ACS Applied Nano Materials
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2024
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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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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
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IF 6.9
Ping Zhang,Feiping Zhao,Penggang Li,Junhao Zheng,Weichun Yang,Qingzhu Li,Zhihui Yang
Electrocoagulation (EC) is a facile technique for removing arsenic (As) pollutants from different water matrices with high efficiency. In this work, a novel strategy of Mn-assisted Fe EC was developed to further enhance the removal efficiency of arsenite [As(III)] from wastewater. When 1 mM of MnCl 2 was added to an Fe-EC system, the As removal efficiency reached 99.99%, and the residual concentration was only 9 μg/L, which is lower than the World Health Organization’s limit for drinking water . The characteristics of the generated flocs by four different EC processes in Fe, Fe-Mn, Fe-As, and Fe-Mn-As systems were investigated. The results showed that Mn 2+ promoted the formation of FeOOH, FeO x , MnO x , FeHAsO 4 , and MnHAsO 4 through low crystallinity and a high surface area . Density functional theory simulation and crystal orbital hamiltonian population confirmed that the generated Fe-Mn flocs had a greater adsorption affinity for As(III) and arsenate [As(V)]. The possible reactions in the EC processes and reaction mechanisms were also hypothesised. The current work provides meaningful insights into understanding the mechanisms of Mn-assisted Fe-EC systems, and further confirms its potential for practical applications in As pollution treatment.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 14
·14350-14361
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IF 2.914
Wu Kang,Si Xiongyuan,Jiang Jin,Si Youbin,Sun Kai,Yousaf Amina
In this study, a novel Fe–Mn binary oxide (FMBO), which combined the oxidation capability of iron and manganese oxides, was constructed to remove sulfamethoxazole (SMX) effectively using the simultaneous co-precipitation and oxidation methods, and the reaction products were probed by liquid chromatography-mass spectrometry (LC/MS). Particularly, FMBO-mediated transformation mechanisms of SMX were explored using radical scavengers and electron paramagnetic resonance (EPR). Results indicated that the best removal efficiency was obtained at a pH of 4.0, with the H 2 O 2 of 6.0 mmol/L and the FMBO dosage of 2.0 g/L, giving 97.6% removal of 10 mg/L SMX within 60 min. More importantly, we found that the hydroxyl (•OH) radicals generated by FMBO through Fenton-like reaction were responsible for the SMX oxidation. EPR studies were confirmed that the peak intensities of hydroxyl adduct decreased remarkably with increasing pH values. Moreover, the four SMX degradation intermediate products were detected by LC/MS and a reaction pathway for the possible mineralization of SMX, with •OH radicals as the main oxidant, was proposed. These findings provide a novel insight into the removal of SMX by FMBO-mediated radical reactions in aquatic environments. Moreover, this research suggested that FMBO can act as an efficient catalyst to remove SMX in hospital wastewater.
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Advanced Energy Materials
·
2025
·
IF 26
Zongge Li,Wenjun Kang,Jingkai Lin,Rui Li,Konggang Qu,Suyuan Zeng,Lei Wang,Fanpeng Meng,Huayang Zhang,Haibo Li
The oxygen electrocatalytic activity of transition metal catalysts can be tuned by tailoring their microstructure to optimize electronic configuration. Here, a one-step Coordination-Selective Synthesis strategy is developed to integrate Co single-atom sites and Fe-based nanoparticles within the same matrix, enabling long-range electronic interactions that enhance Co-N 4 reactivity and improve oxygen reduction reaction performance. X-ray absorption spectroscopy confirmed that remote Fe-based nanoparticles modulate the electron distribution at Co-N 4 sites. Structural characterizations reveal that the optimal catalyst, Co 50% Fe 50% -NC, contains metallic Fe, Fe 3 O 4 , and Fe 4 N species. Electrochemical measurements show that it achieves onset and half-wave potentials of 0.984 and 0.927 V versus RHE, surpassing Co 100% -NC with only Co-N 4 sites. Additionally, it demonstrates efficient oxygen evolution reaction performance, achieving an overpotential of 298 mV at 20 mA cm −2 , comparable to RuO 2 . Density functional theory calculations reveal that Fe 4 N optimizes O-containing intermediate adsorption/desorption, lowering the theoretical overpotential. Zn-air batteries assembled with Co 50% Fe 50% -NC exhibited superior performance to Pt/C, highlighting its potential for bifunctional oxygen electrocatalysis. This study provides an approach for designing high-performance catalysts by utilizing synergistic interactions between atomic and nanoscale metal species.
