SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Minghui Xiang,Zhen Lu,Siyang Li,Hui Li,Chen Wang,Jin Zhang,Lide Jin,Chunyang Li
In recent years, new heterogeneous catalysts derived from metal organic frameworks (MOFs) have been widely used in advanced oxidation processes (AOPs). In this work, zeolite imidazole framework-67 (ZIF-67) and sulfide nanozero-valent iron (S-Fe) were used as precursors to prepare S-Fe/Co bimetallic nanoparticles embedded in graphitized carbon (S-Fe/Co@GC) and used to activate peroxymonosulfate (PMS) to degrade tetrabromobisphenol A (TBBPA). Morphological and structural characterization indicated that S-Fe/Co@GC compared to pre-carbonization, the pore size of the material became larger, formed a graphite carbon skeleton with excellent electrical conductivity. In a 0.2 g/L S-Fe/Co@GC and 0.6 mM PMS system, 96.1% of TBBPA (20 mg/L) was degraded within 30 min, and the degradation yielded a total organic carbon (TOC) removal of 56.2% in 60 min. This excellent catalytic activity was attributed to the synergistic effect of graphitic carbon, sulfide nanozero-valent iron and metallic cobalt. Radical quenching experiments and electron paramagnetic resonance (EPR) technology indicated that reactive oxygen species (ROS) included HO • , SO 4 •− , O 2 •− and 1 O 2 , among which O 2 •− plays a leading role in the degradation of TBBPA. Based on the LC-MS analysis of the degradation intermediates, the degradation pathway of TBBPA in the S-Fe/Co@GC/PMS system was proposed. In addition, S-Fe/Co@GC showed a low ion leaching rate, and the regenerated S-Fe/Co@GC still had high catalytic performance. This work will extend the development of MOFs encapsulate functional nanoparticle materials for environmental remediation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Libo Deng,Lei Qiu,Rong Hu,Lei Yao,Zijian Zheng,Xiangzhong Ren,Yongliang Li,Chuanxin He
Single-atom catalysts (SAC) stabilized by nitrogen in carbon support are promising candidates for oxygen reduction reaction (ORR). However, conventional preparation methods usually lead to encapsulation of metallic centers in matrix and thus the utilization efficiency (UE) is underexploited. Herein, we report a novel strategy to prepare an Fe-SAC with all Fe atoms anchored on the surface of carbon nanospheres , which exhibited an extraordinary UE of 80% for ORR. This efficiency was achieved by coating polydopamine spheres with silica, followed by the pyrolysis of their blend with FeCl 3 . During thermal treatment, Fe migrates across the silica shell by atomic exchange with silicon, which inhibits the aggregation of Fe and allows Fe atoms to anchor on the surface. As such, it showed excellent ORR activity at a low Fe content. Zn-air batteries assembled using this catalyst showed a peak power density of 113 mW cm −2 and specific capacity of 710 mAh g Zn −1 .
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MATERIALS LETTERS
·
2021
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IF 3.423
Y.G. Wang,M. Wang,Y.Q. Wang,Q. Zhang,H.N. Zhou,H.L. Zhao
Prussian green (PG) film was directly grown on FTO glass by one-step hydrothermal process for excellent electrochromic performance. The electrochromic devices (ECDs) based on as-grown PG film can show reversible color changes between green, blue and colorless states. The existence state of iron elemental in PG film at different color states was studied by X-ray photoelectron spectroscopy. Compared with the traditional Prussian blue ECDs, PG ECDs achieve a higher optical modulation range (42.7%) and a shorter switching time (t c /t b =1.0/7.4 s). This study provides a novel method for preparing high-performance three-color ECDs by a simple hydrothermal method, and clearly shows the evolution of Fe ions during the discoloration process.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Shiyu Zhang,Qiuyu Qiao,Yangfeng Wen,Kena Ren,Xiaoyu Ma,Haisheng Tao
A novel composite of acetic acid-modulated AC-NH 2 -MIL-101(Fe) was prepared by mild chemistry . The catalyst was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), Brunaure-Emmett-Teller (BET) and X-ray photoelectron spectroscopy (XPS). Acetic acid can control the crystal size, so that the catalyst had a large specific surface area (99.35 m 2 ·g −1 ) and pore size (0.13 cm 3 ·g −1 ), the adsorption amount of Rhodamine B (RhB) up to 446.965 mg·g −1 , after the addition of peroxydisulfate (PDS), the catalytic degradation efficiency of RhB was as high as 99.7%. Electronic paramagnetic resonance spectrometer (EPR) and quenching experiments showed that the catalytic process may involve radical (·OH, SO 4 -· and O 2 ·- ) and non-radical ( 1 O 2 ) processes, in which the contribution of 1 O 2 to degradation reached 63.55% and played a major role.
