ChemCatChem
·
2022
·Vol. 14
·期 13
·e202200253
·
IF 5.497
Mingsheng Luo,Tong Qin,Qinglong Liu,Zhi Yang,Fengli Wang,Hong Li
Graphical Promoting : A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized by the hydrothermal method. The Fe-modified CeO 2 nanorod catalysts exhibit a remarkably promoting effect on the formation of DMC from CO 2 and methanol. A series of Fe-modified CeO 2 catalysts with nanoparticle, nanorod, nanocube and nano-octahedron morphologies were synthesized and applied for direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol. The Fe-modification shows a remarkably promoting effect on the formation of DMC over Fe-modified CeO 2 nanorod. The DMC yield was improved from 0.202 to 2.568 mmol DMC per g cat by 2 %Fe-modification of CeO 2 nanorod. A synergistic effect among the moderate acid-basic sites, specific surface area and surface composition resulted from Fe-modification was proposed to be crucial to obtaining the high reactivity of DMC formation.
研究领域:
催化化学
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材料科学
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环境科学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2018
·
IF 4.61
Xinyue Wang,Yingnan Sun,Lu Yang,Qingkun Shang,Dan Wang,Tongtong Guo,Yihang Guo
Photocatalysis is one of the effective strategies to eliminate various organic pollutants in water body. In this paper we have prepared a series of new composite photocatalysts to degrade phenol and norfloxacin under visible light irradiation. They were [Fe II (dpbpy) 2 (H 2 O) 2 ]/TiO 2 , [Fe II (dpbpy)(phen) 2 ]/TiO 2 and [Fe II (dpbpy)(bpy) 2 ]/TiO 2 (dpbpy: 2,2′-bipyridine-4,4′-diphosphoric acid, phen: 1,10-phenanthroline, bpy: 2,2-bipyridyl). The results show that their photocatalytic performance and cyclic stability are much better than that of pure TiO 2 or P25. Phenol can be degraded almost completely and the active groups or substituents of norfloxacin (NOR) can be destroyed also, which greatly reduced the biological toxicity of phenol and norfloxacin in water. The possible mechanisms of improving the photocatalytic activity and stability of TiO 2 by using Fe-complex are proposed based on free radical capture test and density functional theory calculation. It is clearly that the interfacial interaction between Fe-complex and titanium dioxide directly affects the photocatalytic activity and stability of the composite photocatalyst. The conjugated structure of the complexes plays a crucial role.
研究领域:
环境科学
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材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shaoqi Zhang,Haiyang Yu,Yi Wang,Yuxiang Yan,Jun Dai,Dajun Shu,Xinglong Wu
CO2 possesses extraordinary thermodynamic stability, and its reduction reaction involves multiple electron-transfer processes. Thus, high-density electron occupation on a catalyst surface is an effective driving force for improving the photocatalytic activity. Here, we report on the fabrication of Fe-doped Bi2O3 catalysts (denoted as FexBi2-xO3) with different Fe contents using the solvothermal method. The self-assembled catalyst has a nanoflower-like morphology, and its performance of CO2 reduction to CO is improved largely dependent on the Fe content. In the sample with a 7.0% Fe content (Fe0.07Bi1.93O3), the CO evolution rate reaches 30.06 μmol g–1 h–1, which is about 6 times higher than the 4.95 μmol g–1 h–1 of pristine Bi2O3, and shows excellent photostability after three cycles, with each cycle lasting for 7 h. Theoretical calculation and spectral characterization reveal that such a good CO2 reduction reaction performance arises from effective surface occupation of Fe, which not only enhances sunlight absorption but also significantly increases the surface electron density on the double metal active sites. This work provides a new strategy for improving the photocatalytic performance by surface metal doping in some metal oxide photocatalysts.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yibing Feng,Kun Qiao,Xiaohan Jiang,Huiling Ji,Jiang Meng,Jigang Wang
A photocatalysis–self-Fenton system (PSFs) offers a viable solution to the continuous hydrogen peroxide (H 2 O 2 ) dosing and insufficient Fe 2 + regeneration challenges in conventional Fenton chemistry. An oxygen-doped g-C 3 N 4 microrod (OCNT)-based PSFs was synthesized via a facile oxalic acid-mediated supramolecular self-assembly route, enabling efficient pollutant degradation. In situ H 2 O 2 production was achieved through a two-electron oxygen reduction reaction (2e − -ORR), with photogenerated electrons accelerating Fe 2+ /Fe 3+ cycling and enhancing H 2 O 2 utilization. The system exhibited an apparent rate constant of 0.071 min −1 for tetracycline (TC) removal, 12.2- and 4.2-fold higher than pristine g-C 3 N 4 and a photo-Fenton system, respectively. Density functional theory (DFT) calculations and experimental results indicated that oxygen heteroatom doping increased the molecular dipole moment and optimized the band structure, while the one-dimensional microrod morphology exposed abundant active sites. These synergistic effects facilitated charge-carrier separation, improved interfacial mass transfer, and promoted the two-electron oxygen-reduction pathway, thereby accelerating Fe 2+ /Fe 3+ cycling and hole oxidation. The platform demonstrated broad pH adaptability, strong anti-interference capability, and long-term operational stability. This work provides an effective strategy for on-site H 2 O 2 generation and utilization in photocatalytic–Fenton systems for the degradation of organic contaminants.
