CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Bingyang Liu,Yu Wang,Xue Hao,Xuetao Liang,Qi Yang
In this work, a carbon-based catalyst Fe/Co@C with MOF as a self-sacrificing template was prepared by high-temperature roasting of FeCo-MIL101, which was applied to activate PMS for the degradation of chlorotriazine herbicides (ATZ and SIM) showing excellent performance. Characterization analysis revealed that Fe/Co@C possesses a certain graphene structure and has a saturation magnetization rate of 0.87 emu/g, which can be separated from the solution easily and quickly. The degradation of ATZ and SIM was enhanced by introducing chloride ions into the system, and 100 mmol/L Cl - could lead to the complete removal of ATZ and SIM in 6 min, while improving the interfacial electron transfer of Fe/Co@C/PMS. In combination with quenching experiments, ESR test results and DFT calculations, two important roles of chlorine radicals in the reaction are proposed: (1) direct electron transfer and (2) indirect promotion of 1 O 2 generation through the production of HOCl. In addition, the testing of the influencing factors of the catalyst in the system (catalyst dosing, PMS dosing, pH, temperature), the testing of coexisting anions in the aqueous matrix, and the reusability all showed satisfactory performance. Finally, the degradation mechanisms of ATZ and SIM were proposed in combination with GC–MS determination of contaminant intermediates and analysis of their toxicity.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Yurong Gao,Hanbo Chen,Zheng Fang,Nabeel Khan Niazi,Kwasi Adusei-Fosu,Jianhong Li,Xing Yang,Zhongzhen Liu,Nanthi S. Bolan,Bin Gao,Deyi Hou,Chenghua Sun,Jun Meng,Wenfu Chen,Bert F. Quin,Hailong Wang
Sorption and oxidation are two potential pathways for the decontamination of trivalent antimony (Sb(III))-bearing water, using iron (Fe)-modified biochar (FeBC). Here we investigated the sorption and oxidation behavior of FeBC for Sb(III) in aqueous solutions. Results revealed that Sb(III) removal by FeBC was significantly improved showing the maximum Sb(III) sorption (64.0 mg g −1 ). Density functional theory (DFT) calculations indicated that magnetite (Fe 3 O 4 ) in FeBC offered a sorption energy of −0.22 eV, which is 5 times that of non-modified biochar. With the addition of peroxymonosulfate (PMS), the sorption of Sb(III) on FeBC was 7 times higher than that on BC, indicating the sorption capacity of FeBC for Sb(III) could be substantially increased by adding oxidizing agents . Electrochemical analysis showed that Fe modification imparted FeBC higher electron-donating capacity than that of BC (0.045 v. s. 0.023 mmol e − (g biochar) −1 ), which might be the reason for the strong Sb(III) oxidation (63.6%) on the surface of FeBC. This study provides new information that is key for the development of effective biochar-based composite materials for the removal of Sb(III) from drinking water and wastewater. The findings from this study have important implications for protecting human health and agriculture.
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Journal of Water Process Engineering
·
2023
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IF 7
Fang Zhang,Lei Wang,Lutao Yang,Yong Dai,Jun Zhang,Lei He,Juqing Cui,Jian Shen,Zhe Wang
Immobilized microbial technology is a simple, cost-effective, and efficient technique to minimize the difficulty and energy consumption of heavy oil extraction, as well as the COD of oilfield wastewater. In this work, PC- g -Mag(Fe-MOF) was prepared to immobilize microorganisms obtained by grafting lecithin after magnetization using Fe-MOF. The orthogonal tests showed that the optimum temperature for immobilized microorganisms was 38 °C, the optimum pH was 7, the optimum inoculum was 7 % and the desired mineralization level was <20,000 ppm. The viscosity of free and immobilized microorganisms decreased by 61.5 % and 76 %. The recovery efficiency of the carrier with two species of bacteria after 5 cycles of experiments was 87.5 % and 73.2 %, respectively. The removal rate of COD in the 5th time was 69.3 %, the viscosity reduction rate of heavy oil was 61.6 %. The recovery efficiency of heavy oil was increased by 25.09 %. Fe-MOF acts as a biocarrier to immobilize bacteria and enhance the metabolic activity of their microbial communities and improves COD removal from oilfield wastewater and viscosity reduction in heavy oil.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xinqiang Liu,Haoran Yin,Shifan Zhang,Menghan Huang,Tayirjan Taylor Isimjan,Xiulin Yang,Dandan Cai
