APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Huan Yang,Jun Li,Shuai Hu,Yi Liu,Cheng Peng,Chengfei Deng,Qinglin Chen,Tianding Hu,Shaoyun Shan,Yunfei Zhi,Hongying Su,Lihong Jiang
It’s extremely urgent to remove ciprofloxacin (CIP) pollutant from wastewater since the extensively used CIP is difficult to be degraded in natural environment, seriously threating the ecological environment and human health. Herein, a series of Fe-doped zeolitic imidazolate framework-8 (Fe-ZIF-8) adsorbents were fabricated by doping Fe ion into the ZIF-8. Systematic adsorption experiments were conducted to evaluate the possibility of Fe-ZIF-8 in removing CIP from aqueous solutions. Accordingly, the maximum adsorption capacity of Fe-ZIF-8 for CIP could reach an ultrahigh value of 1484 mg g −1 , which is higher than that of any reported adsorbents. The CIP adsorption on Fe-ZIF-8 followed pseudo-second-order kinetics model and fitted well with Freundlich isotherm model, indicating the presence of the chemosorption and multilayer adsorption. The outstanding adsorption capacity of CIP could be ascribed to the high surface area and large pore volume of Fe-ZIF-8 as well as the synergetic effects including surface complexation, electrostatic attraction, π-π and hydrogen bonding interactions. These unrivalled traits certify the great potential of Fe-ZIF-8 in practical application.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 10
·4806-4813
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IF 3.925
Jie Song,Leilei Sun,Hongchao Geng,Wenlong Tan,Deshuai Zhen,Qingyun Cai
β-Phase NaYF4:Yb,Tm,Gd up-conversion nanorods (UCNRs) with high uniformity were synthesized by a solvothermal method. The optimal fluorescence intensity of UCNRs was explored. After further modification with Materials of Institute Lavoisier-100(Fe) (MIL-100(Fe)) by the layer-by-layer self-assembly method, near-infrared light-triggered UCNR@MIL-100(Fe) nanomaterials with excellent antibacterial performances were constructed. A core–shell structure was constructed and confirmed by transmission electron microscopy (TEM). Reactive oxidizing species (ROS) detection indicated that the nanomaterials owned good photodynamic efficacy. The antibacterial experiments showed that the nanomaterials with 980 nm light irradiation and hydrogen peroxide (H2O2) had good antibacterial activity against Gram-negative and Gram-positive bacteria. Under 980 nm laser excitation, UCNRs generated ultraviolet and visible light to activate MIL-100(Fe) and induced a photo-Fenton reaction, which further produced oxygen species for antibacterial applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Xiaoqiang An,Li Quan,Jianqiao Liu,Qingwen Tang,Huachun Lan,Huijuan Liu
Designing non-precious electrocatalysts with multiple active centers and durability toward overall water splitting is of great significance for storing renewable energy. This study reports a low-cost Mo, Fe codoped NiCoP x electrocatalysts derived from Co-Fe Prussian blue analogue and following phosphorization process. Benefitted from the optimized electronic configuration, hierarchical structure and abundant active sites, the Mo,Fe-NiCoP x /NF electrode has shown competitive oxygen evolution reaction ( ƞ 10 = 197 mV) and hydrogen evolution reaction performance ( ƞ 10 = 99 mV) when the current density is 10 mA cm −2 in 1 M KOH solution. Moreover, the integrated water splitting device assembled by Mo,Fe-NiCoP x /NF as both anode and cathode only needs a voltage of 1.545 V to reach 10 mA cm −2 . Density functional theory results further confirm that the Mo, Fe codoped heterostructure can synergistically optimize the d-band center and Gibbs free energy during electrocatalytic processes, thus accelerating the kinetics of electrochemical water splitting. This work demonstrates the importance of rational combination of metal doping and interface engineering for advanced catalytic materials.