研究领域:
环境化学
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材料科学
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催化
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水处理技术
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物理化学
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纳米技术
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产品关联
DOI
高影响因子
ENVIRONMENT INTERNATIONAL
·
2025
·
IF 9.7
Jiaqi Shi,Yan Li,Qi Wei,Xin Zhu,Shaohua Cao,Wenyi Xie,Yang Guo,Jing Wei,Zekai Li,Tao Long
The widely used rubber antioxidant N-(1,3-Dimethylbutyl)-N’-phenyl-p-phenylenediamine (6PPD) and its ozonated product, 6PPD-quinone (6PPD-Q), are highly toxic to aquatic life, yet understanding on their environmental behaviors is limited. This study comprehensively investigated their adsorption and transformation processes on natural Fe-Mn nodules (NFMN), which commonly exist in sediments and soils through a combination of diverse experimental and computational methods. The maximum adsorption capacity of 6PPD-Q (719.2 μg·g −1 ) is significantly higher than that of 6PPD (133.8 μg·g −1 ) at 293 K, and it is more difficult to desorb. They follow different kinetic and isothermal adsorption models, and environmental conditions (including temperature, pH, and anions) exert distinct influences on the adsorption of the two substances. Adsorption mechanisms involving electrostatic attraction, charge transfer, hydrogen bonding, and Lewis acid-base complexation were unveiled. For 6PPD, electrostatic adsorption and Lewis acid-base complexation contribute significantly to its adsorption. Conversely, for 6PPD-Q, the contribution of Lewis acid-base complexation outweighs that of hydrogen bonding, while the effect of electrostatic adsorption is relatively negligible. The stronger electrostatic attraction, more efficient charge transfer, and a greater number of binding sites for hydrogen bonding and Lewis acid-base complexation with NFMN results in more robust adsorption of 6PPD-Q. Furthermore, 6PPD can transform into 6PPD-Q on NFMN, facilitated by dissolved Mn(III). This study advances understanding of the adsorption behavior and mechanism of 6PPD and 6PPD-Q, and highlights a new pathway for 6PPD-Q formation, which provides valuable reference for assessing the water body exposure risks and formulating environmental remediation strategies for such pollutants. Environmental Implication This study offers the first comprehensive insight into the interactions between 6PPD/6PPD-Q and NFMN, illuminating their environmental behavior in water and soil systems. It reveals the adsorption discrepancy between 6PPD and 6PPD-Q, and elucidates the mechanisms underlying the difference in adsorption. Additionally, it uncovers a novel pathway for 6PPD-Q formation, offering valuable implications for risk assessment and environmental remediation strategies.
研究领域:
环境科学
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化学
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产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 8
·3467-3477
·
IF 3.3
Wenhui Hu,Zhongxin Song,Lingna Sun,Lei Zhang,Qianling Zhang,Xiangzhong Ren,Yongliang Li
Efficient separation of photogenerated charge carriers is essential for maximizing the photocatalytic efficiency of semiconductor materials in oxygen evolution reactions (OER). This study presents a novel trimetallic photocatalyst, MIL-100(Fe)/TiO2/CoOx, synthesized through a facile microwave-assisted hydrothermal method followed by atomic layer deposition (ALD). The porous MIL-100(Fe) serves as a support for the sequential deposition of TiO2 and CoOx layers via ALD, which enhances electron–hole pair separation and minimizes their recombination. Characterization using transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) confirms the uniform deposition of TiO2 and CoOx layers on the MIL-100(Fe) surface. The optimized photocatalyst, processed with 20 deposition cycles of Co, exhibits exceptional photocatalytic OER performance, with an oxygen evolution rate of 558.3 μmol g−1 h−1. This enhancement in activity is attributed to the synergistic interaction between the spatially separated TiO2 and CoOx cocatalysts, which facilitates efficient charge transfer and increases the number of active sites. These findings highlight the potential of ALD-fabricated heterostructures in the development of advanced photocatalysts for sustainable energy production.
