RSC Advances
·
2017
·Vol. 7
·期 84
·53622-53630
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IF 3.108
Changming Li,Hong Zeng,Pingle Liu,Jian Yu,Feng Guo,Guangwen Xu,Zhan-guo Zhang
The development of new routes for the utilization of red mud (RM) waste is very urgent due to its huge accumulation and potential environmental harm. By taking advantage of its Fe–Al–Si–Ti composition and excellent plasticity, we developed a ball milling and acid–base neutralization method to reuse the RM waste as Fe-based denitration catalysts. The resulting RM catalysts demonstrate excellent catalytic activity and stability with >90% NO conversion above 400 °C in the presence of SO2 and H2O, which is even much better than that of a commercial V–W–Ti catalyst. Characterization data reveal that our treatment eliminates poisonous alkaline metal elements and increases dispersion of RM particles, making the RM active for denitration reactions. The formation of ferric sulfate species with more reducible Fe3+/Fe2+ active sites by a SO2 activation method can further enhance the denitration activity. Moreover, NH3-TPD and in situ IR results demonstrate that the NH3-SCR reaction over the RM catalyst follows the Eley–Rideal mechanism at high temperature and the increased absorption of NH3 for alkaline metal-eliminated or SO2-activated samples accounts for its high DeNOx efficiency. The demonstrated feasibility for reusage of the RM as DeNOx catalyst has promising industrial prospects for its extremely low cost, no toxicity, and high efficiency.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·
IF 3.7
Yi Jing Jia,Jin Quan Tao,Hao Ran Liu,Wen Bin Huang,Rongpeng Yao,Miaomiao Niu,Rongrong Li,Qiang Wei,Ya Song Zhou
To enhance the CO 2 hydrogenation activity and low-carbon olefin selectivity of Fe-based catalysts, a strategy involving the use of metal promoters to modulate the structure of active metal centers in catalyst preparation was proposed. The incipient wetness impregnation method was used to introduce modifying agents K and/or Co into the Fe/Al 2 O 3 catalyst. Characterization techniques such as XRD, BET, SEM, HRTEM, H 2 -TPR, XPS, CO 2 -TPD, NH 3 -TPD, and TG were employed to investigate the effects of the modifying agents on the dispersion, reducibility, electronic properties, and acid–base properties of active metal species. Furthermore, the influence of K and Co modification on the CO 2 hydrogenation activity and low-carbon olefin selectivity of Fe/Al 2 O 3 catalysts was explored. The results revealed that the introduction of K generated more basic sites and electron-rich active metal centers in the catalyst, facilitating the adsorption and activation of CO 2 , while suppressing the hydrogenation of olefins and the formation of methane, thus improving the selectivity towards low-carbon olefins. Co promoter facilitated the dispersion of Fe species, exposing more active sites and enhancing the FTS reaction activity, leading to more CO being converted into C 2+ hydrocarbon products. Under the synergistic effect of K and Co, the CO 2 conversion activity of the Fe-based catalyst significantly increased, achieving a CO 2 conversion rate of 37%, while the selectivity towards C 2 -C 4= increased to 31.9%.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 11
·3383-3391
·
IF 2.936
Zhang Luping,Tu Xuewei,Han Weihang,Chen Liangchen,Chen Yutong,Zheng Hui
As the main resource of greenhouse gas, CO 2 needs to be fixed into different chemicals to relieve the environmental problem. Fe-based catalyst and g-C 3 N 4 have received extensive attention due to their easy preparation, low cost, and environmental friendliness. Herein, a heterogeneous catalyst system consisting of rich-electron g-C 3 N 4 and strong electron-withdrawing groups Fe-complex [Fe(bpy)(CO) 2 (Cl) 2 ] was developed, which could promote electron transfer and enhance the electronic interaction for fixing CO 2 . o -phenylenediamine substrates with different electron-donating/withdrawing groups were employed to fix CO 2 into high-valued heterocycle benzimidazoles. The optimum reaction conditions were examined by orthogonal experiments. A series of benzimidazole derivatives were synthesized with yield up to 98%, which indicated the catalyst had the ability of fixing CO 2 . This catalyst provides a new pathway for fixing CO 2 into valuable benzimidazole derivatives. Graphical Abstract
研究领域:
化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Haripal Singh Malhi,Zhenzhou Zhang,Yanling Shi,Xinhua Gao,Wenqi Liu,Weifeng Tu,Yi-Fan Han