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ACS Omega
·
2024
·
IF 3.7
Boyao Sun,Xuewei Zheng,Xiaoyu Zhang,Huaiyu Zhang,Yang Jiang
Oxaliplatin (Oxa) is a commonly used chemotherapy drug in the treatment of gastric cancer, but its toxic side effects and drug resistance after long-term use have seriously limited its efficacy. Loading chemotherapy drugs with nanomaterials and delivering them to the tumor site are common ways to overcome the above problems. However, nanomaterials as carriers do not have therapeutic functions on their own, and the effect of single chemotherapy is relatively limited, so there is still room for progress in related research. Herein, we construct Oxa@Mil-100(Fe) nanocomposites by loading Oxa with a metal–organic framework (MOF) Mil-100(Fe) with high biocompatibility and a large specific surface area. The pore structure of Mil-100(Fe) is conducive to a large amount of Oxa loading with a drug-loading rate of up to 27.2%. Oxa@Mil-100(Fe) is responsive to the tumor microenvironment (TME) and can release Oxa and Fe3+ under external stimulation. On the one hand, Oxa can inhibit the synthesis of DNA and induce the apoptosis of gastric cancer cells. On the other hand, Fe3+ can clear overexpressed glutathione (GSH) in TME and be reduced to Fe2+, inhibiting the activity of glutathione peroxidase 4 (GPX4), leading to the accumulation of intracellular lipid peroxides (LPO), and at the same time releasing a large number of reactive oxygen species (ROS) through the Fenton reaction, inducing ferroptosis in gastric cancer cells. With the combination of apoptosis and ferroptosis, Oxa@Mil-100(Fe) shows a good therapeutic effect, and the killing effect on gastric cancer cells is obvious. In a nude mouse model of subcutaneous tumor transplantation, Oxa@Mil-100(Fe) shows a significant inhibitory effect on tumor growth, with an inhibition rate of nearly 60%. In addition to its excellent antitumor activity, Oxa@Mil-100(Fe) has no obvious toxic or side effects. This study provides a new idea and method for the combined treatment of gastric cancer.
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Environments
·
2024
·Vol. 11
·期 7
·136
·
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
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2024
·
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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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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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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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xingyu Zhong,Baoan Xu,Jianing Li,Weiyu Fang,Yuxuan Shen,Mei Bai,Xiulan Hu
High-efficiency oxygen reduction electrocatalysts is crucial for low-carbon development. Iron-nitrogen co-doped carbon materials (Fe-N-C) prepared from ZIF-8 are well recognized for their remarkable potential to enhance ORR reaction rates. However, the challenge of limited and singular active sites due to insufficient metal loading has impeded the progress of Fe-N-C-based materials. In this paper, the above-mentioned problems were alleviated by introducing a second transition metal (Co, Mn, Zr) to form a bimetallic catalyst with Fe. Carboxylates are also introduced for assistance to generate one-dimensionally entangled carbon nanotubes, then the material can perform charge transfer better. In the alkaline medium, the half-wave potential of FeCo-N-C-OAc synthesized with carboxylate added reached 0.907 V, FeMn-N-C-OAc was 0.893 V, and FeZr-N-C-OAc was 0.892 V, which was improved compared with the samples without carboxylate added. In the range of 100–1000 ppm oxygen concentration, the oxygen sensors based on three catalysts that with carboxylate added showed good linearity and high response currents, especially FeMn-N-C-OAc showed an average response time of 53 s and a relative current fluctuation of only 4 % after 28 days. When improving the performance of Fe-N-C-based catalysts used in coulometric electrolytic oxygen sensors, this work can be regarded as a new strategy.
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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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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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