ACS Applied Energy Materials
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2024
·
IF 5.4
Wenyan Zhang,Yihan Wang,Weidong Tao,Hangmin Guan,Chaoqun Jiang,Wenjie Tian,Lingyun Hao
Montmorillonite (MMT), a layered hydrated aluminum silicate mineral, emerges as a promising catalyst support due to its substantial specific surface, ion storage capacity, thermal stability, and cost-effectiveness. Despite the success of MMT-based photocatalysts in degrading compounds, their potential for the photocatalytic hydrogen evolution reaction (HER) is underexplored. Furthermore, the reliance on noble metals and dye sensitization in MMT-based photocatalysts leads to elevated costs. This study introduces an MMT-based photocatalyst modified with Fe species (denoted as Fe@MMT) for photocatalytic HER without the reliance on noble metals and dye sensitization. The incorporation of Fe species has a dual impact, expanding the light harvesting region of MMT and modulating the aluminum-silicate framework. Simultaneously, it facilitates the exfoliation of individual sheets from stacked MMT layers, generating abundant active sites and inner electronic fields that can promote the separation of photoexcited electrons and enhance the photon-to-electron conversion. In comparison to pristine MMT, Fe@MMT exhibits a 43% reduction in the charge transfer resistance in the dark and a 52% reduction under illumination. Additionally, the majority carrier density within the space charge region increased by 33%. Due to these advantages, the photocatalytic HER efficiency over Fe@MMT was improved, approximately 2.9 times that of pristine MMT.
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CHEMOSPHERE
·
2024
·
IF 8.1
Yunzhan Ying,Shikun Liang,Fayang Zhang,Xiangwei Xu,Chenbo Qian,Long Jiang,Jing Zhou,Yulong Wan,Lie Wang,Yuyuan Yao
The harmful impact of organic pollutants on aquatic ecosystems underscores the pressing need for effective remediation. While activating peroxymonosulfate (PMS) with Fe catalyst offers a promising approach for eliminating these pollutants, its widespread use is hindered by the sluggish regeneration of Fe 2+ from Fe 3+ . Here, this study demonstrates for the first time that combining an Fe catalyst with Mo 2 C (Fe-Mo 2 C) enhances the Fe³⁺/Fe 2 ⁺ cycle, thereby improving PMS activation. The Fe-Mo 2 C/PMS system achieved near-complete degradation of carbamazepine (CBZ) within only 8 minutes, with an impressive observed rate constant ( k obs ) of up to 0.624 min -1 , about 15 times greater than that of Fe-C catalyst. It also exhibits the capability to degrade a broad range of common antibiotics, phenols, and dye-like organic compounds. Through electron paramagnetic resonance (EPR) analysis and quenching experiments, it was verified that hydroxyl radicals (·OH), sulfate radicals (SO 4 ·- ), singlet oxygen ( 1 O 2 ), and superoxide radicals (·O 2 - ) species during the reaction, with the former three serving as the primary active species. These findings offer a hopeful avenue for the systematic development and enhancement of catalysts specifically designed to efficiently remediate organic pollutants in wastewater.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Shengkang Zhang,Yu Xiao,Qiwei Feng,Ziqiang Lei
The oxygen evolution reaction (OER) plays a pivotal role in the hydrolysis process of zinc–air batteries. Consequently, it is essential to develop cathode catalysts with both cost-effectiveness and high oxygen evolution activity. In this study, we synthesized the FeFFIVE-1-Ni two-dimensional (2D) metal–organic framework (MOF) nanosheets via a straightforward solvothermal approach and oxidized them in an air atmosphere. During the calcination process in an air atmosphere, the heteroatoms (O, F) within the FeFFIVE-1-Ni 2D MOF nanosheets combine with iron and nickel metal ions, forming FeOF and NiF2 compounds. The synergy between these compounds and the creation of surface cracks during calcination yield catalytic active power and catalytic active sites essential for the oxygen evolution reaction. Notably, the overpotential of FeFFIVE-1-Ni 2D MOF nanosheets calcined in air under alkaline test conditions (η10 = 286 mV) was lower than that of commercial RuO2 catalysts (η10 = 355 mV). This work presents an effective strategy for replacing noble metal catalysts such as RuO2 by simply treating fluorinated metal–organic frameworks.