研究领域:
材料科学
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能源化学
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产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Tingting Xiang,Qingchao Zhu,Tanyu Zhou,Chenglong Chen,Ruibo Wang,Tieyu Hu,Bing Li,Ziwei Xu,Juan Yang
Graphical Fe−N−C catalysts, doped with phosphorus, show improved ORR activity. Fe-NPC catalyst exhibits high metal loading, excellent ORR performance (onset potential of 1.00 V, half-wave potential of 0.864 V), and promising application in Zn-air batteries (758.8 mAh g −1 Zn ). DFT calculations reveal that phosphorus enhances O 2 activation and reduces the energy barrier for the rate-determining step. Atomically dispersed iron and nitrogen co-doped carbon materials (Fe−N−C) represent promising non-precious metal catalysts for the oxygen reduction reaction (ORR), offering potential alternatives to noble metal-based benchmarks. In our study, we investigated the influence of phosphorus doping on the catalytic activity of Fe−N−C. The experimental research demonstrate that the doping of phosphorus significantly enhances the ORR activity. Specifically, the resulting Fe-NPC exhibits high metal loading and excellent ORR activity in 0.1 M KOH with an onset potential of 1.00 V and a half-wave potential of 0.864 V. Density functional theory (DFT) simulations reveal that phosphorus improves the electrocatalytic activity by activating O2 molecules and reducing the energy barrier (the hydrogenation reaction *OH→H2O) of the rate-determining step. Furthermore, Fe-NPC exhibits promising application prospects as an air cathode in Zn-air batteries, delivering a high maximum discharge power density of 180.3 mW cm −2 and outstanding discharge specific capacity (758.8 mAh g −1 Zn ) at a discharge current density of 10 mA cm −2 .
研究领域:
材料科学
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电化学
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催化
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产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2023
·
IF 3.9
Fengye Guo,Wenhua Li,Yefan Liu,Qianqiao Chen,Qin Zhong
Transition metal phosphides with excellent performance are one of the effective alternatives to noble metal catalysts in overall water splitting. In this paper, the Fe–NiCoP–MoO3 composite was prepared by a facile synthesis as the bifunctional electrocatalyst. Fe–NiCoP–MoO3 achieves an operating current density of 10 mA/cm2 at a low overpotential of 65 mV for hydrogen evolution reaction and drives an operating current density of 50 mA/cm2 at only 293 mV for oxygen evolution reaction. Significantly, Fe–NiCoP–MoO3 was employed as the anode and cathode for overall water splitting, which only requires a cell voltage of 1.586 V to reach 10 mA/cm2 as well as shows excellent stability. The electrocatalytic activity of Fe–NiCoP–MoO3 exceeds most of the recently reported typical bifunctional electrocatalysts. This may be due to the coupling effect between the polymetallic phosphides. In addition, heterogeneous catalysts generally expose more active sites than homogeneous catalysts. In addition, replacing MoO3 with WO3 and VO3 can also improve the performance of Fe–NiCoP. This work provides an idea for the modification of phosphides.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2019
·Vol. 9
·期 3
·288
·
IF 3.444
Feihu Liu,Zhong Wang,Da Wang,Dan Chen,Fushan Chen,Xuebing Li
The CeO2ordinary amorphous, nanopolyhedrons, nanorods, and nanocubes were prefabricated by the hydrothermal method, and employed as carriers of Fe/W–CeO2catalysts to selectively catalyze the reduction of NO with ammonia. Characterization results indicated that the morphology of CeO2support originated from selectively exposing different crystal surfaces, which has a significant effect on oxygen vacancies, acid sites and the dispersion of Fe2O3. The CeO2nanopolyhedrons catalyst (Fe/W–CeO2–P) showed most oxygen vacancies, the largest the quantity of acid sites, the largest BET (Brunauer-Emmett-Teller) surface area and the best dispersion of Fe2O3, which was associated with predominately exposing CeO2(111) planes. Consequently, the Fe/W–CeO2–P catalyst has the highest NO conversion rate in the temperature range of 100–325 °C among the ordinary amorphous, nanorods, and nanocubes Fe/W–CeO2catalysts.Keywords:morphology;Fe/W–CeO2;nanopolyhedra;CeO2(111) planes
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 14
·40534-40550
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IF 5.8
Fang Lei,Wu Guojian,Yao Keyu,Zhang Dongyang,Zhou Yongchao
A novel heterogeneous catalyst named MoS 2 /MIL-53(Fe, Cu) (MMFC) was prepared by hydrothermal method and applied in a heterogeneous electro-Fenton (hetero-EF) system for lomefloxacin (LOM) degradation in this work. Under the optimal conditions of current density 3 mA/cm 2 , catalyst dosage 0.100 g/L, and initial pH 6, 93.5% LOM (2 mg/L) removal efficiency was achieved in the MMFC hetero-EF system within 60 min, indicating an obvious improvement compared with the MIL-53(Fe, Cu) hetero-EF system. The good catalytic activity was attributed to more effective active sites of the catalyst and the conversion of Fe(II)/Fe(III) and Cu(I)/Cu(II) promoted by Mo(IV) in MoS 2 , which could be inferred by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) characterizations. The reusability and stability of MMFC were explored based on five cyclic experiments, and the average degradation efficiency reached 73.9%. Furthermore, the hetero-EF system could achieve the total removal of moxifloxacin and tetracycline within 6 min and 40 min, respectively. Quenching experiments revealed that the hydroxyl radicals (·OH) were the main reactive radicals while superoxide radicals (·O 2 − ) and singlet oxygen ( 1 O 2 ) played a certain part in LOM degradation. Finally, the possible mechanism of the hetero-EF process and LOM degradation pathways were proposed, including substitution, elimination, and cleavage of ring structures. Accounting for good catalytic performance, low preparation cost, and satisfactory versatility, the MMFC exhibited good potential to work as a hetero-EF catalyst for wastewater treatment.