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ChemSusChem
·
2022
·Vol. 15
·期 6
·e202102642
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IF 9.14
Lingling Zheng,Yingji Zhao,Hongjuan Zhang,Wei Xia,Jing Tang
Graphical There's no space : Highly dispersed Fe−N x anchored on concave N-doped carbon is synthesized by space-confined strategy. The resulting NC@Fe−N−C exhibits superior oxygen reduction activity, originating from the combination of intrinsic activity and acceleration of mass electron transfer. Carbon-based electrocatalysts with atomically dispersed Fe−N−C display promising performance for oxygen reduction reaction (ORR) amongst non-precious electrocatalysts. Nonetheless, increasing the number and utilization of Fe−N−C active sites is challenging. Designing morphologies and adjusting the pore structure of carbon-based electrocatalysts would boost the mass transfer, enhance the utilization of the active sites, and increase the overall ORR performance. In this work, a concave N-doped carbon cubes structure adorned with highly external Fe−N x was designed and produced by the space-confined induced strategy. The optimal electrocatalyst revealed excellent ORR activity in both alkaline and acidic electrolytes, with half-wave potentials of 0.86 and 0.75 V, respectively. The superior performance arose from its unique concave structure, possessing more accessible active sites with improved intrinsic activity, which holds promising potential for preparing advanced ORR electrocatalysts.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Xuan Jiang,Zhaodong Nan
Multiple oxidation states of first-row transition-metal cations were always doped in g-C3N4 to enhance the catalytic activity by the synergistic action between the cations in the Fenton-like reaction. It remains a challenge for the synergistic mechanism when the stable electronic centrifugation (3d10) of Zn2+ was used. In this work, Zn2+ was facilely introduced in Fe-doped g-C3N4 (named xFe/yZn-CN). Compared with Fe-CN, the rate constant of the tetracycline hydrochloride (TC) degradation increased from 0.0505 to 0.0662 min–1 for 4Fe/1Zn-CN. The catalytic performance was more outstanding than those of similar catalysts reported. The catalytic mechanism was proposed. With the introduction of Zn2+ in 4Fe/1Zn-CN, the atomic percent of Fe (Fe2+ and Fe3+) and the molar ratio of Fe2+ to Fe3+ at the catalyst’s surface increased, where Fe2+ and Fe3+ were the active sites for adsorption and degradation. In addition, the band gap of 4Fe/1Zn-CN decreased, leading to enhanced electron transfer and conversion from Fe3+ to Fe2+. These changes resulted in the excellent catalytic performance of 4Fe/1Zn-CN. Radicals •OH, •O2–, and 1O2 formed in the reaction and took different actions under various pH values. 4Fe/1Zn-CN exhibited excellent stability after five cycles under the same conditions. These results may give a strategy for synthesizing Fenton-like catalysts.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Mengzhen Song,Jingru Han,Yingzhi Wang,Lungang Chen,YanYan Chen,Xiaoyuan Liao
Fe-based MOFs (Fe-MOFs) are deemed promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, their inferior catalytic activity, iron leaching, and low H2O2 utilization always hinder their application as Fe-based MOF catalysts. In this work, we manipulated the structure of Fe-oxo nodes in MIL-88B(Fe) via a CuI species substitution method, affording a mixed-valence (Cu-incorporated Fe-MOFs) with highly improved Fenton-like performance. It is found that the CuI serves as a shuttle to promote transfer between FeII/FeIII, inducing the formation of a larger amount of stable FeII sites, which was proven by experimental and DFT calculation results. A linear relationship was observed for the Fenton-like performance and the amount of CuI species for the catalysts. The corresponding value of the •OH formation is 2.17 eV for Cu-incorporated MIL-88B(Fe), which is significantly lower than that of MIL-88B(Fe) (2.69 eV). Meanwhile, the enriched CuI species suppress Fe species leaching during the catalytic reaction. The Fe-ion leakage of 0.4Cu@MIL-88B is very tiny (0.01–0.03 mg/L), significantly less than that of MIL-88B (2.00–3.02 mg/L). At the same time, H2O2 utilization for 0.4Cu@ MIL-88B(Fe) is 88%, which is almost 4.4 times that of pure MIL-88B(Fe). This work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for wastewater treatment.
