NEW JOURNAL OF CHEMISTRY
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2019
·Vol. 43
·期 24
·9725-9731
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IF 3.069
Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta
Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.
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WATER ENVIRONMENT RESEARCH
·
2019
·Vol. 91
·期 8
·770-779
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IF 1.24
Jinhong Fan,Hehe Qin,Yunfei Zhang,Simin Jiang
In this study, Fe/Cu bimetal composite was prepared by high-energy ball milling (BM) method for the removal of refractory organics. The BM Fe/Cu bimetal was characterized by SEM-EDS, XRD, and XPS. Evenly distributed Fe and Cu was observed in the EDS mapping. In contrasting experiments, the removal rate of 4-chlorophenol (4-CP) by BM Fe/Cu materials was about 10-fold faster than that by chemical substitution deposition (CSD) of Fe/Cu material. Complete 4-CP removal and 66.7% of total organic carbon (TOC) mineralization in the BM Fe/Cu–O 2 system were achieved. Dissolved oxygen plays a crucial role for 4-CP degradation through the in situ generation of reactive oxygen species (ROS) such as H 2 O 2 , ·OH, and via oxygen activation reactions. The predominant reactive radicals were identified to be and ·OH through ESR technique and inhibition experiments. The coexistence of oxidation and reduction of 4-CP in the BM Fe/Cu-O 2 system was proposed. Practitioner points 4-CP removal rate by BM Fe/Cu is 10-fold faster than that by CSD Fe/Cu at the same conditions. Complete 4-CP removal and 66.7% of TOC reduction were achieved. All three ROS including ·OH, , and H 2 O 2 coexisted in the BM Fe/Cu-O 2 system. A harmonious coexistence of oxidation and reduction mechanism was proposed.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Yuanfeng Wei,Xingwen Yu,Chengbin Liu,Jianhong Ma,Shudan Wei,Tao Chen,Kai Yin,Hui Liu,Shenglian Luo
Although Fe-chitosan adsorbents are attractive for removing arsenite from water, the practical applications of these granular adsorbents are mainly limited by slow adsorption kinetics. In this study, radially porous Fe-chitosan beads (P/Fe-CB) were prepared using freeze-casting technique. The P/Fe-CB particles possess radially aligned micron-sized tunnels from the surface to the inside as well as excellent acid resistance. Kinetic studies show that the adsorption equilibrium time of P/Fe-CB to 0.975 mg/L As(III) (within 240 min) is considerably shorter than that of compact Fe-chitosan beads (over 600 min). The maximal adsorption capacity of P/Fe-CB for As(III) is 52.7 mg/g. It can work effectively in a wide pH range from 3 to 9, and the coexisting sulfate, carbonate, silicate and humic acid have no significant effect on As(III) removal. The addition of H 2 O 2 can further accelerate and promote the As(III) removal except at high pH (11) and phosphate concentration (50 mg/L). The fixed-bed experiments demonstrate that the P/Fe-CB column can effectively treat about 3000 bed volume (BV) of simulated As(III)-containing groundwater to meet the drinking water standard (<10 μg As/L). This study would extend the potential applicability of porous Fe based chitosan adsorbent and millimeter-sized adsorbent combined with H 2 O 2 to a great extent.