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ACS Applied Nano Materials
·
2023
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IF 5.9
Yingli Luo,Xiaoming Yu,Yizhu Yao,Lin Zhu,Wenxiang Qin,Zhuohan Shan,Lanlan Song,Jilong Wang,Liangxing Wang,Hanhan Yan,Mayun Chen
Synergistic therapeutic nanomedicine with great biosafety was regarded as a promising strategy for cancer therapy in clinic. Due to the drug resistance and insufficient performance of chemotherapy, the response rate in non-small cell lung cancer is limited. As another effective strategy against tumor, ferroptosis may enhance the sensitivity of chemotherapy. Herein, we reported a biomimetic iron metal–organic framework (Fe-MOF) nanomedicine responding to the intracellular environment of non-small cell lung cancer therapy to accelerate tumor cell death by inducing the ferroptosis and apoptosis of tumor cells. We demonstrated that the doxorubicin (DOX)-loaded biomimetic Fe-MOF (mFe-MOFDOX) could dramatically promote degradation for Fe2+ generation and release of DOX in the intracellular acidic microenvironment. The mFe-MOFDOX nanoparticles enhanced the generation of reactive oxygen species (ROS) to induce comparable glutathione peroxidase 4 (GPX4)-mediated ferroptosis and assisted DOX-mediated apoptosis. Eventually, the combination of biomimetic nanoparticle-induced ferroptosis and chemotherapy-induced apoptosis inhibited tumor growth and lung metastasis, suggesting the promising potential of ferroptosis induction for promoting non-small cell lung cancer chemotherapy.
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ChemSusChem
·
2023
·Vol. 16
·期 17
·e202300633
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IF 8.4
Wen Guo,Tao Yang,Hongyan Zhang,Hao Zhou,Maoshuai He,Wenxian Wei,Wenjie Liang,Yilin Zhou,Tingting Yu,Hong Zhao
Graphical A thick Ni-based catalyst layer derived from nickel foam was synthesized by a Fe 3+ -induced strategy. In addition to the remarkable conductivity, high stability and more accessible active sites, Mo,Fe co-modulation also optimizes the adsorption free energies of the OER intermediates, boosting the catalytic activities. A highly active catalyst for the oxygen evolution reaction (OER) is critical to achieve high efficiency in hydrogen generation from water splitting. Direct conversion of nickel foam (NF) into nickel-based catalysts has attracted intensive interest due to the tight interaction of the catalysts to the substrate surface. However, the catalytic performances are still far below expectation because of the problems of low catalyst amount, thin catalyst layer, and small active area caused by the limitations of the synthesis method. Herein, we develop a Fe 3+ -induced synthesis strategy to transform the NF surface into a thicker catalyst layer. In addition to the excellent conductivity and high stability, the as-prepared FeMo-Ni 2 P 2 O 7 /NF catalysts expose more active sites and facilitate mass transfer due to their thicker catalyst layer and highly dense coral-like micro-nano structure. Furthermore, the Mo, Fe co-modulation optimizes the adsorption free energies of the OER intermediates, boosting catalytic activities. Its catalytic activity is among the highest, and it exhibits a small Tafel slope of 34.71 mV dec −1 and a low overpotential of 161 mV for delivering a current density of 100 mA cm −2 compared to reported Ni-based catalysts. The present strategy can be further used in the design of other catalysts for energy storage and conversion.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2023
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IF 3.8
Qiulin Li,Xiang Li,Ke Zhang,Jiaqi He,Yongbing Lou,Jinxi Chen