Strategically tuning the composition and structure of transition metal phosphates (TMPs) holds immense promise in the development of efficient oxygen evolution reaction (OER) electrocatalysts. However, the effect of crystalline phase transformation for TMPs on the catalytic OER activity remains relatively uncharted. In this study, we have deftly orchestrated the reaction process of anion-etched precursor to induce the amorphization process of FeCo-PO x from crystalline to amorphous states. The as-obtained amorphous FeCo-PO x (A-FeCo-PO x ) exhibited an optimized OER performance with a low overpotential of 270 mV at a current density of 10 mA cm −2 , which could be attributed to the flexibility of its amorphous structure and the synergistic effect of oxygen vacancies . Moreover, when incorporated into an overall water splitting (OWS) device configured as A-FeCo-POx (+) ||Pt/C (–) , it displayed long-term solid stability, sustaining operation for 300 h at a current density of 200 mA cm −2 . This work not only provides valuable insights into understanding the transformation from crystalline to amorphous states, but also establishes the groundwork for the practical utilization of amorphous nanomaterials in the field of water splitting.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Meiling Chen,Lin Ding,Shijun Zhu,Xiuqin Xiong,Xinkai Yuan,Yanhua Peng,Liming Yang,Hui Shi,Penghui Shao,Xubiao Luo
The slow Fe(II)/Fe(III) cycle during the Fenton reaction process strongly impedes oxidation efficiency in practical applications. In this study, an activated carbon (AC) assisted Fenton reaction system was used to treat electroplating wastewater containing Ni-ethylenediaminetetraacetic acid (Ni-EDTA). AC was found to enhance the removal of Ni-EDTA in Fenton/Fenton-like reactions. The reported results revealed that AC could effectively promote the regeneration of Fe(II) from Fe(III) species via electron transfer to improve the reaction rather than directly enhancing the H 2 O 2 decomposition to accelerate the production of hydroxyl radicals (•OH). Quenching experiments and EPR also demonstrated that •OH and •O 2 − took part in the radical oxidation process, in which the contribution of •OH was dominant. XPS and FT-IR analysis further confirmed that the carbonyl group (C O) on the surface of AC could indeed act as the dominant active site and an electron donor to directly reduce Fe(III). In addition, electrochemical tests indicated that AC could increase the oxidation potential of Fe(III) to boost the reaction between Fe(III) and H 2 O 2 , thus enabling the transfer of electrons from H 2 O 2 to Fe(III) to facilitate the Fe(II)/Fe(III) cycle. This study might contribute to a new insight into the mechanisms of AC-catalyzed Fenton oxidation processes for the decomplexation heavy metal-EDTA.
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Bioactive Materials
·
2021
·
IF 14.593
Xiyu Li,Juan Wu,Danxue Li,Qin Zou,Yi Man,Ling Zou,Wei Li
Insufficient early osteogenesis seriously affects the later stage osteogenic quality and osseointegration of dental implants. To promote early osteogenesis, we first designed a Ti dental implant with a built-in magnet (mTi) to produce a local static magnetic field (SMF). Then, a dental implantation system comprising the mTi implant and the superparamagnetic hydroxyapatite (HA:Yb/Ho–Fe, named HYH-Fe) particles was implanted into the alveolar bone of beagles. The results showed that the mTi + HYH-Fe group displayed better early osteogenesis and later stage osseointegration than the Ti + HA and mTi + HA groups. A combination of the local SMF (mTi) and superparamagnetic HYH-Fe particles had a positive effect on the pro-osteogenesis of Ti implants. The results also indicated that week 10 could be adopted as the key time point to evaluate the early osteogenic effect of the mTi + HYH-Fe implantation system, which would be a promising prospect for promotion of osteogenesis, in vivo tracking investigation of material-bone relationships, and clinical applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Chen Chen,Yongxiao Tuo,Qing Lu,Han Lu,Shengyang Zhang,Yan Zhou,Jun Zhang,Zhanning Liu,Zixi Kang,Xiang Feng,De Chen
