promising route for recycling carbon sources from exhaust gases. Herein, well-constructed CeO2-based nanoparticle catalysts promoted by various Fe contents were synthesized via a facile co-precipitation method and demonstrated to be highly effective for direct DMC synthesis. The uniform doping of iron species in ceria lattice resulted in the formation of more surface oxygen vacancies, and thereby more coordinatively unsaturated surface metal cations and lattice oxygen anions were generated, which served as the Lewis acidic-basic sites required for the reaction. Based on in-situ DRIFTS results, it was deduced that the oxygen vacancies played a crucial role in activating CO2 to reactive bidentate carbonates and the formation of active terminal methoxy intermediates was also enhanced by Fe incorporation. Consequently, the maximum DMC yield of 3.84 mmol h-1 g-1 cat was obtained on Fe0.04Ce0.96Ox under relatively mild reaction conditions of 130 °C and 3.0 MPa. Additionally, in the tandem reaction system using 2-cyanopyridine (2-CP) as a dehydrating agent, the catalytic activity for 2-CP hydration was found to be closely associated with the total basicity of the catalysts, and in turn a higher hydration rate was more conducive to the DMC synthesis through enhancing in-situ water removal efficiency. As expected, the present work provides in-depth insights into the structure-performance relationship of Fe-modified ceria-based catalysts for direct DMC synthesis from CO2 and methanol, and offers meaningful guidance for the advancement of highly efficient catalysts.
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JOURNAL OF GEOPHYSICAL RESEARCH-PLANETS
·
2024
·Vol. 129
·期 4
·e2023JE008031
·
IF 3.9
Xinyi Xiang,Peixin Du,Binlong Ye,Hongling Bu,Dong Liu,Jiacheng Liu,Jian Hua,Xiaolong Guo
Ferrihydrite, a nanocrystalline iron (oxyhydr)oxide mineral, is widely distributed in soils and sediments on Earth and is probably an important component and/or precursor of widespread nanophase iron minerals on Mars. Terrestrial ferrihydrite often co-occurs with amorphous silica and/or contains a certain amount of Si in its structure. However, it remains ambiguous how environmental Si concentration affects the formation-evolution and structure-spectral features of ferrihydrite in the Fe(III)-Si systems. To this end, hydrolysis experiments were carried out for Fe-Si systems at an unprecedentedly wide range of initial Si/(Fe + Si) molar ratios (0–0.80), followed by characterizing the products detailly. X-ray diffraction, Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, Mössbauer spectroscopy, and transmission electron microscopy results showed that at Si/(Fe + Si) molar ratios ≤0.30, the main phase of the products was ferrihydrite, of which the unit cells enlarged, the crystallinity decreased, and the existing state of Fe changed with increased Si contents; at Si/(Fe + Si) molar ratios ≥0.40, ferrihydrite was no longer formed and a novel amorphous Fe-O-Si phase was instead obtained, with the excess Si forming amorphous silica. The visible and near-infrared spectroscopy, the most powerful tool to detect hydrous minerals on the surface of Mars at global or regional scales, showed weakness in identifying ferrihydrite-like materials obtained in the Fe-Si systems. Raman spectroscopy can identify ferrihydrite and Si-containing ferrihydrite but cannot differentiate between them. Mössbauer spectroscopy showed great potential in both identifying and differentiating between ferrihydrite and Si-containing ferrihydrite, and thus can be used to characterize the poorly ordered iron (oxyhydr)oxides on Mars. Key Points Hydrolysis experiments of Fe(III)-Si systems were performed at an unprecedentedly wide range of initial Si/(Fe + Si) molar ratios (0∼0.80) The environmental Si concentration controls the formation and evolution of ferrihydrite in the Fe(III)-Si systems Mössbauer spectroscopy shows great potential in identifying and differentiating between ferrihydrite-like materials Plain Language Summary On the surface of ancient Mars where liquid water was available, Fe-Si hydrolysis systems were likely common as a result of the high abundances of Fe and Si in the crust of Mars. By performing hydrolysis experiments of Fe-Si systems at an unprecedented wide range of Si/(Fe + Si) molar ratios, we found that the hydrolysis products of Fe-Si systems varied among combinations of ferrihydrite, Si-containing ferrihydrite, an unknown Fe-O-Si phase, and amorphous silica. We also found that the visible and near-infrared reflectance spectroscopy, the most powerful tool to remotely detect hydrous minerals on the surface of Mars at global and regional scales, showed weakness in identifying ferrihydrite, Si-containing ferrihydrite, and the novel Fe-O-Si phase; Raman can be used to identify ferrihydrite-like materials but cannot be used to differentiate between ferrihydrite and Si-containing ferrihydrite; mid-infrared spectroscopy can differentiate ferrihydrite from Si-containing ferrihydrite and the novel Fe-O-Si phase; Mössbauer spectroscopy (recorded at varied temperatures) provided clues to identifying and further differentiating between ferrihydrite-like materials and thus holds great potential for detecting Fe/Si-rich phases on the surface of Mars.
