ACS Applied Nano Materials
·
2023
·
IF 5.9
Dongmei Jia,Yuejin Li,Huamin Cai,Yongzheng Duan,Jing Li,Chen Ling
Capture of heavy metal ions from aqueous solutions is a critical but challenging step in environmental treatment. In this work, NH2-MIL-101(Fe) nanoparticles were synthesized by simple solvothermal methods and applied to capture Cr(VI) anions from aqueous solutions. The results revealed that NH2-MIL-101(Fe) exhibited a high capture capacity (375.2 mg g–1) and an ultrafast capture rate (4 min reaching equilibrium). The competitive effects of coexisting ions such as Cl–, HCO3–, PO43–, Cd2+, Ca2+, and Cu2+ on Cr(VI) are very weak, suggesting that the adsorption selectivity significantly enhanced by loading amino groups on MIL-101(Fe). Density functional theory (DFT) calculation was performed to better understand the adsorption mechanism of Cr(VI), showing that the amino groups could increase the adsorption energy of Cr(VI) for enhancing the adsorption capacity. Based on powder X-ray diffraction, X-ray photoelectron spectroscopy, and DFT calculations, the Cr(VI) capture mechanism by NH2-MIL-101(Fe) nanoparticles was a combination of coordination between Fe and Cr(VI), electrostatic interaction between Cr2O72– and the protonated amino group, and reduction of Cr(VI) to Cr(III).
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CHEMOSPHERE
·
2023
·
IF 8.8
Qiong Wu,Chunying Dong,Maoxiang Chen,Yu Zhang,Meiqiang Cai,Yan Chen,Micong Jin,Zongsu Wei
In this study, SiO 2 -composited biochar decorated with Fe/Mn was prepared by co-pyrolysis method. The degradation performance of the catalyst was evaluated by activating persulfate (PS) to degrade tetracycline (TC). The effects of pH, initial TC concentration, PS concentration, catalyst dosage and coexisting anions on degradation efficiency and kinetics of TC were investigated. Under optimal conditions (TC = 40 mg L −1 , pH = 6.2, PS = 3.0 mM, catalyst = 0.1 g L −1 ), the kinetic reaction rate constant could reach 0.0264 min −1 in Fe 2 Mn 1 @BC-0.3SiO 2 /PS system, which was 12 times higher than that in the BC/PS system (0.00201 min −1 ). The electrochemical, X-ray diffractometer (XRD), Fourier transform infrared spectrum (FT-IR) and X-ray photoelectron spectroscopy (XPS) analysis showed that both metal oxides and oxygen-containing functional groups provide more active sites to activate PS. The redox cycle between Fe(II)/Fe(III) and Mn(II)/Mn(III)/Mn(IV) accelerated the electron transfer and sustained the catalytic activation of PS. Radical quenching experiments and electron spin resonance (ESR) measurements confirmed that surface sulfate radical (SO 4 •− ) play a key role in TC degradation . Three possible degradation pathways of TC were proposed based on high-performance liquid chromatography coupled with high-resolution mass spectrometry (HPLC-HRMS) analysis, the toxicity of TC and its intermediates was analyzed by bioluminescence inhibition test. In addition to the enhanced catalytic performance, the presence of silica also improved the stability of the catalyst, as confirmed by cyclic experiment and metal ion leaching analysis. The Fe 2 Mn 1 @BC-0.3SiO 2 catalyst, derived from low-cost metals and bio-waste materials, offer an environmentally friendly option to design and implement heterogenous catalyst system for pollutant removal in water.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Wenhua Tong,Xinhang Du,Jiepeng Wang,Hao Yan,Tonghui Xie,Yabo Wang,Yongkui Zhang
Organophosphate esters (OPEs) waste is difficult to dispose effectively because of its stability and the potential risk of P element. In this study, taking one typical organic extractant of tributyl phosphate (TBP) as an example, we proposed a strategy to treat OPEs inspired by chemical looping combustion (CLC) technology—oxygen carrier immobilization process (OCIP), aiming at efficient TBP degradation and simultaneous P immobilization. Adopting Fe-Mn bimetallic oxide (FMBO) as oxygen carrier, an almost 100% P immobilization efficiency was achieved under recommended conditions which were obtained by response surface methodology . Meanwhile, gaseous products released from TBP degradation, e.g., non-methane hydrocarbon, was lower than the maximum allowable emission concentration limit. Further characterizations implied that P-species released from reaction process were mainly immobilized as stable inorganic forms of metaphosphate, phosphate and pyrophosphate. On the basis of identifying degradation intermediates, we proposed a possible degradation pathways. FMBO as an oxygen carrier provided sufficient oxygen molecules for flameless combustion of OCIP process. Electron paramagnetic resonance measurement confirmed the existence of oxygen vacancies on FMBO surface, which contributed to the formation of •O 2 − . Oxidation by oxygen molecules and •O 2 − attack resulted in the degradation and mineralization of TBP, with simultaneously achieving P stabilization.