Metal-organic frameworks (MOFs) have recently emerged as promising precursors to construct efficient non-noble metal electrocatalyst for oxygen evolution reaction (OER). Herein, a Co-Ni-Fe spinel oxide-carbonitrides hybrids (CoNiFeO x -NC) electrocatalyst with hierarchical structure was synthesized from Fe-MIL-101-NH 2 through a unique ion-exchange based strategy. The ion exchange of Fe-MIL-101-NH 2 with both Ni and Co ions induced a hierarchically structured 2-D ternary metal MOF shell layer encapsulated 3-D octahedral MOF crystals as a core. This prevents the collapse of MOF frameworks during the air calcination process and affords highly porous structure and large surface area. Additionally, the unique combination of Co-Ni-Fe in spinel oxides derived from calcination of the hierarchically structured core-shell MOF provides a favorable electronic environment for the adsorption of OER intermediates, which was further verified by the XPS characterizations and DFT calculations. DFT study revealed the Ni-Co coordinated O h sites in the MFe 2 O 4 reverse spinel structures as the main active sites, which tuned the binding strength of oxygen species with a catalyst through electron transfer of Fe→Co→Ni, thereby lowered the energy barriers for OER. As a result, the rationally designed CoNiFeO x -NC catalyst manifests superior OER performance with a low overpotential of 265 mV at 50 mA cm −2 and a decent Tafel slope of 64.1 mV dec -1 . The ion-exchange based strategy may serve as a versatile platform for rational design and synthesis of multi-metallic MOF derived electrocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Li Li,Qian Zhang,Yuecheng She,Yongbo Yu,Junming Hong
Mn–Fe bimetal catalyst possesses excellent activation properties, and the enhancement of Mn/Fe redox cycle for electron transfer is related to the crystalline structure and surface functional groups. Therefore, material structure optimization is an effective strategy to improve its activation performance in advanced oxidation . In this study, Mn–Fe LDO catalyst with strong Mn/Fe synergistic effect was synthesized, and used for bisphenol A degradation. Under the condition of 0.4 g/L Mn-Fe LDO, 1.5 mM PMS and pH 7.0, Mn-Fe LDO/PMS system exhibited excellent degradation performance that 100% of BPA (20 mg/L) and 72.0% of COD could effective be degraded within 50 min. Five-run recycle and metal ions leaching experiments proved the excellent reusability and stability of Mn-Fe LDO. To deepen the understanding of catalytic mechanism, the synergistic effect and electron transfer between Mn and Fe were confirmed via XPS and CVs results. Moreover, the indispensable role of surface hydroxyl groups were clarified via phosphate masking experiment, ATR-FTIR and LSV analysis. The presence of Mn and Fe active sites and hydroxyl groups on Mn-Fe LDO surface could efficiently promote electron transfer, thus accelerating the redox cycles of Mn 3+ /Mn 2+ and Fe 3+ /Fe 2+ . The generation of SO 4 ·− and HO· as the main radicals was occurred on the surface of Mn-Fe LDO, and SO 4 ·− played a major role during the reaction. On the basis of these experimental conclusions, the mechanisms of Mn–Fe LDO/PMS system for high-efficiency BPA degradation were proposed. GC-MS analysis was performed to detect the BPA degradation intermediates and propose the possible degradation pathways.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2021
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IF 6.789
Qiang Zeng,Hui Zhong,Zhiguo He,Liang Hu
Developing materials from natural minerals to efficiently remove arsenite (As(Ⅲ)) from solution is vital important for resources comprehensive utilization and environment protection. In this study, biotite containing minerals was used to prepare a novel composite of amino modified silica supported MnO 2 /Fe–Al hydroxide (SNMFA composite), which was then applied to remove arsenite. Scanning electron microscope (SEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results indicated that many amorphous MnO 2 and Fe–Al hydroxide nano sheets were loaded on the surface of layered silica structure. Batch experiments showed that this composite could efficiently remove As(Ⅲ) from aqueous solution, and the maximal removal capacity was identified as 46.11 mg/g. As(Ⅲ) adsorption behaviours of SNMFA composite were confirmed by the pseudo-second-order kinetic model and Langmuir model, indicating that As(Ⅲ) adsorption on its surface was monolayer adsorption. The adsorption process was a pH and temperature dependent process, and increasing pH and temperature have facilitated the removal of As(Ⅲ). Thermodynamic analysis showed that As(Ⅲ) adsorption process was a spontaneous endothermic reaction . The As(Ⅲ) removal was mainly relied on the stable inner-sphere coordination model, and the corresponding mechanisms were involved in chelation, precipitation, oxidation-adsorption and electrostatic interaction.