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高影响因子
CARBON
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2019
·
IF 7.466
Chao Hu,Ye Mu,Silin Bai,Juan Yang,Lijun Gao,Shao-Dong Cheng,Shao-Bo Mi,Jieshan Qiu
Electrochemically converting CO 2 into fuels or high value-added chemicals hold a great promise for the utilization of emitted CO 2 in the future. Metal-nitrogen active sites (such as Fe–N, Co–N and Ni–N) are supposed to be effective for the electrochemical reduction of CO 2 to CO, whereas their catalytic activities are largely dependent on the dispersibility and bonding structures of the catalytically active metals. In this work, we develop atomically dispersed Fe, N-codoped sandwich-like porous carbon sheets using Fe-containing zeolitic imidazolate framework-8 and graphene oxide as precursors and polyvinyl pyrrolidone (PVP) as a mediator. Compared to catalysts without PVP or with another mediator (i.e. polyetherimide), the PVP-mediated carbon sheets show a porous morphology with a higher specific surface area and a more exposed number of Fe–N active sites. Benefiting from this favourable structure, the resultant Fe, N-codoped porous carbon sheets show higher current densities and improved faradaic efficiencies up to 98.6% at −0.62 V ( vs. the reversible hydrogen electrode, RHE) for the electrochemical reduction of CO 2 to CO. This PVP-mediated strategy could be applied to the fabrication of other metal/nitrogen codoped carbon materials for electrocatalysis.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Bo Sheng,Fei Yang,Yihao Wang,Zhaohui Wang,Qian Li,Yaoguang Guo,Xiaoyi Lou,Jianshe Liu
Despite the success of Fe(II)/peroxymonsulfate (PMS) process in detoxifying organic pollutants, its intrinsic drawback of sluggish Fe(III) conversion to Fe(II) limits its large-scale practical application. Here we report that commercial MoS 2 , a common metal sulfide, can be used to unlock this kinetic constrain. Addition of MoS 2 greatly accelerates the reduction of Fe(III) to Fe(II), decomposition of PMS, and thus results in enhanced degradation efficiency of 2,4,6-trichlorophenol (TCP) (>95%) and other biorefractory halogenated organic compounds within 30 min. Mass spectroscopy data indicate that TCP can be destructed into low-molecular-weight organic acids, manifesting its powerful oxidation capacity of MoS 2 -assisted Fe(II)/PMS process. Once the Fe(III) in aqueous solution is stabilized by its organic or inorganic ligands, the boosting effects of MoS 2 are largely inhibited and less than 80% of TCP is degraded. Sulfate radicals and hydroxyl radicals are identified as the dominant reactive oxidants in the MoS 2 /Fe(II)/PMS process by radical scavenging tests. The unsaturated S on the fresh MoS 2 surface and the exposed Mo(IV) sites are supposed to react with PMS and Fe(III) in the aqueous solution, respectively. No iron oxides and Mo oxides are detected in X-ray photoelectron spectroscopy (XPS) and X-ray powder diffraction (XRD) measurement, indicating the accelerated Fe(II)/PMS process mainly occurs in the homogeneous solution. MoS 2 exhibits excellent recyclability and sustainable reactivity for the degradation of TCP after 5 consecutive runs. Overall, the present study provides a novel strategy to overcome the rate-limiting step of Fe(III)/Fe(II) that is commonly challenging Fe-based advanced oxidation processes (AOPs) and enable Fe(II)/PMS as efficient as typical Co(II)/PMS.
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Journal of Cleaner Production
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2019
·
IF 6.395
Xufang Li,Weiyu Chen,Luming Ma,Yuanxing Huang,Hongwu Wang
Iron shavings were modified and used as the catalyst (named as Fe-shaving-based catalyst) for the ozonation of bio-treated coking wastewater. The difference of organic pollutants oxidation between catalytic and sole ozonation processes was characterized by MW (Molecular Weight) distribution and 3DEEM (Three-dimensional Excitation and Emission Matrix Fluorescence) analysis. Removals of the pollutants with MW of 5–10 kDa and 10–20 kDa in catalytic ozonation process were 81.5% and 85.2%, which were far better than that in sole ozonation process (31.1% and 41.8%). Organics with MW of 0.3–2 kDa and 2–5 kDa would accumulate in both two processes, while the accumulation amount in catalytic ozonation process was half of it in sole ozonation process. The removal of fluorescent substances in catalytic ozonation process experienced a procedure of lower firstly (<15 min) and then higher (>15 min) than that in sole ozonation process. The slight residual fluorescent substances were completely removed in catalytic ozonation process, while remained unchanged in sole ozonation process with the reaction time increasing to 180 min. The catalytic effect of Fe-shaving-based catalyst was better than commonly used powder catalysts and the TOC (Total Organic Carbon) removal attained to 78%. Hydroxyl radicals (·OH) were confirmed to be the effective oxidant in catalytic ozonation process through inhibition experiments. The cumulative ·OH formations with 200 g/L Fe-shaving-based catalyst during 180 min were 362 μmol, which explained the better catalytic effect of it. The surface hydroxyl groups were determined to be the most probable active sites for ·OH generation through phosphate inhibition experiments. Besides the excellent catalytic effect, using Fe-shaving-based catalyst provided a feasible resource utilization method of industrial waste Fe-shavings. Thereby, it is a promising catalyst for practical industrial wastewater advanced treatment with catalytic ozonation process.