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APPLIED CLAY SCIENCE
·
2012
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IF 2.474
Zhujian Huang,Pingxiao Wu,Xing Zhang,Xiaorong Wang,Nengwu Zhu,Jinhua Wu,Ping Li
In this study, intercalation of Fe(III) complexes [Fe(Ox) 3 ] 3− and [Fe(Cit) 2 ] 3− in Mg 2 Al layered double hydroxides (LDHs) had been carried out by different routes: direct self-assembly, reconstruction and anion exchange. The result of XRD indicated that these two kinds of Fe(III) complexes intercalated LDHs (LDHs/Fe-complexes) could be successfully synthesized by anion exchange obtaining two well crystallized LDHs both with a large basal spacing. The chemical environment of iron ion in the intercalated Fe complexes was determined by FTIR , XPS and XAFS, the results of which concertedly proved that the intercalated Fe complexes were well preserved in the interlayer of LDHs. The arrangement of the Fe(III) complexes anions in the galleries of LDHs was studied by one-dimensional electron density projection. The results showed that the [Fe(Ox) 3 ] 3− anions were probably accommodated in the gallery of LDHs as an interdigitated bilayer arrangement, and the [Fe(Cit) 2 ] 3− were perpendicularly arranged against the LDHs sheets. Through the research, it is proved that the obtained LDHs/Fe-complexes markedly enhanced the UV–vis absorption ability of Fe complexes.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2024
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IF 4.3
Kaining Zhang,Hao Sun,Long Wei,Rui Hu,Hao Liu,Yongchao Lai,Xun Li
Glutathione (GSH) levels have been well validated to correlate with a variety of physiological and pathological conditions, such as malignancy, cardiovascular disease and aging, making the development of accurate, robust and sensitive GSH detection methods highly desirable. In this study, a novel metal–organic framework (MOF-Fe(DTNB))-based colorimetric method with a favorable dual-triggering function was proposed. MOF-Fe(DTNB) exhibits high peroxidase activity, which can catalyze the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue ox-TMB by hydrogen peroxide (H 2 O 2 ). This oxidation process of TMB can be inhibited not only by the reducing action of GSH, but also by the thiol exchange reaction between DTNB and GSH, in which the disulfide bond of DTNB in MOF-Fe(DTNB) is cleaved. Thus, with this dual triggering mechanism, the GSH concentration can be robustly measured in the MOF-Fe(DTNB)-derived colorimetric strategy. Significantly, this method is accurate (RSD < 6 %), selective and sensitive in biological plasma samples, with satisfactory recovery rates (96.7–103.3 %). It requires less instrumentation and has less interference from other substances. The linear range of the method is 0–80 µM, and the detection limit is as low as 0.28 µM. This dual-triggering MOF-Fe(DTNB)-derived colorimetric strategy has greatly simplified the GSH detection processes with improved accuracy, in both acidic and basic environments, which has potent applications in biochemical analysis and point-of-care testing.
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Environments
·
2024
·Vol. 11
·期 7
·136
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IF 3.5
Junhao Zheng,Mei Jiang,Qingzhu Li,Weichun Yang
Fe/Mn (hydr)oxides are metallic compounds that exhibit significant redox activity in environmental media and play a pivotal role in geochemical processes, thereby influencing the fate of metals in porous media. The morphology of Fe/Mn (hydr)oxides in natural environments and their interactions with trace metals are significantly influenced by the presence of natural organic matter (NOM). However, there is limited understanding regarding the formation, transport, and stability of Fe/Mn (hydr)oxides in the environment. The present study employed humic acid (HA) as a representative NOM material to investigate the positive influence of HA on the formation of Fe/Mn colloids. However, there remains limited comprehension regarding the formation, transport, and stability of Fe/Mn (hydr)oxides in the natural environment. In this study, we investigated the positive effect of natural organic matter (NOM) on the formation of Fe/Mn colloids using humic acid (HA) as a representative NOM material. We comprehensively characterized the chemical and physical properties of HA–Fe/Mn colloids formed under various environmentally relevant conditions and quantitatively analyzed their subsequent aggregation and stability behaviors. The findings suggest that the molar ratios of C to Fe/Mn (hydr)oxide play a pivotal role in influencing the properties of HA–Fe/Mn colloids. The formation and stability of HA–Fe/Mn colloids exhibit an upward trend with increasing initial molar ratios of C to Fe/Mn. Redox and metal–carboxylic acid complexation reactions between HA and hydrated iron/manganese oxides play a pivotal role in forming colloidal HA–Fe/Mn complexes. Subsequent investigations simulating porous media environments have demonstrated that the colloidal structure resulting from the interaction between HA and Fe/Mn facilitates their migration within surrounding porous media while also enhancing their retention in the surface layers of these media. This study offers novel insights into the formation and stabilization mechanisms of HA–Fe/Mn colloids, which are pivotal for comprehending the behavior of Fe/Mn colloids and the involvement of Fe/Mn (hydr)oxides in geochemical cycling processes within porous media.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