There is an urgent need to design effective and affordable noble metal-free oxygen evolution electrocatalysts for the realization of hydrogen production technology through overall water splitting. In this work, we synthesized CoMoO 4 /Fe-MOF composite catalysts on nickel foam by solvothermal method and explored them as electrodes towards oxygen evolution reaction. At 10 mA cm −2 , CoMoO 4 /Fe-MOF demonstrated a small overpotential of 238 mV, with a relatively small Tafel slope of 49.22 mV dec -1 and exhibited excellent stability after 30 h of testing. The enhanced OER activity and good durability of CoMoO 4 /Fe-MOF could be attributed to the self-supported growth of Fe-MOF nanosheets as well as the tight binding to the rod-like CoMoO 4 . The coupling of CoMoO 4 with Fe-MOF established a rich boundary, thus improving conductivity, increasing specific surface area and exposing more active sites. These results suggested that the combination of MOFs with binary transition metal oxides provided an effective route to develop robust and efficient electrocatalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Jian Xu,Atian Xie,Haotian Sun,Yuting Wu,Chengcai Li,Changguo Xue,Jiuyun Cui,Jianming Pan
Here, a polyvinylidene difluoride composite membrane (PVDF@TA–Fe membrane) was prepared via the repeated spraying of tannic acid (TA) and Fe 3+ to form a TA–Fe complex on the hydrophobic PVDF membrane, which endows the membrane surface superhydrophilicity. The effects of the number of sprays on the surface wettability and emulsion separation capacity of membrane were systematically investigated. It was found that the TA-Fe(III)-complex network formed on the membrane significantly increased the hydrophilicity of the membrane, and the PVDF@TA–Fe membrane was found to exhibit superhydrophilicity/underwater superoleophobicity. The PVDF@TA–Fe membrane was found to exhibit good separation efficiencies (above 99%) and high fluxes (1189.1–2310.0 L m −2 h −1 bar −1 ) when used to separate oil and water in various oil/water emulsions. The repeated separation experiments show that the membrane has a good antifouling performance and maintains a good oil/water separation performance after more than 10 cycles. The present work is of great importance to the large-scale preparation of superhydrophilic membranes and treatment of oily wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jianqing Ma,Nanzhengfang Jia,Huixia Jin,Sijing Yao,Kefeng Zhang,Yin Kai,Wenliang Wu,Yuezhong Wen
The removal of Cr(VI) from wastewater still faces many challenges. This study reports on chitosan-induced synthesis of few-layer MoS 2 /Fe-doped biochar (Mo-Fe 0.5 -CS) with dual applications in Cr(VI) removal. Using chitosan as a soft template, the MoS 2 in the composite had only about 3 layers with an interlayer spacing greater than that of pure MoS 2 , while Fe was embedded in the carbon skeleton in the form of 6-coordination with O/N. The Mo-Fe 0.5 -CS composite showed high affinity for Cr(VI), with rapid adsorption reaching 100% removal within 15 min for a single solution of Cr(VI). It follows the Langmuir isotherm model with a maximum adsorption capacity of up to 180 mg/g. Furthermore, the Mo-Fe 0.5 -CS composite demonstrated catalytic activity for Fenton-like reactions, which allowed for the simultaneous removal of organic pollutants and Cr(VI). In a mixture solution of Cr(VI) and Acid Red 73 (AR73), the removal efficiencies using Mo-Fe 0.5 -CS and H 2 O 2 in 30 min were 99.7% and 96.6%, respectively. The MoS 2 acted as a cocatalyst to improve the reduction of Fe(III), and the catalysis of Cr(VI) also contributed to the removal of AR73 to a certain extent. Even at pH 10, the system was effective due to the 1 O 2 produced in the reaction and the acidic microenvironment constructed by unsaturated S atoms. These findings provide insights into the effective removal and utilization of Cr(VI) in wastewater treatment .
