RSC Advances
·
2023
·Vol. 13
·期 20
·13902-13910
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IF 3.9
Jing Tian,Weixin Qian,Haitao Zhang,Hongfang Ma,Weiyong Ying
In this paper, catalysts with different aluminum contents were prepared by a co-precipitation method using LDHs (layered double hydroxides) as the precursors through the adjustment of Cu2+ : Fe2+, and the catalysts were named LDO catalysts. The effect of aluminum on CO2 hydrogenation to methanol was investigated by evaluating the characterization. With the addition of Al, Ar physisorption results showed an increase in BET-specific surface area, TEM demonstrated a decrease in catalyst particle diameter, XRD showed that Cu and Fe existed in the catalyst mainly in the form of CuFe2O4 and CuO, XPS demonstrated a decrease in electron cloud density and an increase in base sites and oxygen vacancies, and CO2-TPD and H2-TPD results indicated that Al promoted the dissociation and adsorption of CO2 and H2. When the reaction temperature was 230 °C, the pressure was 4 MPa, H2/CO2 = 2.5 and the space velocity was 2000 ml (h gcat)−1, the best conversion (14.87%) and the highest methanol selectivity (39.53%) of the catalyst were obtained at 30% aluminum content.
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FUEL PROCESSING TECHNOLOGY
·
2021
·
IF 7.033
Enkang Fu,Yu Qiu,Huaichang Lu,Sijun Wang,Lishan Liu,Hanjun Feng,Yanxin Yang,Zizhan Wu,Yunlong Xie,Feng Gong,Rui Xiao
Ammonia (NH 3 ) has been regarded as an attractive energy source for hydrogen production via catalytic decomposition , especially over non-noble metal catalysts . Owing to the decent performance and low cost, nickel (Ni) based catalysts have been widely studied for catalytic decomposition of NH 3 where the decomposition rates, can be further tailored by adding other metals. Herein, we synthesized bimetallic M(M = Co, Fe, Cu)Ni/Al 2 O 3 catalysts delivering superior catalytic performance at a wide temperature range of 350–750 °C. Co-Ni/Al 2 O 3 demonstrated nearly 100% conversion of NH 3 decomposition to H 2 at 700 °C and the gas hourly space velocity of 30,000 ml g −1 min −1 , which was ~20.85% higher than that of intrinsic Ni/Al 2 O 3 . The structural characterizations indicated that Co could decrease the particle size and enhance the dispersion of active sites. The density functional theory calculations substantiated that the associative decomposition of N to generate N 2 was the rate-determining step of the NH 3 decomposition reactions . NH 3 Temperature Programmed Desorption (TPD) results suggested that the enhanced catalytic performance was predominantly attributed to the Co that decreases the energy barrier for the associative decomposition of N to form N 2 . This study provides new insights in designing diverse catalysts for efficient NH 3 decomposition for controllable H 2 production.
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CATALYSIS COMMUNICATIONS
·
2008
·
IF 2.394
Yunlai Ren,Zhifei Liu,Shuang Zhao,Xinzhe Tian,Jianji Wang,Weiping Yin,Shebin He
Commercially available and inexpensive ethylenediamine/Cu(OAc) 2 · H 2 O has been found to be a highly effective catalyst system for the cyanation of aryl bromides in the solvent of NMP. At the same time, the highly activated aryl chlorides with NO 2 groups gave corresponding benzonitriles in good yields. Similar to the previous observation, it is not necessary to use an excess of K 4 [Fe(CN) 6 ] in the cyanation reaction (only 20 mol% of K 4 [Fe(CN) 6 ] was used). In other hand, a more remarkable KI-accelerated effect was observed for the cyanation reaction: the addition of KI increased the yield from 6% to 91% in the cyanation of bromobenzene.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Jie Wang,Yumei Chen,Shuyan Guan,Jianchao Shi,Mingbin Li,Baozhong Liu
Hydrolytic dehydrogenation of ammonia borane (AB) has attracted much attention due to its high hydrogen content and stability. Therefore, the design and construction of low-cost and high-performance catalysts for AB hydrolysis are of great significance. In this work, Co/CoFeO x -X (X is the additional content of Fe precursor) bimetallic oxide nanofilms having an amorphous structure were prepared on an (IL)/water interface for the hydrolysis of AB. Strategies including the rapid addition of metal precursors and variation of Co/Fe atom ratios were employed to induce an amorphous structure for inhibiting the rearrangement of the formed metal nuclei and optimizing the alloying effect on the IL/water interface. This ultrathin amorphous nanofilm structure can expose more metal active sites. Moreover, the electronic interaction between Fe and Co after doping Fe into the Co/CoO x nanofilms facilitates the adsorption and activation for AB and H 2 O molecules. As a result, the optimized Co/CoFeO x -25 catalyst exhibits excellent catalytic activity with a turnover frequency (TOF) value of 12.25 mol H2 ·mol Co –1 ·min –1 , which is considerably higher than that of the monometallic Co/CoO x catalyst. This enhanced activity can be ascribed to the morphology advantages and the electronic effect of Fe and Co on the Co/CoFeO x -25 catalyst. This work provides a promising method to design the highly efficient non-noble metal catalysts for the hydrolysis of chemical hydrides.
