ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Sihan Ma,Jun Xie,Lin Wang,Zonglang Zhou,Xian Luo,Jianghua Yan,Guang Ran
Photothermal/photodynamic therapy (PTT/PDT) and synergistic therapeutic strategies are often sought after, owing to their low side effects and minimal invasiveness compared to chemotherapy and surgical treatments. However, in spite of the development of the most PTT/PDT materials with good tumor-inhibitory effect, there are some disadvantages of photosensitizers and photothermal agents, such as low stability and low photonic efficiency, which greatly limit their further application. Therefore, in this study, a novel bismuth-based hetero-core–shell semiconductor nanomaterial BiNS–Fe@Fe with good photonic stability and synergistic theranostic functions was designed. On the one hand, BiNS–Fe@Fe with a high atomic number exhibits good X-ray absorption, enhanced magnetic resonance (MR) T2-weighted imaging, and strong photoacoustic imaging (PAI) signals. In addition, the hetero-core–shell provides a strong barrier to decline the recombination of electron–hole pairs, inducing the generation of a large amount of reactive oxygen species (ROS) when irradiated with visible–NIR light. Meanwhile, a Fenton reaction can further increase ROS generation in the tumor microenvironment. Furthermore, an outstanding chemodynamic therapeutic potential was determined for this material. In particular, a high photothermal conversion efficiency (η = 37.9%) is of significance and could be achieved by manipulating surface decoration with Fe, which results in tumor ablation. In summary, BiNS–Fe@Fe could achieve remarkable utilization of ROS, high photothermal conversion law, and good chemodynamic activity, which highlight the multimodal theranostic potential strategies of tumors, providing a potential viewpoint for theranostic applications of tumors.
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Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 9
·3636-3645
·
IF 6.482
Xiaoqin Li,Taotao Gao,Qilin Liu,Yanxue Xu,Jing Li,Dan Xiao
Fiber-shaped energy storage devices (FESDs) are indispensable for developing portable and wearable electronic products. Aqueous rechargeable Ni/Fe batteries are an appropriate candidate due to the cost-effectiveness, high ionic conductivity, and great safety. However, their energy density is still far from satisfactory, hindering further practical applications. Herein, we focused on studying binder-free fibrous electrodes for high-performance FESDs based on rechargeable Ni/Fe batteries. A fast microwave-assisted synthesis method was adopted to grow active materials with a 3D conductive network which is constructed from carbon nanotubes decorated with Fe–Fe3C nanoparticles. Due to the heterogeneous structure, the active materials depicted improved electron/ion transfer, boosting the electrochemical performance of the anode. A flexible Ni/Fe battery is successfully fabricated using the aforementioned anode coupled with a NiCoO-based cathode which is synthesized by electrodeposition and a post-annealing process. Thanks to the special structure of the active materials and the fast redox reaction, the assembled flexible Ni/Fe battery achieved high electrochemical properties with a maximum volumetric specific capacity of 1.61 mA h cm−3 and energy density of 1.28 mW h cm−3. The cycling stability and mechanical flexibility were also tested, which demonstrated the prospects for practical application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
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IF 16.683
Cong Gao,Yan Su,Xie Quan,Virender K. Sharma,Shuo Chen,Hongtao Yu,Yaobin Zhang,Junfeng Niu
Heterogeneous Fenton-like reaction was a promising approach for generating •OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X = NH 2 , CH 3 , H, Br and NO 2 ) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO 2 , with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential ( E Fe(III)/Fe(II) = 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7–20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe 2+ . This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
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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 GEOPHYSICAL RESEARCH-PLANETS
·
2024
·Vol. 129
·期 4
·e2023JE008031
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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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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 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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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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Catalysts
·
2023
·Vol. 13
·期 7
·1057
·
IF 3.9
Rongwei Zheng,Ruifan Tan,Yali Lv,Xiaoling Mou,Junqiao Qian,Ronghe Lin,Ping Fang,Weidong Kan
Iron-based materials are widely applied in Fenton chemistry, and they have promising prospects in the processing of wastewater. The composition complexity and rich chemistry of iron and/or oxides, however, hamper the precise understanding of the active sites and the working mechanism, which still remain highly controversial. Herein, iron oxides of four different model systems are designed through a conventional precipitation method plus H2reduction treatment. These systems feature Fe@Fe3O4with abundant oxygen vacancy, Fe0and Fe3O4particles with interface structures, and Fe3O4-dominated nanoparticles of different sizes. These materials are applied in the decomposition of methyl orange as a model reaction to assess the Fenton chemistry. The Fe@Fe3O4with core–shell structures exhibits significantly higher decomposition activity than the other Fe3O4-rich nanoparticles. A thin Fe3O4layer formed by auto-oxidation of iron particles when exposed to air can boost the activity as compared with the Fe0and Fe3O4particles with interface structures but poor oxygen vacancy. The unique hetero-structure with the co-existence of both metallic iron and oxygen vacancy displays excellent redox propensity, which might account for the superior Fenton activity. This finding provides a new perspective to understand and design highly efficient iron-based Fenton catalysts.
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RSC Advances
·
2023
·Vol. 13
·期 35
·24812-24818
·
IF 3.9
Songtao Xiao,Yubing Xue,Jing Zhao,Xiechun Liu,Haifeng Cong,Tian Lan,Xiaojuan Liu,Dashu Pan,Lingyu Wang,Guoan Ye,Yinggen Ouyang
The significant differences in the catalytic properties caused by different ‘isotopic catalysts’ were discovered for the first time. The commonly purchased Fe2O3 is a ‘mixture’ of different Fe isotopic oxides which means the catalytic effect of Fe2O3 is theoretically a synthetical result of all isotopic compounds. In this work, the differences in catalytic properties of α-Fe2O3 with natural abundance ratio and separated isotopic α-Fe2O3 (α-54Fe2O3, α-56Fe2O3, and α-58Fe2O3) catalyzing thermal decomposition of ammonium perchlorate (AP) were investigated, and are mainly attributed to the difference in the charge distribution of the nuclei of different iron isotopes. The result suggests that isotope effects in different isotopes when utilized as catalysts are caused by nuclear morphology and the nuclear charge distribution. This study will serve as a base as well as an initiation for future studies of the isotopic catalyst.
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