JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Chenjie Ding,Shifei Kang,Wenxin Li,Weikang Gao,Zhihao Zhang,Lulu Zheng,Lifeng Cui
Heterogeneous photo-Fenton catalysts prepared by doping metal ions in g-C 3 N 4 are promising alternatives to traditional homogeneous Fenton catalysts, but are restricted by poor mesoporous structure and agglomerate of metal species. Recently, the highly uniformly dispersed metal-N active sites in various photocatalysts have been proved to be the critical reason for their enhanced catalytic activity. In this study based on reasonable control of mesoporous structure and metal-N active sites, mesoporous Fe-g-C 3 N 4 was synthesized using a simple one-step thermal shrinkage polymerization method using ferrous oxalate as iron source and pore-forming agent. The Fe and N elements in the triazine ring skeleton of Fe-g-C 3 N 4 form a σ-π bond, thus the photogenerated electrons can be quickly transferred to Fe 3+ to form Fe 2+ under the interaction of chemical bonds, accelerating the Fenton reaction rate. Density functional theory calculations results demonstrate that the energy band structure and electron cloud density distribution of Fe-Nx active structure are better than that of routine FeOx crystal structure with metal species agglomeration. In addition, the excellent mesoporous structure of Fe-g-C 3 N 4 creates conditions for the high exposure of Fe-Nx active sites in the photo-Fenton reaction under visible light. The as-developed Fe-g-C 3 N 4 system shows high recyclability and excellent photo-Fenton performance for removal of typical intractable pollutants (The degradation rate of dye and tetracycline reaches 98.2% and 98.7% at 60 and 120 min, respectively). This work provides a facile and sustainable route to develop mesoporous highly-active heterogeneous Fenton-like catalysts and even further general the design of general catalyst with ideal metal-N active sites, thereby promoting a feasible and efficient wastewater remediation solution.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xianfa Zhang,Mingzhao Huang,Zuoming Zhou,Xiaodan Zhao,Guohua Jing
Sulfite activation with iron-based heterogeneous activators is a promising technology for the removal of organic contaminants from water. However, the slow valence transformation of >Fe(II)/>Fe(III) compromises sulfite activation efficiency. Regarding that the oxygen vacancy (Vo) can modulate the charge distribution and thus enhance >Fe(II)/>Fe(III) valence transformation via rapid electron transfer, Vo-enriched γ-Fe 2 O 3 is constructed for sulfite activation (simplified as the γ-Fe 2 O 3 -Vo/sulfite system). The γ-Fe 2 O 3 -Vo/sulfite system exhibits excellent abatement performance for iohexol (IOX) with the efficiency as high as 90.2 % within 1 h of reaction at pH 8.5, in which sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) are the major species. Electrochemical and DFT calculations reveal that Vo-enriched γ-Fe 2 O 3 possesses lower electrical impedance and the concomitant higher electron transfer efficiency. According to a series of characterizations, the enhance >Fe(II)/>Fe(III) valence transformation is confirmed to contribute to sulfite activation via the regulation of the electronic structure by the Vo. In addition, the degradation pathways of IOX are proposed by analyzing the degradation products of IOX by UPLC-QTOF-MS. Finally, the effects of different influencing factors on the degradation of IOX and the cyclic performance suggest the system shows strong resistance to interference and reusability, exhibiting superior application potential.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Zixuan Zhang,Chenying Zhou,Yiming Sun,Peng Zhou,Yang Liu,Heng Zhang,Ye Du,Chuanshu He,Zhaokun Xiong,Bo Lai
Fenton oxidation technology is a widely-used advanced oxidation technology. However, the generation of hydroxyl radicals is restrained by the sluggish recovery of Fe(II), thus affecting its long-lasting performance for water decontamination. Here, a novel niobium carbide (Nb 2 C) MXene material was applied as a green co-catalyst. Nb 2 C MXene can significantly promote Fenton reactions to produce hydroxyl radicals for degrading dimethyl phthalate (DMP) with high efficiency and high stability for long-term operation, which outperforms than various reported co-catalysts. Meanwhile, the Nb 2 C/Fe(III)/H 2 O 2 system is capable of non-selectively degrading a wide spectrum of refractory pollutants. Mechanism investigation reveals that Nb 2 C MXene as an electron donor can straight reduce Fe(III), meanwhile mediate electron shuttle from Fe(II) to H 2 O 2 to strongly expedite the generation of hydroxyl radicals. In addition, four main degradation routes of DMP were proposed. Therefore, this study offers an updated and valid strategy for the refractory organic pollutants elimination by coupling Nb 2 C MXene and Fenton oxidation.