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FIBERS AND POLYMERS
·
2023
·Vol. 24
·期 6
·1983-1994
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IF 2.5
Feng Jiangli,Sun Hui,Yu Bin,Yang Xiaodong,Xu Lei,Liu Peng,Cui Xiaogang
A kind of NH 2 -MIL-101(Fe)@viscose spunlaced nonwoven material (VSN) was prepared by in situ solvothermal method for the adsorption of organic dyes in wastewater and then carbonized in a tube furnace under N 2 atmosphere at 300 °C to improve the adsorption performances. The results showed that the synthesized NH 2 -MIL-101(Fe) particles with a polyhedral structure were uniformly loaded on the VSN surface. After being carbonized, the NH 2 -MIL-101(Fe)@viscose spunlaced nonwoven porous carbon material (VSNC) were obtained. Compared with uncarbonized NH 2 -MIL-101(Fe)@VSN, the adsorption efficiency of NH 2 -MIL-101(Fe)@VSNC for methylene blue (MB) significantly enhanced and could reach 98.3% under the condition of water bath temperature of 30 °C and pH 9. According to adsorption thermodynamic analysis, the MB adsorption process by NH 2 -MIL-101(Fe)@VSNC was spontaneous. The quasi-secondary adsorption kinetic model was more suitable to describe the whole adsorption process of NH 2 -MIL-101(Fe)@VSNC, implying that the adsorption mechanism of NH 2 -MIL-101(Fe)@VSNC for MB was mainly chemical adsorption. NH 2 -MIL-101(Fe)@VSNC presented good structure stability and reusability during the adsorption process. After being recycled five times, the MB adsorption efficiency still maintained about 86.3%.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Donghuan Meng,Ye Lei,Menghan Pang,Jianrong Qiu,Chenghua Fan,Yuyan Feng,Dongbo Wang
In the graphitic carbon nitride-based photocatalytic reaction, the redox ability and electron transport ability of photocatalyst have an important influence on its activity. The Photo-Fenton reaction system was constructed by modifying N-doped carbon quantum dots (N-CQDs) on the surface of supramolecular self-assembled carbon nitride and introducing Fe ions into the carbon nitride planar structure . The xFe/N-CQDs/MCN1 catalysts with different iron contents were prepared, which had significant degradation effect on organic pollutants . Among them, 0.2Fe/N-CQDs/MCN1 degraded 76% of ciprofloxacin (CIP) within 120 min. Various characterizations demonstrate that photocatalytic activity are enhanced due to the surface modification of N-CQDs enhancing electron transfer rate on the surface of photocatalysts and the doping of Fe ions providing active sites for Fenton reaction . At the same time, the formation of chemical bonds limits the leaching of iron and avoids secondary environmental pollution . These results indicate that the novel catalyst has excellent application potential in the field of environmental photocatalysis .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chengcheng Xu,Jing Deng,Shijun Zhu,Xiao Ling,Songtu Shen,Hongguang Guo,Qiongfang Wang,Xueyan Li
The introduction of ascorbic acid (AA) into Fe(III)/PS system exhibited extremely high activity on the removal of N,N-diethyl- meta -toluamide (DEET) and other pollutants. The removal efficiency of DEET within 30 min reached 90.13%, its dynamic curve obeyed second-order kinetic model and the k obs was calculated to be 0.150 L·mg −1 ·min −1 . Compared with other reducing agents, AA was tested to be the most suitable. The optimal dosages of Fe(III), PS and AA were tested to be 0.1, 1.0 and 0.5 mM, respectively. Furthermore, the introduction of AA extended the working pH to 2.5–9.3. Common anions posed different degrees of inhibition on DEET degradation at relatively high concentration, while a small dosage of HCO 3 − (<1 mM) abnormally exerted a positive role. In terms of reaction mechanism, scavenger experiment and EPR observation illustrated that ·OH and ·SO 4 − dominated DEET degradation, yet slight Fe(Ⅳ) was also found during the reaction, which indicated that Fe(Ⅳ) may also contribute to DEET removal. Different from the rapid consumption of Fe(II) in Fe(II)/PS system, Fe(II) in Fe(III)/PS/AA system entered a dynamic equilibrium state in the later stage of the reaction, which can decompose PS to form ·SO 4 − continuously. Furthermore, the reduction and chelation ability of AA both functioned a key role. According to the degradation intermediates identified by LC-MS analysis, the degradation pathways of DEET could be divided into two directions, which covered opening benzene ring and removing side chain.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Chengbao Liu,Dongchen Shen,Zhengkai Tu,Song Li
Li + doping is regarded as an effective strategy to enhance the room-temperature hydrogen storage of metal-organic frameworks (MOFs). In this work, Li + is doped into both MIL-100(Fe) and MIL-100(Fe)/graphene oxide (GO) composite, and it is demonstrated that the hydrogen uptake of Li + doped MIL-100(Fe)/GO (2.02 wt%) is improved by 135% compared with Li + doped MIL-100(Fe) (0.86 wt%) at 298 K and 50 bar, which is ascribed to its higher isosteric heat of adsorption (7.33 kJ/mol) resulting from its more accessible adsorption sites provided by doped Li + ions and ultramicropores. Grand canonical Monte Carlo (GCMC) simulation reveals that Li + ions distributing in the interface between MIL-100(Fe) and GO within MIL-100(Fe)/GO composite is favorable for hydrogen adsorption owing to the increased number of adsorption sites, thus contributing to the enhanced hydrogen storage capacity. These findings demonstrate that MIL-100(Fe)/GO is a more promising Li + doping substrate than MIL-100(Fe).