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RSC Advances
·
2021
·Vol. 11
·期 18
·10540-10547
·
IF 3.361
Anxia Li,Xiaoxin Yang,Juan Chen
Metal–organic frameworks (MOFs), such as MIL-53(Fe), have considerable potential as drug carriers in cancer treatment due to their notable characteristics, including controllable particle sizes, high catalytic activity, biocompatibility and large porosity, and are widely used in a broad range of drugs. In this study, a new approach for the synthesis of MIL-53(Fe) nanocrystals with controlled sizes has been developed using a non-ionic surfactant PVP as the conditioning and stabilizing agent, respectively. During the nucleation of MIL-53(Fe), the PVP droplet, as a nano-reactor, controlled the growth of the crystal nucleus. The size and aspect ratio (length/width) of nanocrystals increased with an increase in PVP in the synthetic mixture. The MIL-53(Fe) nanocrystals showed a homogeneous morphology, with approximately 190 nm in length and 100 nm in width. MIL-53(Fe) not only was used to load the anticancer drug doxorubicin (DOX) but also generated hydroxyl radicals (˙OH) via a Fenton-like reaction for ROS-mediated/chemo-therapy of cancer cells. The approach was expected to synthesize numerous types of nano-size iron(III)-based MOFs, such as MIL-53, 89, 88A, 88B and 101. The MIL-53(Fe) nanocrystals hold great promise as a candidate to improve the controlled release of drugs and treatment effect for cancer therapy.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
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IF 4.539
Bin Ren,Junfeng Miao,Shasha Wang,Yuelong Xu,Zuozhao Zhai,Xiaoxi Dong,Zhenfa Liu
In this study, a 3D Fe-based and N-doped coral-like carbon composite (Fe-NGLC) was successfully prepared via the simple impregnation of a self-made 3D nitrogen-enriched and porous layered graphene-like support with Fe 2 (SO 4 ) 3 as the precursor. It was characterized through X-ray diffractometry, scanning electron microscopy, X-ray photoelectron spectroscopy, etc.; Fe-NGLC exhibited regular three-dimensional coral-like structures with dense porosity and high of Fe–N species content. As a heterogeneous Fenton catalyst of the methylene blue (MB) degradation, the prepared composite showed impressive activity over a wide pH range (4–10). Almost 100% of the MB could be degraded in 60 min, and the results agreed well with the pseudo-first-order kinetic model . To identify the crucial active sites of MB degradation, the correlation between the rate constant derived from the pseudo-first-order kinetic model and the different Fe species in the catalyst prepared under various conditions was investigated. This revealed the key role of the Fe–N complexes for the heterogeneous Fenton reaction. Moreover, Fe-NGLC exhibited recyclability and only a slight decrease in removal efficiency after five cycles. The excellent performance of Fe-NGLC demonstrates its great potential as a Fenton catalyst for wastewater treatment .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Di Chen,Guofu Li,Xing Chen,Qian Zhang,Jing Sui,Chengjie Li,Yingchao Zhang,Jing Hu,Jianhua Yu,Liyan Yu,Lifeng Dong
Rational construction of advanced bifunctional catalysts with dual-active-sites is still challenging for both oxygen reduction (ORR) and oxygen evolution reactions (OER). Herein, metal-doped dicyandiamide formaldehyde resin is innovatively exploited to synthesize N/Co/Fe/Ni multi-doped carbon nanotubes (denoted as CoFeNi@CNT) with metal-nitrogen-carbon (M N C) and CoFeNi nanoparticles as the ORR and OER active sites, respectively. Abundant active sites and high degree of graphitization enable CoFeNi@CNT with a high ORR half-wave potential of 0.82 V and a low OER overpotential of 440 mV at 10 mA cm −2 , which are comparable or superior to noble-metal catalysts. Particularly, the CoFeNi@CNT air electrode of rechargeable Zn-air batteries shows remarkable open circuit potential (1.46 V), discharge power density (152.3 mW cm −2 ), specific capacity (814 mAh g −1 ), and cycling stability for more than 250 h. It is worth emphasizing that this synthesis strategy is rather simple, low-cost, high yield, and the proportion and amount of doped metal ions can be easily adjusted according to the needs for different applications.
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