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JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Zhihao Shen,Shuming Wen,Yongchao Miao,Han Wang,Qicheng Feng
Unavoidable metal ions commonly exist in the pulp during flotation. These ions can affect the floatability of minerals, and they can also result in the differences in the surface features between different minerals. In this study, how Fe 3+ affected the flotation behavior of cerussite was investigated by micro-flotation tests. The corresponding adsorption characteristics of the sulfidizing agent and collector on the surfaces of cerussite were investigated by surface-analysis techniques. The results of micro-flotation tests showed that the floatability of cerussite significantly decreased when Fe 3+ was added before Na 2 S and xanthate. The flotation recovery of cerussite decreased compared with that obtained without participation of Fe 3+ . Additionally, the results of xanthate and Na 2 S adsorption tests, X-ray photoelectron spectroscopy (XPS), time-of-flight secondary ion mass spectrometry (ToF-SIMS) and zeta potential measurements verified that Fe 3+ and its hydrophilic hydroxyl derivatives (Fe-OH compounds) resulted in reduced amounts and reactive activities of S-bearing species adsorbed on the surfaces of cerussite. This decreased the adsorption capacity of subsequently added xanthate, resulting in the difficulty in effectively recovering cerussite in the sulfidization-xanthate system.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 56
·84166-84179
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IF 5.19
Gao Panting,Li Yuran,Lin Yuting,Chang Liping,Zhu Tingyu
Catalytic hydrolysis of carbonyl sulfur (COS) from blast furnace gas is one of the keys to achieving ultra-low emission in the iron–steel industry. To improve the COS hydrolysis activity on γ-Al 2 O 3 catalyst at low temperature, catalysts with Fe or La as the active component were prepared by the impregnation method, the physical and chemical properties of the catalyst were characterized by ICP, XRF, XRD, BET, and TPD. The hydrolysis activity of COS and sulfur resistance ability on various catalysts were investigated in a fixed bed reactor combined with gas chromatography. The results show that the addition of Fe or La improves the COS hydrolysis activity due to the increase in alkaline sites on the catalyst surface. The roles of various alkaline sites on catalysts have been recognized. The weak alkaline center is the reaction site of COS hydrolysis, the middle and strong alkaline centers are the adsorption and oxidation sites of H 2 S. The Fe/Al 2 O 3 catalyst has higher hydrolytic activity and oxidative capacity for H 2 S removal due to forming more sulfate species on Fe. The La/Al 2 O 3 catalyst has higher hydrolysis efficiency in that H 2 S rapidly desorbs from the catalyst surface to the gas phase, and then, the activity of reaction sites is recovered. This provides an idea for the preparation of sulfur-resistant catalysts.
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Frontiers in Chemistry
·
2021
·
IF 5.221
Zhang Hui,Zhou Liang,Li Jing,Rong Sijia,Jiang Jianping,Liu Shengquan
Herein, we report a novel carboxymethyl cellulose (CMC)/MIL-101 (Fe)/poly(β-cyclodextrin) (β-CDP) hydrogel with high photocatalytic activity. β-CDP can significantly enhance the photoactivity of MIL-101(Fe) in the hydrogel prepared by a simple solvothermal method. The structure and property of this composite hydrogel were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. Tetracycline was selected as a model pharmaceutical antibiotic to evaluate the photocatalytic activity of the composite hydrogel under visible light irradiation and darkness, respectively. This composite hydrogel shows excellent activity for degrading pharmaceutical antibiotics under visible light irradiation. The increased photocatalytic activity can be attributed to β-CDP, which acts as a promoter and affords an efficient separation of photogenerated electron-hole pairs of MIL-101(Fe). Moreover, the composite hydrogel is shown to have good water retainability. The hydrogel is inexpensive and shows high photocatalytic activity. Hence, it can be used as an efficient photocatalytic material.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 16
·15733-15742
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IF 2.8
Fu Xiaori,Dionysiou Dionysios D.,Brusseau Mark L.,Zaman Waqas Qamar,Zang Xueke,Lu Shuguang,Qiu Zhaofu,Sui Qian
This study presents a performance comparison of Fe(II)-catalyzed sodium percarbonate (SPC), Fe(II)-EDDS-catalyzed SPC, and of the innovative hydroxylamine hydrochloride (HA)-Fe(II)-EDDS-catalyzed SPC for the degradation of trichloroethylene (TCE) in water. TCE degradation was greater in the Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-catalyzed SPC system, indicating the effectiveness of adding EDDS as an enhancement factor for the removal of TCE. Moreover, TCE degradation was faster in the HA-Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-EDDS-catalyzed SPC system, illustrating that HA can play a synergistic role in TCE degradation. Analysis of iron distribution in the three systems demonstrated that EDDS addition maintained iron in soluble form, and that the generation of soluble ferrous from ferric iron was expedited with addition of HA. Studies using nitrobenzene and carbon tetrachloride probes provided insights on the generation of hydroxyl radical (HO • ) and superoxide anion radical (O 2 •− ) in the three systems. A gradual increasing contribution of O 2 •− to TCE removal in Fe(II)-catalyzed SPC, Fe(II)-EDDS-catalyzed SPC, and HA-Fe(II)-EDDS-catalyzed SPC systems was verified through free-radical scavenger tests. Finally, monitoring of Cl − concentrations manifested the complete dechlorination of TCE. A possible mechanism of TCE degradation involving two pathways of HO • oxidation and O 2 •− reaction was proposed.