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2021
·
IF 6.789
Zixuan Zhang,Jingfang Li,Yunliang Zhao,Tong Wen,Tingting Zhang,Shaoxian Song
In this work, the iron-containing smectite nontronite (NNT) was artificially prepared by hydrothermal process and used as a heterogeneous catalyst to activate bisulfite (BS) for degradation of tetracycline (TC). Two NNT samples with different iron content (NNT1 and NNT2) were characterized by XRD, FTIR, XPS and SEM-EDS analysis. Under dark condition, the TC removal rates of NNT1/BS and NNT2/BS reached about 91.7% and 95.5% respectively at 60 min. Due to the heterogeneous catalysis of structural Fe(III), the NNT catalysts showed great catalytic activity and low iron leaching at the pH range 3.0–7.5. In addition, NNT particles were also stable and reusable in activating BS for TC removal. According to the EPR and radical quenching experiments, it could be proved that the precursor radical • SO 3 ˉ was first generated in NNT/BS system, then • SO 4 ˉ and • OH were the active species that played a role in TC degradation . The synthetic NNT clay is a promising Fe-based catalyst for treatment of TC wastewater thanks to its high activity, good stability and effective reusability .
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 24
·7943-7954
·
IF 6.119
Hao Zhang,Xiaojing Song,Hao Sun,Zhenyu Lei,Shouxin Bao,Chen Zhao,Dianwen Hu,Wenxiang Zhang,Jingyao Liu,Mingjun Jia
Developing highly efficient and durable eco-friendly heterogeneous catalysts for the Friedel–Crafts acylation (FCA) reaction has been a long-term and significant target, yet remains a great challenge. Herein, a series of Fe–Ni alloy nanoparticles (NPs) encapsulated inside N-doped carbon spheres (FexNi1−x@NC) was rationally fabricated by pyrolyzing the Fe–Ni bimetallic metal–organic frameworks (BMOFs-FexNi1−x) to this end. Various characterization results demonstrated that FeNi alloy NPs (25 nm) covered by a thin carbon shell (5 nm) were uniformly distributed throughout the entire carbon-based composite. A number of oxidized metal species (Fe3+, Ni2+) are present on the surface of the inner bimetallic core, which should be the main source of catalytically active centers of the carbon-wrapped metal NP catalysts. The composition-optimized Fe0.8Ni0.2@NC with relatively higher positive surface charges exhibited the highest catalytic activity and excellent stability for the acylation of aromatic compounds with acyl chlorides. The density functional theory calculations revealed that the catalytic activity of the FexNi1−x@NC catalysts could arise from the electron transfer, i.e., from the outermost layer of the carbon shell to the inner positively charged Fe-based metal NPs, which can lead to a positive charge distribution (by acting as weak Lewis acid sites) on the external surface of the carbon-encapsulated metal NP catalysts. In this case, the external carbon shell can function as ‘chainmail’ to transfer the Lewis acidity (positive charge), and also to protect the inner metal core from the destructive reaction environment, thus resulting in the formation of highly efficient and durable FCA catalysts.
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