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Energy Technology
·
2019
·Vol. 7
·期 7
·1801128
·
IF 3.163
Weicheng Cui,Hongye Bai,Konggang Qu,Fagen Wang,Peng Guan,Dongbo Xu,Weiqiang Fan,Weidong Shi
Kinetics play a critical role in the photoelectrochemical (PEC) system, whereas co-catalysis is mainly responsible for reducing the reaction barrier and facilitates water splitting. Here, the unsaturated Fe sites through the metal-organic framework (MOFs) structure promote the kinetics of water oxidation over TiO 2 are successfully in situ decorated. This heterostructure further helps us to better understand the PEC behaviors of organic–inorganic hybrid systems. MIL-100(Fe), as the typical MOFs model, is facilely achieved by an FeOOH sacrificial template method, a strategy which could anchor the compact and ultrathin MIL-100(Fe) films on the surface of TiO 2 to obtain abundant unsaturated Fe sites. The photocurrent density of MIL-100(Fe)/TiO 2 reaches about 2.4 times at 1.23 V vs reversible hydrogen electrode (RHE) compared with bare TiO 2 , and the incident photon to current conversion efficiency value increases up to 47% (at 390 nm). Furthermore, the photocurrent density of MIL-100(Fe)/TiO 2 is maintained at 84% after 3 h, showing that the organic component of MIL-100(Fe) takes a nature of favorable stability. The configuration of MIL-100(Fe)/TiO 2 will bring a new insight for learning the basic function of unsaturated metal sites in the PEC system.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Yaqiong Wang,Jing Zhang,Chuyu Zhang,Bingjie Li,Jiaojiao Wang,Xuejun Zhang,Dong Li,Shao-Kai Sun
Fe–polyphenols coordination polymers have emerged as a versatile theranostic nanoplatform for biological applications owing to the appealing biocompatibility of precursors from nature. Incorporating bioactive molecules with Fe–polyphenols coordination polymers is greatly significant to take full advantages of their superiorities for advanced application. Herein, we show functional-protein-assisted fabrication of Fe–gallic acid (GA) nanonetworks via a mild and facile biomineralization for photothermal therapy. Mild alkaline condition is crucial to obtain protein–Fe–GA nanonetworks with intense near-infrared absorption and their unique network structure allows reducing the leakage to the surrounding normal tissues, benefiting high photothermal therapeutic efficacy and minimal side effects. The proposed bovine serum albumin–Fe–GA nanonetworks are successfully used to eradicate tumor in vivo. In addition, this universal method can be extended to synthesize other protein-involved nanonetworks, such as human serum albumin–Fe–GA and ovalbumin–Fe–GA. More importantly, the intrinsic bioactivity of protein can be retained in the nanonetworks, and the ovalbumin–Fe–GA nanonetworks enable inducing the maturation of immune cells, showing the successful fusion of immune activity of ovalbumin into the nanonetworks. The proposed biomineralization strategy shows a bright prospect in incorporating various functional proteins, such as enzymes and antibodies, to form protein–Fe–GA nanonetworks with good biocompatibility, favorable photothermal effect, and specific biological function.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2018
·
IF 4.841
Yuxiang Cai,Xinbo Zhu,Wenshuo Hu,Chenghang Zheng,Yang Yang,Menghan Chen,Xiang Gao
Plasma-catalytic decomposition of low concentration ethyl acetate with LaMO 3 (M = Co, Mn and Fe) perovskite catalyst was investigated in a coaxial dielectric barrier discharge (DBD) reactor. The combination of perovskite catalyst and plasma enhanced ethyl acetate decomposition, and the activity sequence was LaCoO 3 > LaMnO 3 > LaFeO 3 . Characterizations results indicated that the activation of surface oxygen species and amount of oxygen vacancies contributed to ethyl acetate decomposition remarkably. FT-IR analysis demonstrated that the employment of LaCoO3 catalyst also reduced the amount of unwanted by-products. Based on these results, reaction mechanism of ethyl acetate plasma-catalytic decomposition process was proposed.
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ANALYST
·
2018
·Vol. 144
·期 2
·656-662
·
IF 3.864
Shujuan Zhuo,Yuanyuan Guan,Hui Li,Jing Fang,Ping Zhang,Jinyan Du,Changqing Zhu
In this paper, we have presented a novel strategy to fabricate Fe-doped carbon quantum dots (Fe-CQDs) for dopamine sensing applications. The Fe-CQDs are obtained by one step hydrothermal carbonization, using ethylenediamine tetraacetic acid salts and ferric nitrate as the carbon and iron source, which simultaneously incorporates Fe (dopamine-bonding site) and luminescent carbon quantum dots (fluorophores). The added dopamine containing catechol groups might form complexes with Fe ions (doped in CQDs) due to coordination. Subsequently, dopamine was oxidized to generate dopamine-quinone (a known potent electron acceptor) species by ambient O2. Thus, the coordination induced dopamine in proximity to the CQDs, which provided favourable electron acceptors in close proximity to the CQDs and produced high quenching efficiencies. Such fluorescence responses can be used for well quantifying dopamine in the range of 0.01–50 μM with a detection limit of 5 nM (S/N = 3). The proposed sensing system has been successfully used for the assay of dopamine in human urine samples. Preliminary cell image study indicates that the obtained Fe-CQDs possess high photostability and low cytotoxicity, which make them promising for biological applications.