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ACS Applied Nano Materials
·
2019
·
IF 0
Yan Zheng,Fei He,Jiaming Wu,Delong Ma,Huailin Fan,Shufei Zhu,Xiang Li,Yizhong Lu,Qing Liu,Xun Hu
Iron (Fe)- and nitrogen (N)-codoped carbon materials hold broad application prospects in the oxygen reduction reaction (ORR) because of their abundant reserves, low cost, and excellent catalytic activity. In this study, a N-doped carbon nanotube (CNT)–graphene framework with encapsulated Fe/Fe3N nanoparticles (Fe–N–CNT@RGO) is designed and synthesized by annealing a mixture of iron acetylacetonate, dicyandiamide, and graphene oxide via a one-step calcination strategy. Fe–N–CNT@RGO has a better ORR catalytic activity than reduced graphene oxide (RGO), N-doped graphene, and N-doped CNTs with encapsulated Fe/Fe3N nanoparticles with respect to the onset potential, limiting current density, and kinetic current density. Fe–N–CNT@RGO also has high stability and a high discharging cell voltage, which approaches those of platinum/carbon in zinc–air batteries. The relationship between the structure and activity of Fe–N–CNT@RGO demonstrates that the high density of Fe–N and pyridinic N sites, moderate wettability, and positive ζ potential promote exposure of the active sites, accelerate the transmission of hydrated oxygen, and enhance the adsorption of HO2– for the 4e– ORR.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2019
·
IF 3.073
Juan Ma,Baiqin Zhou,Hong Zhang,Wenbo Zhang,Zhilong Wang
Tetracycline with high solubility and biodegradation-resistance has been widely detected from both surface and ground water, and has been proved negative impact on water environment and human health. Adsorption is considered as an environment-friendly and efficient approach to deal with TC contamination in wastewater treatment . In this work, KOH activating municipal wasted sludge biochar with different amounts of nanoscale Fe/Cu was prepared and used to remove TC from water with high performance. The removal efficiency of the composite was found to be significantly improved after loading Fe/Cu particles and the highest removal amount could reach to 386.93 mg/g under the optimum molar ratio of Fe:Cu = 5:3. The analytical results of isotherms, kinetics and thermodynamics suggested that the excellent removal performance of TC by the composite was involved many mechanisms, such as physical adsorption, hydrogen bonding, π–π interaction, complexation and electron transfer. The removal mechanisms of TC and the characteristics of composite were also confirmed by FTIR, XRD , XPS and BET determination. The excellently improved adsorption capacity , environmental-friendly and readily-made properties entrusted the novel sludge-based composite with great potential for TC removal from wastewater.
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高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Ruijie Xie,Gaoyuan Liu,Dingping Liu,Shimin Liang,Dongxue Lei,Hanying Dong,Haibao Huang,Dennis Y.C. Leung
The traditional treatment processes for volatile organic compounds (VOCs) removal generally suffered several disadvantages, such as secondary air-pollutants. To overcome these issues, wet scrubber coupled with heterogeneous UV/Fenton was developed for gaseous VOCs (i.e. toluene) removal. ZSM-5 supported iron oxide (Fe/ZSM-5) was prepared as a multifunctional catalyst for activation of H 2 O 2 and enhancement of gas-liquid mass transfer. Toluene was removed efficiently by this coupled process with the removal efficiency of 85% during 120 min. Many intermediates were detected in the solution by GC-MS while no intermediates were observed in the outlet gas, suggesting that wet scrubber coupled with heterogeneous UV/Fenton could significantly reduce secondary air pollutants . The possible mechanism of toluene oxidation was proposed including the physical adsorption by Fe/ZSM-5 and OH oxidation. This study provides an environmentally benign and highly efficient chemical scrubbing process for gaseous VOCs removal.