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IF 12.2
Pengtao Cai,Tong Chen,Mingxiu Zhan,Xiaojun Ma,Masaki Takaoka,Chen Sun,Xiaodong Li
Global concern over per- and polyfluoroalkyl substances (PFASs), especially perfluorooctane sulfonate (PFOS), disposal prompts the search for effective degradation methods. Subcritical water hydrothermal treatment shows promise but suffers from unclear degradation pathways, hindering engineering application design due to unknown intermediate products. This study introduces Fe-based amorphous alloy to enhance the subcritical water hydrothermal degradation of PFOS, achieving a degradation rate of approximately 85 % under optimized conditions of 325 °C and 1 M sodium bicarbonate (NaHCO₃), compared to 56 % without the alloy. Analysis of liquid and gas-phase products, along with identification of potential intermediate products, led to proposing a reaction pathway for Fe-based amorphous alloy-enhanced subcritical water hydrothermal PFOS degradation. Additionally, the distribution of fluorine in PFOS was determined by fluorine-19 nuclear magnetic resonance ( 19 F NMR), and the energy changes of key degradation steps were calculated based on DFT, which provided concrete evidence for the degradation process and verified the mechanism of subcritical hydrothermal degradation of PFOS enhanced by Fe-based amorphous alloys. Most importantly, the Fe-based amorphous alloy demonstrated effectiveness upon repeated use after water washing. These results endorse its potential as a PFOS degradation catalyst.
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ENVIRONMENTAL TECHNOLOGY
·
2024
·
IF 2.2
Yiqing Liu,Linghan Xu,Xin Li,Shixiang Wang
Ascorbic acid (AA) was used as a reducing agent to improve the Fe(III)-activated peracetic acid (PAA) system for the removal of sulfamethoxazole (SMX) in this work. The efficiency, influencing factors and mechanism of SMX elimination in the AA/Fe(III)/PAA process were studied. The results exhibited that AA facilitated the reduction of Fe(III) to Fe(II) and subsequently improved the activation of PAA and H2O2. Various radicals, including organic radicals (e.g. CH3C(O)O• and CH3C(O)OO•) and hydroxyl radical (HO•), were rapidly formed from the activated PAA and H2O2, resulting in SMX removal. Increasing dosages of PAA and Fe(III) contributed to enhanced SMX degradation, while excessive PAA and Fe(III) did not further promote SMX degradation. Due to the radicals' quenching effect, excess AA hindered SMX elimination in the AA/Fe(III)/PAA process. The presence of HCO3− and Cl− inhibited SMX removal in this system, whereas NO3−, SO42− and natural organic matter had little impact on SMX degradation. The transformation pathways of SMX in the AA/Fe(III)/PAA system included hydroxylation, bond cleavage and amino oxidation. This research provides a strategy to enhance the Fe(III)-activated PAA system for the elimination of refractory organic pollutants.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Mengyue Qi,Huamei Tong,Gaojie Li,Xinyu Zheng,Yu Liu,Cheng Ye,Zaoxue Yan,Deli Jiang
Designing and development of electrocatalysts with high catalytic capacity and stability for oxygen evolution reaction (OER) is significant for sustainable water splitting. In this study, we rationally designed Fe-doped Co 2 RuO 4 /RuO 2 heterostructure electrocatalysts on nickel foam (NF) through mixture hydrothermal, ion exchanging, and calcining methods. The synergistic effect between the Fe-Co 2 RuO 4 /RuO 2 heterogeneous interfaces can result in superior inherent activity. Meanwhile, the unique nanosheet on nanosheet structure delivers abundant exposed active sites, leading to improved catalytic activity. The resultant Fe-Co 2 RuO 4 /RuO 2 heterostructured catalysts possessed superior OER property, attaining a current density of 50 mA cm −2 with only 253 mV overpotential in 1.0 M KOH alkaline solution, and demonstrating good durability with continuous operation for up to 50 h. This research provides robust support for the research and development of RuO 2 -based electrocatalysts through effective interface engineering and doping strategies, and opens up new avenues for the industrial application of water splitting technology.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yunlong Yao,Peng Zhang,Yao Wang,Zhou Du,Zhichao Sun,Ying-Ya Liu,Anjie Wang