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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.
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INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Wei Wang,Mehran Amiri,Tao Huang,Lev N. Zakharov,Yining Zhang,May Nyman
Isolating Fe(III) clusters from water without stabilizing ligands is significantly challenged by the high acidity of Fe3+-bound water, leading to uncontrolled precipitation of iron oxyhydroxides. Here we demonstrate a freeze-drying solvent-exchange method that enabled the isolation of a metastable Fe(III) sulfate decameric cluster formulated [Fe10O2(SO4)12(OCH3)2]·14CH3OH (Fe10). Without stabilization by solvent-exchange, the aqueous species undergoes rapid conversion to the iron sulfate mineral schwertmannite. Monitoring the hydrolysis process from cluster intermediates to schertmannite by small-angle X-ray scattering, we observe the progression from Fe10 to 37 Å soluble nanoparticles prior to the precipitation process. This condensation behavior of Fe10 is further exploited to develop a simple laboratory synthesis of schwetmannite. In addition, we demonstrate the versatility of the freeze-drying solvent-exchange method by isolating Al(III), Zn(II), and Cd(II) substituted Fe(III) sulfate clusters. The freeze-drying solvent-exchange method provides a unique opportunity to isolate cluster intermediates and models to aid in our understanding of metal-ion hydrolysis processes in environmental, material science, and geological studies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2019
·
IF 6.361
Zhefu Li,Binling Chen,Xianfeng Wang,Jun Nie,Guiping Ma
In this work, a novel catalyst of oxygen reduction reaction (ORR) was designed and fabricated by electrospinning, photo-curing and carbonization, based on polymer poly(dimethylsilylene ethynylenephenyleneethynylene) (PMSEPE) and metal organic frameworks (MOFs)—Materiaux de l'Institute Lavosier-101(Fe) (MIL-101(Fe)). The optimal catalyst PMSEPE/MIL-101(Fe)-800, which was carbonized at 800 °C, presented a bamboo-like nanofiber structure with a high degree of graphitization, a high specific surface area (302.3 m 2 /g) and a high yield (64.17%). Fe 3 C particles were found to be encapsulated into the Fe-Si-N co-doped carbon nanofibers. In the electrochemical tests, PMSEPE/MIL-101(Fe)-800 showed an onset potential of 0.935 V ( vs . RHE) and a diffusion limit current of 6.01 mA/cm 2 ( vs . RHE) in 0.1 M KOH aqueous solution, of which performances are competitive to commercial 20 wt% Pt/C. PMSEPE/MIL-101(Fe)-800 also exhibited a higher methanol tolerance and duration stability. Further Zn-air battery test used by PMSEPE/MIL-101(Fe)-800 suggested its potential for the application of fuel cell.
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JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2019
·Vol. 66
·期 12
·1610-1618
·
IF 1.188
Tao Wang,Aiyun Hu,Haijun Wang,Yongmei Xia
Layered double hydroxides (LDHs) and their derivatives have been reported to be widely used as heterogeneous catalysts in various reactions. Herein, Ni-Fe LDHs with the controlled Ni/Fe molar ratios (2:1, 3:1, 4:1) were synthesized via an easy hydrothermal method, which were used to catalyze the selective reduction of biomass-derived furfural into furfuryl alcohol using 2-propanol as a H-donor under autogenous pressure and characterized using FT-IR, XRD, TGA, BET, SEM, NH 3 -TPD, and CO 2 -TPD. It was found that the LDH with a Ni/Fe molar ratio of 3:1 demonstrated the best catalytic activity among the LDHs with different Ni/Fe molar ratios, which showed 97.0% conversion of furfural and 90.2% yield of furfuryl alcohol at 140°C for 5 hr. This was attributable to the synergistic effect of acidic sites and basic sites of the catalyst.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Guoru Li,Xiaobo He,Fengxiang Yin,Biaohua Chen,Huaqiang Yin
The development of highly efficient electrocatalysts with low cost for oxygen reduction reaction (ORR) is urgently required for metal-air batteries and fuel cells. In this work, Fe Co/MIL-101(Cr) with various molar ratios of Fe/Co as hybrid catalysts was prepared by a facile and mild impregnation method. MIL-101(Cr) increased the specific surface areas of the hybrid catalysts, thus improving the dispersion of Fe and Co species at their surfaces. The effects of Fe and Co species on ORR activity of the hybrid catalysts were investigated. It is found that the synergistic effects between the well-dispersed Fe and Co species contribute mainly to ORR activity. More specifically, Fe species exert a partial-charge-transfer-activation effect on Co ones, which reduces the charge transfer resistance and thus improves the catalytic activity . As a result, Fe Co/MIL-101(Cr) showed the excellent ORR activity, in which Co 50 Fe 50 /MIL-101(Cr) exhibited the superior ORR activity to the other prepared hybrid catalysts.
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