研究领域:
环境科学
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化学工程
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材料科学
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废水处理
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产品关联
DOI
PubMed
高影响因子
Frontiers of Environmental Science & Engineering
·
2025
·Vol. 19
·期 12
·1-17
·
IF 6.4
Wei Biao,Liu Daoqing,Peng Ran,Zhou Yi,Li Qianwei,Zhao Huazhang
The remediation of nitroaromatic-contaminated water systems remains a critical environmental challenge, creating the urgent need for cost-effective, non-precious metal catalysts to increase wastewater biodegradability. In this study, we present an Fe/N-functionalized three-dimensional porous carbon (Fe–N–C) catalyst synthesized via a straightforward pyrolysis approach that enables efficient nitrobenzene (NB) degradation via electrochemical and chemical reduction pathways. The high-temperature pyrolysis process facilitates the iron-catalyzed reconstruction of the carbon matrix, resulting in a hierarchically porous structure with increased graphitization and uniformly distributed macrocyclic Fe–N 4 coordination sites. These structural features give the Fe–N–C catalyst exceptional electron transfer kinetics, catalytic activity, and pH adaptability, surpassing conventional graphite (GR) and nitrogen-doped carbons (NPCs) in NB reduction. Systematic evaluation of the electrochemical reduction performance revealed that the Fe–N–C electrode achieved the highest NB removal efficiency. To further assess the versatility of the catalyst, a functionalized Fe–N–C/zero-valent iron (ZVI) composite was engineered by integrating Fe–N–C as a catalytic layer onto the reductant ZVI. Compared with ZVI alone, this composite markedly increased the NB reduction efficiency. These findings provide valuable insights into the electrochemical reduction process of Fe–N–C and new directions for the rational design of efficient nitrobenzene reduction systems.
研究领域:
环境科学
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材料科学
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电化学
·
催化
·
水处理
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Si-Jia Guan,Peng Zhang,Shen-Jing Ji,Yu Cao,Nian-Tzu Suen
It is well known that the “iron” impurity will influence the oxygen evolution reaction (OER) in an alkaline electrolyte, especially for the Ni-based electrocatalyst. Many research studies have investigated the function of Fe in the OER active phase, such as M(OH)2/MOOH (M = Ni and/or Fe), while, surprisingly, very few studies have examined the function of Fe in the “precatalyst” system. Accordingly, in this work, the Ni3–xFexP (x = 0, 0.5, 1) series as an Ni-based precatalyst was employed to inspect the function of internal and external Fe in the Ni-based precatalyst system. It was realized that the sample with internal Fe (i.e., Ni2.5Fe0.5P and Ni2FeP) exhibits efficient OER activity compared to that of the Fe-free one (i.e., Ni3P) owing to the large amount of active M(OH)2/MOOH formed on the surface. This indicates that the internal Fe in the present system may have the ability to facilitate the phase transformation; it was later rationalized from electronic structural calculations that the d band center of the internal Fe (middle transition metal) and Ni (late transition metal) holds the key for this observation. Adding excessive ferrous chloride tetrahydrate (FeCl2·4H2O) as the external Fe in the electrolyte will greatly improve the OER performances for Ni3P; nevertheless, that the OER activity of Ni2FeP is still much superior than that of Ni3P corroborates the fact that the Fe impurity is not the only reason for the elevated OER activity of Ni2FeP and that internal Fe is also critical to the phase transformation as well as OER performance.
研究领域:
电化学
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材料科学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）