The multi-walled carbon nanotubes (MWNTs) supported Fe-based catalysts, including FeZnNa/MWNTs, FeZnK/MWNTs, and FeZnRb/MWNTs were synthesized through co-precipitation, and incipient wetness impregnation approaches. The physicochemical results demonstrated that the addition of MWNTs had significantly influenced the morphology, reduction, phase structure, adsorption behavior of Fe-based catalysts, and consequently, the reactivity of CO 2 hydrogenation to olefins. Furthermore, adding MWNTs to the alkali metal-promoted FeZn catalysts inhibits the synthesis of CH 4 and CO and favors an improved selectivity for olefins. With the incorporation of MWNTs, the heavy olefins (C 5- C 8 = ) selectivity over FeZnNa, FeZnK, and FeZnRb catalysts increased from 27.1 to 32.2, 27.0–31.1, and 24.2–28.6 %, respectively. The results proved that the superior selectivity of heavy olefin over the MWNTs-supported catalysts might be accomplished by the electron-donating ability of the MWNTs surface, the presence of extra Hägg carbide, and higher adsorption strength with light olefins. In addition, the catalyst supported by MWNTs demonstrated exceptional stability throughout the 100-hour test at 593 K.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
IF 4.3
Ruosong He,Yang Wang,Meng Li,Jianxin Liu,Yongqiang Gu,Wenhang Wang,Qiang Liu,Noritatsu Tsubaki,Mingbo Wu
Graphical Core-shell structured Fe-based catalyst Na−Fe 3 O 4 @C with confinement effect delivered higher productivity of light olefins compared with the naked Na−Fe 2 O 3 counterpart. Multiple characterization and DFT calculation verified that the timely carbon chain-growth termination, as well as unique CO 2 /H 2 ratio and electronic property on the catalytic interface played vital roles in boosting light olefins synthesis. Even though Fe-based catalysts have been widely employed for CO 2 hydrogenation into hydrocarbons, oxygenates, liquid fuels, etc., the precise regulation of their physicochemical properties is needed to enhance the catalytic performance. Herein, under the guidance of the traditional concept in heterogeneous catalysis-confinement effect, a core-shell structured catalyst Na−Fe 3 O 4 @C is constructed to boost the CO 2 hydrogenation performance. Benefiting from the carbon-chain growth limitation, tailorable H 2 /CO 2 ratio on the catalytic interface, and unique electronic property that all endowed by the confinement effect, the selectivity and space-time yield of light olefins (C 2 = −C 4 = ) are as high as 47.4 % and 15.9 g mol Fe −1 h −1 , respectively, which are all notably higher than that from the shell-less counterpart. The function mechanism of the confinement effect in Fe-based catalysts are clarified in detail by multiple characterization and density functional theory (DFT). This work may offer a new prospect for the rational design of CO 2 hydrogenation catalyst.
研究领域:
催化化学
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材料科学
·
能源化学
✓ 已验证
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2025
·
IF 4.2
ChengBo Qian,Yuyuan Yao,Hongliang Zhu
Fe-based catalysts have garnered significant attention due to their high stability, low toxicity and cost-effectiveness, while the construction of highly active heterogeneous Fe-based catalysts through a simple method is still challenging in the environmental catalysis field. Herein, employing the synergistic enhancement effect of the conductive polymer polyaniline (PANI) and co-catalyst MoS2, a highly active PANI-supported Fe-doped MoS2 catalyst (PANI-Fe@MoS2) was prepared via a facile one-step hydrothermal process. Surprisingly, PANI incorporation induced critical structural modifications, including reduced average particle size (1 μm), expanded interlayer spacing (1.09 nm), and enhanced sulfur vacancy density. Interestingly, PANI-Fe@MoS2 achieved nearly 100% elimination of carbamazepine (CBZ) within 10 min, and its removal efficiency (k-value) surpassed most of those reported in the literature. Notably, PANI-Fe@MoS2 exhibited a high removal of TOC (nearly 50%), a wide pH operating range (2–10), and outstanding removal efficiency for various contaminants. Additionally, the quenching and electron paramagnetic resonance (EPR) experiments revealed that singlet oxygen (1O2) and hydroxyl radicals (˙OH) were the main reactive oxygen species (ROSs) for degrading CBZ. Moreover, the potential degradation pathways were proposed based on the intermediates of CBZ. This work provides a strategic paradigm for designing efficient heterogeneous Fe-based catalysts for environmental remediation.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2017
·
IF 4.208
Xufang Li,Weiyu Chen,Luming Ma,Hongwu Wang,Jinhong Fan
An Fe-based catalyst was used as a heterogeneous catalyst for the ozonation of industrial wastewater , and key operational parameters (pH and catalyst dosage) were studied. The results indicated that the Fe-based catalyst significantly improved the mineralization of organic pollutants in wastewater. TOC (total organic carbon) removal was high, at 78.7%, with a catalyst concentration of 200 g/L, but only 31.6% with ozonation alone. The Fe-based catalyst significantly promoted ozone decomposition by 70% in aqueous solution. Hydroxyl radicals (·OH) were confirmed to be existed directly via EPR (electron paramagnetic resonance) experiments, and ·OH were verified to account for about 34.4% of TOC removal with NaHCO 3 as a radical scavenger. Through characterization by SEM-EDS (field emission scanning electron microscope with energy-dispersive spectrometer), XRD (X-ray powder diffraction) and XPS (X-ray photoelectron spectroscopy), it was deduced that FeOOH on the surface of the catalyst was the dominant contributor to the catalytic efficiency. The catalyst was certified as having good stability and excellent reusability based on 50 successive operations and could be used as a filler simultaneously. Thereby, it is a promising catalyst for practical industrial wastewater advanced treatment.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Siyuan Zhu,Jun Ke,Zhongnan Chen,Zhaoyang Yan,Lulu Zhao,Xinhong Qiu
