LANGMUIR
·
2024
·
IF 3.7
Zeqi Wu,Feng Niu,Wenhao Yao,Siyuan Gao,Da Chen,Yuexiang Huang
The activation of an inert C(sp3)–H bond in selective oxidation of hydrocarbons under mild conditions is a critical and challenging process. Herein, we report a stable chlorine-coordinated metal–organic framework (MOF) photocatalyst, MIL-101(Fe), for efficient visible-light-driven photocatalytic selective oxidation of toluene to benzaldehyde in air under ambient conditions. Encouragingly, a benzaldehyde formation yield of 3.11 mmol·g–1·h–1 with a selectivity of 92.1% is achieved in 5 h, which is superior to most of the reported works. Based on the experimental results and characterizations, the high catalytic performance is mainly due to the promoted rate-limiting step of C(sp3)–H bond activation by a chlorine radical (Cl·) from the coordinated −Cl in the MIL-101(Fe) structure. In addition, the present photocatalyst possesses good substrate tolerance for photocatalytic selective oxidation of various toluene derivatives under optimized conditions.
研究领域:
化学
·
材料科学
·
环境科学
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DOI
PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 17
·4194
·
IF 4.2
Kaiwei Ding,Tingsheng Qiu,Xianhui Qiu,Guanfei Zhao,Qinghao Jiao,Jiangjie Fang,Ruisen Lai,Wenhui Yang
The floatability of fluorite and calcite exhibit similar properties, rendering their flotation separation challenging. Macromolecular polysaccharide reagents containing the polyhydroxyl group have shown broad promising application. The selectivity of polysaccharide is relatively low. In this study, the introduction of Fe3+was employed to enhance the selective adsorption capacity of Pullulan polysaccharide towards fluorite and calcite minerals, thereby achieving effective flotation separation. Furthermore, the mechanism underlying intramolecular interactions was elucidated. The DFT calculation and XPS analysis revealed that the adsorption of Fe3+on the calcite surface was more favorable, leading to the formation of a Ca-O-Fe structure. The MD simulation, XPS analysis, and Zeta potential analysis revealed that the Fe-OH groups on the surface of calcite reacted with the -OH groups in Pullulan and formed bonds, resulting in the formation of a Calcite-Fe-Pullulan structure. This facilitated the attachment of a significant number of Pullulan molecules to the calcite surface. The formation of a hydrophilic layer on the outer surface of calcite by Pullulan, in contrast to the absence of such layer on fluorite’s surface, results in an increased disparity in surface floatability between these two minerals, thereby enhancing the efficiency of flotation separation.
研究领域:
矿物学
·
表面化学
·
分子动力学模拟
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DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Xiuying Zhu,Mengjie Li,Xiong-Fei Zhang,Jianfeng Yao
Iron-based metal-organic framework (MIL-100) with intrinsic high surface area and low cost is extremely attractive in the field of organic pollutant remediation. Herein, delignified balsa wood is utilized as substrate/support for the in situ growth and dispersion of MIL-100 particles. Results demonstrate that the MIL-100 particles adhere tightly to the support and a hierarchal architecture is constructed. The MIL-100@Wood composite can be used as adsorbent and filter for the alleviation of organic contamination. With 25.4 wt% of MIL-100 loading, the MIL-100 decorated delignified wood (MD-Wood) exhibits a tetracycline (TC) adsorption capacity of 109.9 mg/g. The composite MD-Wood can be easily fabricated into an all-in-one filter and this filter presents an effective treatable volume of 1100 mL of TC solution (20 mg/L). The MD-Wood is further deposited with Ag particles and the Ag@MD-Wood can be directly applied for the flow catalytic reduction of 4-nitrophenol. Moreover, the composite woods are facile to regenerate and possess superior reusability and stability.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2015
·Vol. 23
·期 7
·6758-6766
·
IF 2.828
Fu Xiaori,Gu Xiaogang,Lu Shuguang,Miao Zhouwei,Xu Minhui,Zhang Xiang,Danish Muhammad,Cui Hang,Farooq Usman,Qiu Zhaofu,Sui Qian
Effective degradation of benzene was achieved in sodium percarbonate (SPC)/Fe(II)-Glu system. The presence of glutamate (Glu) could enhance the regeneration of Fe(III) to Fe(II), which ensures the benzene degradation efficiency at wider pH range and eliminate the influence of HCO 3
− in low concentration. Meanwhile, the significant scavenging effects of high HCO 3
− concentration could also be overcome by increasing the Glu/SPC/Fe(II)/benzene molar ratio. Free radical probe compound tests, free radical scavenger tests, and electron paramagnetic resonance (EPR) analysis were conducted to explore the reaction mechanism for benzene degradation, in which hydroxyl radical (HO•) and superoxide anion radical (O 2
•− ) were confirmed as the predominant species responsible for benzene degradation. In addition, the results obtained in actual groundwater test strongly indicated that SPC/Fe(II)-Glu system is applicable for the remediation of benzene-contaminated groundwater in practice.
研究领域:
环境科学
·
化学工程
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Qiaoyuan Gao,Dagang Lin,Yongjie Fan,Qin He,Qi Wang
Visible-light-active Fe-2MI assemblies were prepared at room temperature using 2-Methylimidazole (2MI) as organic ligand to form complex with Fe(II) or Fe(III). TGA and XRD characterizations indicated that Fe(II) can form more stable complex and higher coordinating percentage with 2MI relative to Fe(III). Besides, Fe(II)-2MI displayed amorphous state with larger BET surface area and higher photocurrent response. At very low catalyst dosage (0.1 g/L), highest activity for Cr(VI) reduction can be achieved using Fe(II)-2MI as photocatalyst. The estimated pseudo-first-order rate constant (0.021 min −1 ) was 1.4 and 2.1 times that on Fe(III)-2MI and Fe(II)-NaOH, respectively. The well-known ZIF-67 (Co-2MI), ZIF-7 (Zn-2MI) and Fe-MOFs with other organic ligands (H 2 BDC, NH 2 -H 2 BDC or FA) were also used as control samples. Optimal activity for photocatalytic reduction of Cr(VI) was achieved by Fe(II)-2MI. The operating factors was optimized at acidic pH (2.0), higher catalyst dosage (0.3 g/L) and appropriate concentration of coexisting organics (2.0 mM) within the tested range. The stability of Fe(II)-2MI was investigated at different pH values (2, 3 and 4.64), which all displayed good stability. Mechanism study indicated that Fe(II)-2MI has adequate conduction and valence band positions for Cr(VI) reduction and organics oxidation, respectively. Therefore, the as-prepared amorphous Fe(II)-2MI assemblies may be cheap, stable and easy available candidate for the photocatalytic disposal of Cr(VI)-containing wastewaters.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
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
·
材料科学
·
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
·
材料科学
·
化学
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DOI
PubMed
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
·
化学
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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
·
材料科学
·
催化
·
水处理技术
·
物理化学
·
纳米技术
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产品关联
DOI
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
·
能源化学
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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
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DOI
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
·
电化学
·
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）