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LANGMUIR
·
2026
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IF 4.4
Yankun Wei,Dan Wang,Jinxiang Chou,Ruopeng Li,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Abstract Developing Fe–N–C electrocatalysts with high active site utilization remains a key challenge for the oxygen reduction reaction (ORR), primarily because of the limited accessibility of Fe-Nx sites. Herein, a hierarchically porous Fe–N–C (HP-Fe–N–C) catalyst is constructed via a ZnO-templated strategy combined with urea-assisted secondary pyrolysis, enabling the simultaneous regulation of the pore structure and Fe-Nx site density. The ZnO template governs the formation of mesoporous architectures, and concurrently, the pyrolysis of urea releases gaseous species that facilitate the enlargement and interconnection of mesoporous channels. Notably, the balanced micromesoporous structure derived from the ZnO template facilitates efficient mass transport and enhances site accessibility, while urea regulates the nitrogen species to promote the formation of dense Fe-Nx moieties. As a result, the HP-Fe–N–C catalyst delivers a high half-wave potential of 0.90 V, along with near four-electron selectivity and excellent durability. The Zn-air battery assembled with the HP-Fe–N–C cathode achieves an open-circuit voltage of 1.52 V, a specific capacity of 745.6 mAh g–1, and favorable charge–discharge stability exceeding 800 h. This work reveals the balance between hierarchical porosity and active site density in the Fe–N–C catalyst for the high-performance ORR.
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Inorganic Chemistry Frontiers
·
2026
·
IF 6.2
Shi-Yu Lu,Chuan Li,Longyu Qiu,Yan Zhang,Jiaming He,Minqi Liang,Xin Peng,Jun Zhang,Yin Liu,Juan Liu,Chuan Tan,Menggang Li,Meng Jin
Targeted regulation of electrocatalyst reconstruction during the oxygen evolution reaction (OER) under alkaline conditions proves essential to achieving highly efficient hydrogen production via electrochemical water splitting. Yet this remains a considerable challenge. Herein, we prepare an iron nickel phosphate (Fe-NPO) catalyst, which possesses substantial oxygen vacancies and an asymmetric Fe-O(P)-Ni coordination structure. This structural merit facilitates the effective deep reconstruction of Fe-NPO, which then transforms into the highly active Fe-Vo-P-NiOOH active phase during OER. For the reconstructed Fe-Vo-P-NiOOH, it effectively tunes the d-band center, bringing it notably closer to the Fermi level. This type of electronic modulation not only strengthens the water adsorption capacity but also optimizes the rate-determining step (RDS) in the OER pathway. The anion-exchange membrane water electrolyzer (AEMWE) integrated with the Fe-NPO catalyst as an anode catalyst achieved high industrial current densities of 500, 1000, 1500 and 2000 mA cm-2 at low applied voltages of 1.68, 1.76, 1.84 and 1.92 V, respectively. This work presents a strategy to realize the deep and efficient conversion of OER catalysts into highly active components through defect engineering and asymmetric coordination regulation, while also confirming Fe-NPO’s considerable potential for practical hydrogen production scenarios.
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Chemical Science
·
2026
·
IF 8.1
Wenlong Zhang,Xiaohui Ning
The Fe/FeCl₂-Graphite battery is an intermediate-temperature molten salt electrochemical system. It employs the solid Fe/Fe2+ redox as the negative electrode reactions and graphite positive electrode based on the intercalation/de-intercalation reaction of AlCl- 4, offering high safety, low material cost and a moderate operating temperature range of 110-150 °C. However, the poor electronic conductivity and high nucleation barrier in the FeCl2 material result in limited electrochemical reversibility and reaction kinetics. Here, we demonstrate that the Fe-FeCl₂ contact interface effectively enhances the redox reversibility and electrode kinetics by providing favorable sites for Fe⁰ nucleation and improving electronic conductivity. The prepared Fe-FeCl₂-CR electrode delivers low voltage hysteresis of 0.09 V and exhibits excellent electrochemical reversibility in the Fe/FeCl₂-graphite molten salt battery, achieving a specific capacity of 162.6 mAh g⁻¹ at 3 mA cm⁻² and retaining 93% of its capacity after 200 cycles. Compared with the pure FeCl₂ electrode, the Fe-FeCl₂-CR electrode shows lower direct‑current pulse resistance and negligible nucleation overpotential, which are primarily attributed to the Fe‑philic nucleation interface. This mechanism is further confirmed by density functional theory (DFT) calculations, revealing that the (110) crystal plane of nano‑Fe possesses the highest binding energy (-55.94 eV) during charging, thereby serving as the potential dominant interface for Fe⁰ nucleation. Additional self‑discharge and capacity expansion tests further confirm the electrochemical reaction stability of Fe-FeCl₂-CR electrode in Fe/FeCl₂-Graphite molten salt battery.