Secondary aluminum dross (SAD) as a hazardous waste has been widely studied on recycling by acid leaching process, but residues accounting for approximately 50 wt% of SAD are still produced and rarely reused. In this study, residues from secondary aluminum dross are retrieved to fabricate Fe-based acidized aluminum ash sludge (FAS) heterojunction catalyst for photocatalytic degrading tetracycline hydrochloride under visible light, which does not only reduce resource utilization cost of SAD, but also realize efficient wastewater treatment by clean photocatalytic technique. Firstly, acidized sludge was obtained from SAD via an acid leaching and then utilized to fabricate FAS by calcination method. From the results of characterizations, BaFeO 3-x and Fe 2 O 3 were demonstrated to be deposited on the surface of acidized sludge, resulting in the successful formation of FAS heterojunction catalyst. As a result, the FAS exhibits an excellent performance in the removal of tetracycline hydrochloride (TCH), reaching to 92.2 % within 150 min under dark adsorption and visible light excitation. To further broaden the application of FAS in actual circumstance, the degradation of mixed dye in wastewater and actual medical wastewater were conducted over the optimal sample of FAS. After four cycles, the removal ability remained at 86.0 %, which shows the exceptional stability.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Tianyue Su,Chun Cai
Heterogeneous catalysts have recently regarded as a promising chose for the thermally-driven generation of the reactive oxygen species (ROS) through catalytic reactions with molecular oxygen , which can facilitate this process by specific geometric and electronic structure. However, the oxidative trifluoromethylation of alkenes to α-trifluoromethylated ketones by CF 3 SO 2 Na is rarely reported in this system. In this work, we report a one-pot polymerization ball milling strategy to construct precursor, and then pyrolyze it to obtain specific carbon nanotubes matrix with Fe/Fe 3 O 4 nanoparticles and single atoms Fe. Remarkably, the optimized catalyst (Fe 3 O 4 -Fe SAs - NPs @NC-1) displays excellent catalytic performance, broad substrates and recyclability for this fluorination reaction via radical pathway. Based on characterizations and mechanistic studies , we discover that the coexistence of Fe/Fe 3 O 4 and Fe-N x not only synergistically facilitates the catalytic efficiency in altering the electronic structure of Fe sites, but also benefits the absorption of O 2 and the ability of the thermally-driven generating ROS which can activate CF 3 SO 2 Na to CF 3 radical. This work offers a method of designing Fe-based catalysts and also opens up a new thermal-heterogeneous catalysis way for the oxidative trifluoromethylation of alkenes .
研究领域:
化学
·
催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Rongji Cui,Suxia Ma,Jie Wang,Shujun Sun
The catalytic gas-phase H 2 O 2 oxidation of NO was achieved over Fe-based catalysts supported on montmorillonite K10, γ-alumina and ZSM-5. ESR tests illustrate that the three catalysts can catalyze decomposition of H 2 O 2 yielding highly reactive hydroxyl radicals , of which Fe/K10 has the fastest rate, followed by Fe/γ-alumina. Fe 3+ in Fe/K10 and Fe/γ-alumina show lower density of electron cloud due to a strong interaction between Fe 3+ and the support, which benefits the electron transfer from the H 2 O 2 to Fe 3+ , thus favoring the production of hydroxyl radicals. Fe species exist on the surface of Fe/K10 mainly in the form of Fe 2 O 3 , whereas Fe species of Fe/γ-alumina and Fe/ZSM-5 exist mainly in the form of Fe 3 O 4 , and it is found that Fe 2 O 3 is more active than Fe 3 O 4 in catalytic gas-phase H 2 O 2 oxidation of NO. Interestingly, Fe/ZSM-5 has the lowest efficiency in generating hydroxyl radicals, its NO removal efficiency is 90%, which is much higher than 47.5% for Fe/γ-alumina and 62.3% for Fe/K10. In-situ IR results suggested that Fe/ZSM-5 are dual functional in oxidation of NO, that is, whether both Fe ion sites and Brønsted acid sites collectively provide the catalytic functionality. In the meantime, a possible reaction mechanism on catalytic gas-phase H 2 O 2 oxidation of NO over Brønsted acid sites is proposed.
研究领域:
环境科学
·
催化化学
✓ 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）