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CHEMICAL GEOLOGY
·
2021
·
IF 4.015
ChunYan Luo,ShuaiLong Wen,YueHan Lu,JiaRu Dai,YingXun Du
The coprecipitation of dissolved organic matter (DOM) and phosphate with Fe(III) at the sediment-water interface plays an important role in the biogeochemical cycle of organic carbon (OC) and phosphorus (P) in aquatic ecosystems . However, studies remain limited towards understanding the strength of ternary DOM-phosphate-Fe(III) coprecipitation in sequestering OC and P. Here, we investigated the behaviors of humic acid (HA) and phosphate during their coprecipitation with Fe(III) and compared the coprecipitation behaviors with those during the adsorption process. The results showed that the coprecipitation of HA and phosphate with Fe(III) enhanced as pH decreased or initial Fe(III) concentrations increased. The presence of phosphate had a moderate inhibition effect on HA coprecipitation, leading to 3%–37% of reduction in precipitated HA. Changes in optical properties of DOM (i.e., SUVA 254 , E 2 /E 3 , and fluorescent components) showed that macromolecular, aromatic molecules preferentially coprecipitated, and this selectivity pattern was not influenced by the presence of phosphate. Compared to the adsorption of HA and phosphate to goethite , coprecipitation with Fe(III) displayed stronger binding ability, sequestering more than10 times of HA and phosphate, and was more efficient in sequestering protein-like compounds. The inhibitory effect of phosphate on HA sequestration was weaker during coprecipitation than during adsorption. Moreover, coprecipitation led to a lower degree of compositional fractionation of HA than adsorption, which may be explained by that inclusion, an important pathway for coprecipitation, has low selectivity for chemical compositions. Collectively, our results demonstrate that coprecipitation plays a crucial role in sequestering both OC and P in aquatic systems, arguing that the formation of ternary OC-Fe-P coprecipitates may be an important pathway for sequestering OC and P over a long term and reducing the internal loading of P in eutrophic lakes.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yantao Wan,Wei Zhang,Xiaolin Han,Lei Zhou,Huajun Zhen,Chengzi Wu,Qi Yu,Guangli Xiu
A novel B,N-decorated carbocatalyst (Fe@BPC-XBN) for peroxymonosulfate (PMS) activation was prepared by a simple pyrolysis method using the iron-based metal organic frameworks (Fe-MOF), boric acid and boron nitride (BN) as precursors. Fe@BPC-20BN removed 93.3% of bisphenol A (BPA) in 90 min compared to 64.9%, 82.1% and 83.5% with Fe@PC, Fe@BPC and Fe@PC-20BN, respectively, with 0.15 g/L catalyst and 1 mM PMS at initial pH of 7. The solo B-doping with boron acid on the Fe-MOF derived porous carbon enhanced its catalytic capacity; moreover, B, N co-doping with BN and boron acid as precursors further promoted the catalytic performance. The addition of BN not only provided more B, N catalytic centers but also improved the stability of the carbocatalyst. In addition, hydroxyl radicals , sulfate radicals, superoxide radicals, and singlet oxygen species were involved in the degradation of BPA. Fe species, –BCO 2 /–BC 2 O, pyridinic N, and pyrrolic N groups on the carbon matrix played the important roles in the BPA degradation. The outstanding catalytic performance of Fe@BPC-20BN could be attributed to the synergistic effects between iron nanoparticles and the B/N codoped carbon matrix. This study gives new insights into the design and preparation of high-efficient B,N-decorated carbocatalysts for environmental remediation.
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Analytical Methods
·
2021
·Vol. 13
·期 48
·5830-5837
·
IF 2.896
Shouhui Chen,Jingguo Yu,Zhen Chen,Zhenzhong Huang,Yonghai Song
The presence of Cd2+, Pb2+, Cu2+ and Hg2+ in drinking-water can be harmful to human health, even if their concentration is fairly low. Hence, it is significant to detect these heavy metal ions in sewage to evaluate the quality of water. Herein, amino-functionalized metal–organic frameworks (NH2-MIL-88(Fe)) embedded with graphitic carbon nitride (g-C3N4) nanosheets and acid-functionalized carbon nanotubes were prepared via a one-pot synthesis. The composite can be directly modified on the surface of glass carbon electrodes without the assistance of Nafion or other binders. The modified glass carbon electrodes can be used to simultaneously detect Cd2+, Pb2+, Cu2+ and Hg2+ in water via square wave stripping voltammetry. The doping of g-C3N4 in the composite, rich in N-containing functional groups, participates in the adsorption of metal ions on the surface of the electrodes. The porous composite provides accommodation room for metals generated by electro-reduction. The detection limit for Cd2+, Pb2+, Cu2+ and Hg2+ is 39.6 nM, 7.6 nM, 11.9 nM, and 9.6 nM, respectively. And the sensitivity for Cd2+, Pb2+, Cu2+ and Hg2+ is 0.0789 mA μM−1 cm−2, 0.4122 mA μM−1 cm−2, 0.2616 mA μM−1 cm−2, and 0.3251 mA μM−1 cm−2, respectively. This work not only enriches the functional design of Fe-MOF materials, but also develops a method for the determination of metal ions using the adsorption sites in g-C3N4.
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