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Results in Chemistry
·
2025
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IF 4.2
Wei Zhang,Ku Yu,Wang Aihe
In this study, pyridine-a representative nitrogen-containing heterrocylic contaminant in coal chemical wastewater-was targeted for photocatalytic degradation. We developed a novel ternary composite photocatalyst through the in-situ integration of layered double hydroxide (LDH) and iron-based metal-organic framework (MIL-101(Fe)) with lanthanum‑iron co-doped TiO 2 via hydrothermal synthesis. These contaminants are characterized by high environmental persistence, low biodegradability, and potential teratogenic/carcinogenic risks. The synthesized LDH/MIL-101(Fe)/La-Fe-TiO 2 composite was systematically characterized using scanning electron microscopy (SEM), UV–Vis diffuse reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and Brunauer-Emmett-Teller (BET) analysis. Key findings revealed that: (1) The composite architecture achieves an exceptional specific surface area of 168.96 m 2 /g through synergistic LDH/MIL-101(Fe) integration; (2) La–Fe co-doping effectively extends the photoresponse threshold of TiO 2 to the visible-light region. Under optimized conditions (25 °C, 300 rpm agitation, 400 W irradiation), the system achieved 96.1 % pyridine degradation (initial concentration: 100 mg/L) within 4 h, following pseudo-first-order kinetics (R 2 = 0.99). Remarkably, the catalyst maintained 94.5 % efficiency after five consecutive cycles, demonstrating superior stability. Mechanistic investigations combining GC–MS analysis, electron paramagnetic resonance (EPR) detection, and radical quenching tests identified the reactive species activity sequence as ∙ h + > ∙ OH > O 2 − , ultimately elucidating the complete pyridine mineralization pathway.
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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 Cleaner Production
·
2023
·
IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
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APPLIED SURFACE SCIENCE
·
2023
·
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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CHEMOSPHERE
·
2023
·
IF 8.8
Chunsheng Ding,Xinze Song,Zhongyi Zheng,Hainan Wang,Yuqiang Pan,Hangtian Zhang,Xueyan Li,Jing Deng
Fe(II)-catalyzed PMS process was widely used in the degradation of refractory pollutants in wastewater, while its performance was restricted by the slow regeneration efficiency of Fe(II). Herein, caffeic acid (CFA), a representative of hydroxycinnamic acids, was introduced into Fe(III)/PMS system to accelerate the transformation of Fe(III) to Fe(II) and promote the removal of bisphenol A (BPA). Under optimum condition of 0.1 mM CFA, 0.05 mM Fe(III), and 0.5 mM PMS, almost complete removal of BPA can be achieved within 20 min, which was roughly 6.2 times higher than that in Fe(III)/PMS system. As the addition of CFA into Fe(III)/PMS system, pH application range was widened from acidic to alkaline conditions. The reduction and chelation of CFA expedited the Fe(III)/Fe(II) cycle by forming CFA-Fe chelate, thereby facilitating the PMS activation . Based on LC-MS analysis and DFT calculation, the intermediate products of CFA were found to play a decisive role in boosting the regeneration of Fe(II), and the toxicity of these intermediates towards organisms was evaluated by ECOSAR . The alcohol-scavenging and chemical probe tests certified that hydroxyl radical (•OH), sulfate radical (SO 4 •- ), and Fe(IV) coexisted in Fe(III)/CFA/PMS system, and the second-order reaction rate constants of •OH and SO 4 •- reacted with CFA were calculated to be 3.16✕10 9 and 2.30✕10 10 M −1 s −1 , respectively. Two major degradation pathways of BPA, •OH addition and SO 4 •- induced hydroxylation reaction, were proposed. This work presented a novel green phenolic compound that expedited the Fe(II)-catalyzed PMS activation process for the treatment of organic contaminants .
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