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高影响因子
ACS Applied Energy Materials
·
2019
·
IF 0
Chenyun Zhang,Baohua Zhang,Zhonghao Li,Jingcheng Hao
The genuine active sites toward oxygen evolution reaction (OER) are usually generated via the in situ transformation of initial electrocatalysts during anodic oxidation. In principle, all the catalysts possessing such a transition might be active toward OER. However, current OER electrocatalysts are still mainly limited in metal oxides, (oxy)hydroxides, phosphides, and chalcogenides, etc. Little attention is paid to the rational design of electrocatalysts based on the transformation-induced strategy. Herein, we demonstrated a Fe-based organic–inorganic hybrid strategy for the construction of OER electrocatalysts based on the in situ transformation. Hierarchically three-dimensional (3D) iron alkoxides of glycerol were synthesized in choline chloride (ChCl)/glycerol deep eutectic solvent (DES). During the OER, the as-prepared Fe-based organic–inorganic hybrid can transform into FeOOH, an active species for electrocatalysis, exhibiting sustainable electrocatalytic performance. It only requires 280 mV to offer a current density of 10 mA cm–2 and has a small Tafel slope of 47 mV decade–1 in 1 M KOH solution, outperforming most reported Fe-based catalysts. This work provides the concept of DES-mediated organic–inorganic hybrid materials as transformation-induced catalysts toward OER, thus casting new light on the rational design of advanced electrocatalysts for water splitting.
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ACS Catalysis
·
2019
·
IF 12.221
Chao Hu,Silin Bai,Lijun Gao,Sucen Liang,Juan Yang,Shao-Dong Cheng,Shao-Bo Mi,Jieshan Qiu
Metal-doped zeolitic imidazolate framework-8 (ZIF-8)-derived carbon materials are attractive for the electrocatalytic reduction of CO2 into CO. In such carbon materials, due to the fusion and aggregation of ZIF-8 precursors during the high-temperature pyrolysis process, it is desirable yet still challenging to create a high specific surface area with more active sites available for reacting with reactants. Using SiO2 as a protective coating on the ZIF-8 surface, we synthesize Fe, N-co-doped porous carbon nanoparticles (Fe-CNPs) which possess a hierarchical pore structure with a specific surface area as high as 1156.6 m2 g–1, much higher than the counterparts without a SiO2 coating (360.1 m2 g–1). Over these highly porous Fe-CNPs, the total current densities are more than 3 times higher than those of the lowly porous ones for the electrochemical CO2 reduction. More importantly, the maximum CO Faradaic efficiency for Fe-CNPs increases from ca. 75.0 to 98.8% in a concentrated KHCO3 solution (1 mol L–1). The porosity-induced high selectivity for CO production is also revealed on Ni-doped and Co-doped ZIF-derived CNPs, suggesting a new pathway for designing high-performance carbon catalysts through engineering the porosity for the electrochemical CO2 reduction.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
·
IF 3.131
Lu Fan,Yingxi Wang,Ling Li,Jianggang Zhou
In this study, 2-amino-terephthalic acid was designed for construction of MOFs , and carbon quantum dots (CQDs) were designed to activate the Metal Organic Frameworks (MOFs) to be used as fluorescent sensor for selectively detection for Fe 3+ and Cu 2+ , enhancing the fluorescence to an “on” state by the hybrid with CQDs in the MOFs as activating agent; quenching the fluorescence to an “off” state by removal of CQDs through the metal competitive coordination substitution strategy. Using this strategy, the prepared CQDs/MOFs material can be used as a fluorescence “on-off” probe for highly sensitive detection of Fe 3+ and Cu 2+ in aqueous solution. It was found that the LOD of CQDs/MOFs for sensing Fe 3+ and Cu 2+ were 2.3 ppb and 1.3 ppb, respectively. It was proved that the CQDs/MOFs has little cytotoxicity to 4T-1 cells, indicating the potential application in the detection for Fe 3+ and Cu 2+ ions in cells.
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高影响因子
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