JOURNAL OF CATALYSIS
·
2017
·
IF 6.844
Chuande Huang,Yanyan Zhu,Xiaodong Wang,Xin Liu,Junhu Wang,Tao Zhang
A series of BaFe 1− x Sn x O 3− δ catalysts were prepared by sol-gel method and tested for N 2 O decomposition to shed light on the effect of B-site substitution on the catalytic behavior of perovskite catalysts. 119 Sn and 57 Fe Mössbauer results confirmed that the 5-fold coordinated Fe 3+ cations with one adjacent oxygen vacancy (Fe 3+ O 5 ) were the main active centers for N 2 O decomposition. Doping of Sn cations can significantly improve the percentage of Fe 3+ O 5 from 30% ( x = 0) to 68% ( x = 0.8). More importantly, the valence state of Fe could be gradually reduced due to weakening of Fe O bond with increasing the Sn content, which was attributed to the stronger force of Sn than Fe in Fe O Sn structure to draw the oxygen anion and expansion of unit cell volume. Such change of Fe chemical state favored the oxygen mobility of the catalyst, leading to reduction in activation energy for N 2 O decomposition from ca. 241 ( x = 0) to 178 kJ mol −1 ( x = 0.8). BaFe 0.2 Sn 0.8 O 3− δ catalyst exhibited the highest intrinsic rate of 1.49 s −1 (550 °C), nearly 4 times larger than that of BaFeO 3− δ (0.43 s −1 ).
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Zhiwen Xu,Lanlu Lu,Weiwei Chen,Fei Yang,Guimei Liu,Yan Sun,Xiaoyi Qiu,M. Danny Gu,Ping Gao,Dong Su,Minhua Shao
Although zinc-air batteries (ZABs) have made great progress in recent years, there still a great challenge to develop low-cost bifunctional electrocatalysts with high catalytic activity and stability. Herein, we report a bifunctional oxygen electrocatalyst consisting of ZIF-derived carbon-anchored Fe/Fe 3 C nanoparticles and Fe single atoms, which are crosslinked by carbon nanotubes (denoted as CNT@Fe/Fe 3 C||FeNC). Benefiting from the synergetic effect of Fe/Fe 3 C nanoparticles, Fe-N 4 active sites, and the 3D interpenetrating network structure, CNT@Fe/Fe 3 C||FeNC shows excellent bifunctional catalytic activities with a low ΔE of 0.671 V. Furthermore, the assembled rechargeable ZAB demonstrates a high peak power density of 187 mW cm –2 and shows excellent cycling stability up to 600 h This work provides new ideas for constructing non-precious metal bifunctional catalysts for practical applications in ZABs.
研究领域:
材料科学
·
电化学
·
能源存储与转换
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DOI
高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2024
·
IF 3.9
Boyu Du,Nan Jiang,Zengbin Chai,Chao Liu,Xing Zhu
DETA-Fe-BTC MOFs with an irregular porous structure is fabricated by a hydrothermal method combining with Diethylenetriamine (DETA) modification and investigated in batch adsorption experiments for arsenic removal from wastewater. DETA-Fe-BTC show high adsorption ability in wide pHs ranged from 2 to 12 and a wide arsenic concentration range from 1 mg/L to 1000 mg/L. The maximal arsenic adsorption capacity reaches 1748.50 mg/g at a pH of 10. Besides, the MOFs reveal a super-fast arsenic-removal rate. 90.58 % of arsenic was removed from wastewater with an initial arsenic concentration of 40 mg/L in 5 s. Arsenic adsorption kinetics and isotherms follow a chemical adsorption mode and a single-molecule adsorption mode that the MOFs offer abundant Fe 3+ active cites forming Fe-O-As coordination with arsenate or arsenite. Considering its strong recyclability and high efficiency, DETA-Fe-BTC will be used as a potential arsenic scavenger for the disposal of arsenic contaminated groundwater or industrial wastewater.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 20
·9185-9195
·
IF 2.7
Shikai Xue,Dongying Zhu,Qing Zuo,Shuangfeng Yang,Haiyan Wang,Qiujun Lu,Guoxing Yin,Guihua Ruan,Fuyou Du
A novel MIL-101(Fe)/ZnCrZr-LBMO heterojunction was successfully constructed and used for the removal of ciprofloxacin (CIP) in this work. The MIL-101(Fe)/ZnCrZr-LBMO composite exhibited significantly enhanced photocatalytic degradation activity, with reaction rates approximately 3.4 and 3.1 times faster than those observed with pristine MIL-101(Fe) and ZnCrZr-LBMO, respectively. The effect of different amounts of ZnCrZr-LBMO, sample pH, CIP concentration, inorganic cations, and anions on CIP removal was investigated, and the possible intermediates and degradation pathways of CIP were speculated. The·O2− radicals dominated CIP degradation, with minor contributions from 1O2, h+, and ·OH radicals. The composite exhibited high removal rates for CIP (94.7%), ofloxacin (86.8%), and tetracycline (96.3%), respectively, within 60 min of light irradiation, and excellent reusability, retaining over 85.1% CIP degradation rate after five cycles. Our work provides a new reference to construct highly efficient and easily recyclable MIL-101(Fe)/ZnCrZr-LBMO photocatalysts for the removal of antibiotic pollutants, promising advancements in real water treatment applications.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
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
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环境科学
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产品关联
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
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表面化学
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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
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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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产品关联
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
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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
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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
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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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
·
能源化学
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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）