This study investigates the catalytic hydrogenation of biomass-derived furfural to value-added products, especially tetrahydrofurfuryl alcohol and furfuryl alcohol. A series of Ni-Fe-Al composite catalysts were synthesized through co-precipitation and subsequent hydrogen reduction. Among these, the Ni 5 Fe 1 Al 2 catalyst demonstrated extraordinary catalytic performance, achieving complete furfural conversion and 92.9 % tetrahydrofurfuryl alcohol selectivity under mild conditions (50 °C, 0.5 MPa H 2 ). Comprehensive characterization using XRD, TEM, and XPS revealed that the optimized Ni 5 Fe 1 Al 2 –400 catalyst possessed high dispersion and abundant oxygen vacancies. The addition of pyridine in the feed had a great impact on the hydrogenation rate of furfuryl alcohol but much less on that of furfural. With pyridine in the feed, the main product shifted from tetrahydrofurfuryl alcohol to furfuryl alcohol, while maintaining complete furfural conversion and achieving 97.5 % furfuryl alcohol selectivity at 50 °C. The Ni 5 Fe 1 Al 2 –400 deactivated in the 50-h run and can be regenerated by simple in-situ reduction, demonstrating excellent regenerability. These findings provide valuable insights into the design of efficient catalysts for selective biomass conversion.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhengang Zhou,Junjie Zheng,Lingyu Shao,Xiao Zhang,Chengjin Pan,Xiuqi Hu,Kai Feng,Hao Song,Shihan Zhang,Chenghang Zheng,Xiang Gao
Catalytic solvent regeneration has garnered significant attention due to its capacity to lower energy demands in industrial processes, promoting broader adoption of carbon capture systems. While progress has been made in catalyst engineering, creating efficient solid acid catalysts still encounters critical obstacles such as synthesizing mesoporous architectures with extensive surface areas and improving the spatial arrangement of active sites. Herein, this study developed a Ni/Fe@KIT-6 catalyst with ordered porosity and dual metal acid sites, leveraging the three-dimensional cubic pore structure of mesoporous silica to enhance liquid-solid mass transfer. The anchored Ni/Fe clusters synergistically enhanced proton transfer, reducing the activation energy of carbamate decomposition through optimized intermediate adsorption configurations. Catalytic testing revealed a 58.1 % enhancement in CO₂ desorption efficiency alongside a 41.2 % decrease in energy requirements relative to non-catalytic systems. The material maintained stable performance across multiple absorption-desorption cycles (efficiency decline <10 %), linked to the KIT-6 framework's retained structural stability and optimized metal-support bonding. Theoretical calculations revealed that the Ni/Fe dual sites lowered the CO 2 desorption reaction energy barrier, aligning with the enhanced CO₂ desorption efficiency. This synergistic interaction of dual metal acid sites within a high-surface-area architecture highlights viable pathways for scalable and energy-efficient CO₂ desorption, thereby advancing practical strategies for large-scale deployment of carbon capture technologies.
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Advanced Science
·
2025
·
IF 14.1
Siqi Qiu,Hao Wan,Yuechao Yao,Xiao Xu,Zhangjian Li,Yongbiao Mu,Biaolin Peng,Hongliang Wu,Jizhao Zou,Lin Zeng
Iron-nitrogen-carbon (Fe-N-C) materials are promising non-precious metal catalysts for the oxygen reduction reaction (ORR), yet their long-term stability remains a critical challenge due to the dissolution of Fe-based active sites and corrosion of the carbon support. Here, a Fe-Zr dual-atom carbon-based catalyst (Fe,Zr-NC) via a one-step solid-state synthesis method is reported. The introduction of atomically dispersed Zr–N units adjacent to Fe–N 4 centers creates a dual-metal coordination structure that modulates the local electronic environment of Fe and weakens * OH adsorption, which is the rate-limiting step in the ORR process. Density functional theory (DFT) calculations reveal that the Fe–Zr synergy positions the catalyst near the apex of the ORR activity volcano. Extended experimental EXAFS confirms a Fe–Zr distance of ≈3.30 Å, closely matching the theoretical optimum (≈3.39 Å). As a result, Fe, Zr-NC achieves a high half-wave potential (0.891 V vs reversible hydrogen electrode (RHE)) with negligible activity loss over 5000 cyclic voltammetry cycles, outperforming commercial Pt/C. In zinc–air batteries, the catalyst delivers a peak power density of 185.7 mW cm −2 and operates stably for over 453 h. This work highlights the importance of dual-atom synergy in tuning intermediate binding energies and provides design principles for next-generation ORR electrocatalysts.
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