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Carbon Resources Conversion
·
2020
·
IF 0
Yuming Li,Qiyang Zhang,Xue Yu,Guiling Jiang,Yajun Wang,Guiyuan Jiang,Zhen Zhao,Chunming Xu
Nitrogen doped carbon species (NC) was introduced into Fe based catalyst and applied into propane non-oxidative dehydrogenation. With characterizations of XRD, TEM and XPS, it was deduced that the NC modification induces the electrons transferred from NC species to Fe species, leading to electron-rich Fe species. Consequently, propane conversion and propene selectivity were increased by suppressing the by-products formation. It was also confirmed that such a modification strategy could be also extended to ones with different supports, iron precursors, and NC precursors.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
·
IF 8.91
Xi Li,Xiao Zhang,Shiwen Wang,Peng Yu,Yanhua Xu,Yongjun Sun
To suppress the electron–hole recombination and enhance the electron transfer on carbon nitride , an Fe-doped porous carbon nitride catalyst (Fe/SCN) was synthesized via supramolecular self-assembly method and applied in heterogeneous Fenton activation for efficient tetracycline (TC) degradation. Various characterizations revealed that the catalyst exhibited excellent visible light capture performance and electron transfer capacity . The highest degradation efficiency and mineralization rate of TC (10 mg L −1 ) were achieved under neutral condition (90.3% and 61.2%, respectively) with the leaching of Fe less than 14 μg L −1 . Free radical quenching experiments and spin-resonance spectroscopy characterizations revealed the dominating role of OH in TC degradation, and density functional theory calculation confirmed the formation of Fe-N X and revealed the interaction between Fe sites and H 2 O 2 . Three possible pathways of TC degradation were proposed, and the biological inhibition test revealed the potential of Fe/SCN/H 2 O 2 system to reduce environmental risks caused by TC. This work provides a new insight into the design of metal-doped heterogeneous Fenton catalyst for the efficient degradation of antibiotic contaminants in water.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2019
·
IF 5.04
Zhewen Ma,Jianxin Zou,Darvaish Khan,Wen Zhu,Chuanzhu Hu,Xiaoqin Zeng,Wenjiang Ding
Two kinds of metal-organic frameworks (MOFs) based on Co (II) and Fe (II) as metal ions and trimasic acid (TMA) as organic linker were synthesized. They were used to prepare corresponding MgH 2 -TM MOF (TM = Co, Fe) composites via ball-milling. X-ray diffraction analyses show the formation of Mg 2 Co and α-Fe phases in MgH 2 -TM MOF composites after decomposition. Both of the well dispersed Mg 2 Co and α-Fe nanoparticles exhibit considerable catalytic efficiency in accelerating the sorption kinetics of MgH 2 . The dehydrogenated MgH 2 -Fe MOF composite shows faster hydriding kinetics than the pure MgH 2 and MgH 2 -Co MOF. Meanwhile, the apparent dehydrogenation activation energy ( E d ) of the MgH 2 -Co MOF and MgH 2 -Fe MOF composites are 151.3 ± 9.4 and 142.3 ± 6.5 kJ/mol H 2 , both of which are lower than that of pure MgH 2 (181.4 ± 9.2 kJ/mol H 2 ). The improvement on the sorption kinetics of the MgH 2 -TM MOF powders is mainly attributed to the catalytic effects of nano-sized Mg 2 Co and α-Fe formed on the surface of Mg/MgH 2 particles.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Ziyan Du,Jingxi Qin,Kang Zhang,Linwei Jia,Ke Tian,Junfeng Zhang,Haijiao Xie
Single atom catalysts with high-catalytic activity have been applied in many fields. In this work, single Fe atoms (FeSA) showed excellent catalytic performance on P-nitrophenol (PNP) degradation with high total organic carbon (TOC) removal rate and high turnover frequency (TOF). The high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) results show that Fe species in FeSA are mainly single Fe atom. X-ray absorption near-edge structure (XANES) and density functional theory (DFT) calculations show that each single Fe atom is anchored by four N atoms in the form of FeN 4 active site. This coordination environment enables FeSA possesses unique geometric configuration and highly uniform active sites, which is conducive to organic pollutant adsorption and peroxymonosulfate (PMS) activation. In addition, FeSA could maintained excellent catalytic activity in complex water bodies containing different anions and humic acids. The active species in the FeSA/PMS system were also investigated. It is found that the main oxidative active species in the system are O 2 •− and 1 O 2 . This work shows that FeSA was a highly efficient single atom catalyst for the degradation of organic pollutants and has a wide application prospect in advanced oxidation processes.
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