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JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS
·
2026
·
IF 3
Long-Xiang Li,Zhi-Yue Li,Si-Rong Lu,Ting-Yong Chen
Exchange bias (EB) is characterized by a horizontal shift in magnetic hysteresis loops, originating from interfacial coupling between ferromagnetic (FM) and antiferromagnetic (AFM) layers. This phenomenon enables key regulation of magnetic coercivity and spin alignment in spintronic devices. Conventionally engineered in FM/AFM heterostructures. We report exchange bias (EB) in self-flux-grown Fe₁.₁Te single crystals, where Fe excess drives stoichiometric deviation. Structural analysis confirms a tetragonal FeTe phase with no secondary phases, while magnetic measurements reveal coexistence of ferromagnetic (FM) behavior (from excess Fe) and intrinsic antiferromagnetism (AFM) of FeTe. This is evidenced by a zero-field-cooled/field-cooled magnetization bifurcation below the Néel temperature ( T N ≈ 65 K). H EB decays linearly with temperature (vanishing near T N ) and scales with the magnitude of the cooling field. We attribute EB to interfacial coupling between FM clusters (Fe-rich) and the AFM FeTe matrix. This work establishes Fe₁.₁Te as a tunable platform for antiferromagnetic spintronics, leveraging stoichiometric control to engineer interfacial magnetic coupling.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Qing Cheng,Yanzhuo Lv,Deyu Li,Ning Li,Qiao Ding,Yinghai Zhao,Qi Zhao
The Sn-Fe alloy coating is a potential choice for decorative coatings and electronic products because of its excellent performance. However, oxidation of the bath is likely to occur in the process of use, which limits the production of electrodeposition of Sn-Fe alloy. Resveratrol has excellent antioxidant capacity and is considered as a non-polluting natural antioxidant. However, the understanding of using of resveratrol as stabilizer for electroplating solution in the field of electrodeposition is limited. In this study, resveratrol, hydroquinone and TBHQ are selected as the stabilizers of the electroplating bath to conduct comparative experiments for measuring the stability effect of resveratrol. The antioxidant capacities of three stabilizers are compared by means of the natural oxidation experiment, H 2 O 2 accelerated oxidation experiment and electrochemical testing. The natural oxidation experiment and H 2 O 2 accelerated oxidation experiment confirm that the antioxidant effect of resveratrol is higher than hydroquinone and TBHQ. To determine the optimal concentration of resveratrol in the electroplating solution, EIS and salt spray test were conducted. These results show that appropriate resveratrol can improve the corrosion resistance of the coating, but excessive resveratrol is detrimental to corrosion resistance. Therefore, the optimal concentration of resveratrol in the electroplating solution is 1.0 g/L.
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Functional Materials Letters
·
2020
·
IF 2
Yao Liu,Ciqun Xu,Huan Ren,Zaixin Wei,Zidong Zhang
Meta-composites with negative permittivity are promising candidates for future electronics such as microwave absorbers, novel capacitors, etc. In this work, we proposed to develop the Fe/BaTiO 3 meta-composites with tuneable negative permittivity. Fe content influenced the conductivity of composites and even led to the change of the conductive mechanism. The tuneable permittivity behavior was achieved by controlling the Fe fraction, and the plasma oscillation theory was employed to explain the negative permittivity behavior. Meanwhile, a frequency-switched negative permittivity was observed in this composite, which could be used to extend applications of meta-composites.
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