SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Jia Deng,Weiguo Chen,Feng Wu,Yitao Dai,Dionysios D. Dionysiou,Li-Zhi Huang
Peroxymonosulfate (PMS)-based advanced oxidation processes have become promising water treatment technologies in recent years. The redox cycle between transitional metals in heterogeneous catalysis is essential for continuous activation of PMS and efficient removal of pollutants. In this work, we prepared Fe 3 O 4 using precipitation method and subsequently added Ni aqueous solution to synthesize Ni-Fe (hydr)oxides. Ni-Fe (hydr)oxides show efficient PMS activation ability, causing the degradation of 96.8 % trichloroethylene (TCE) after 40 min with the dosage of Fe, Ni and PMS at 0.2, 0.1 and 0.2 mM, respectively. The catalyst concentration normalized TCE degradation rate constant of Ni-Fe (hydr)oxides/PMS system reaches 1.48 L g −1 min −1 . Nonradical pathway is dominant at the initial stage of the reaction which generates high-valent metals, SO 5 • − and indirectly produces 1 O 2 . 1 O 2 and dissolved O 2 together participate in the O 2 cycling, •OH generation, and electron transfer involving the reduction of trivalent metals. Divalent metals react with PMS to generate strong oxidative •OH and SO 4 • − through radical pathway in later stage. TCE is degraded and dechlorinated by multiple reactive species in Ni-Fe (hydr)oxides/PMS system. The optimum Ni/Fe ratio of catalysts under the studied conditions was 0.50. Ni-Fe (hydr)oxides show high reactivity and stability in real water matrices, demonstrating Ni-Fe (hydr)oxides are promising catalysts for PMS activation to degrade pollutants in contaminated water.
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INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Qi Gao,Yuyu He,Liangmeng Ni,Hao Ren,Mengfu Su,Shaowen Rong,Zhijia Liu
Fe-N-modified activated carbons (ACs) were prepared from bamboo shoot shells (BSS) by potassium ferrate activation for arsenic adsorption. BSS provided abundant nitrogen and carbon sources for ACs, while potassium ferrate significantly improved the pore volume and specific surface area (SSA), but also loaded iron particles. The highest SSA of AC was 1900 m 2 /g, with the iron content of 4.54–6.52% and nitrogen content of 2.88–3.35%. Based on the arsenic adsorption capacity, the optimized manufacturing process was activation temperature of 800 °C, activation time of 120 min, and activator ratio of 3.5. The optimized AC exhibited excellent arsenic adsorption performance and the maximum adsorption capacity was 9.18 mg/g. The good magnetism of AC was beneficial to recovery and reuse. The adsorption capability retention was still more than 50% after reusing for five times. This work showed that BSS had great potential for commercial development, and also provided a cost-effective production way for arsenic adsorbents.
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Electrocatalysis
·
2023
·Vol. 14
·期 5
·776-787
·
IF 3.1
Zheng Yingping,Yu Dehua,Zhang Ke,Xu Wei,Ma Kaili,Wang Yuhang,Lou Yongbing
As a representative anodic reaction, the oxygen evolution reaction (OER) is often combined with hydrogen evolution, carbon dioxide reduction, and other cathodic reactions. Bimetallic selenides can satisfy the requirement of efficiency and economy for OER. However, the OER performance of Fe-Co-Se is less than satisfactory, restricted by the limited inherent active sites. Therefore, by doping P into Fe-Co-Se, the electron density and mass transfer were successfully adjusted. The 3D dandelion-like flower Fe-Co-Se-P/CC showed η 10 of 210 mV and the 45.3 mV dec −1 Tafel slope better than Fe-Co-Se/CC and RuO 2 . Experimental investigations demonstrated that outstanding OER activity was ascribed to the double modulation influences of P dopant both in electron environment and morphology which could not only improve conductivity but also enrich catalytic reactive sites. This work presents another choice for the design of a transition metal OER catalyzer and propels the development of electrocatalytic oxygen production to higher efficiency and lower cost. Graphical Abstract 3D dandelion-like flowers Fe - Co-Se-P structure anchored on carbon cloth has been firstly synthesized as economy and efficient OER electrocatalyst, which displays outstanding catalytic perform ance (equipped with 210 mV low overpotential at η 10 ) and stability benefited from the double modulation effect of P doping on the electronic environment and morphology.
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Energies
·
2023
·Vol. 16
·期 9
·3684
·
IF 3.2
Ruimin Zhang,Ke Wang,Peng Wang,Yan He,Zhiming Liu
Single-atom catalysts (SACs) within carbon matrix became one of the most promising alternatives to noble metal-based catalysts for oxygen reduction reaction (ORR). Although SACs have significant benefits in reducing the total catalyst cost, it also has the disadvantages of weak interaction between atoms and poor stability. Hence, there is still much room for improvement for the catalyst activity. In response, we designed a Fe-Co-Pt ternary metal single atom catalyst anchored on covalent organic framework (COF)-derived N-doped carbon nanospheres (Pt, Fe, Co/N-C). Due to effective charge transfer between Pt single atom and neighboring Fe-Co components, an intense electron interaction can be established within the Pt, Fe, Co/N-C catalyst. This is beneficial for enhancing charge transfer efficiency, modulating d electronic structure of Pt center and weakening oxygen intermediate adsorption, thus distinctly accelerating ORR catalytic kinetics. As expected, the half-wave potential of Pt, Fe, Co/N-C was 0.845 V, much higher than those of commercial 20 wt% Pt/C (0.835 V), Pt/N-C (0.79 V) and Fe, Co/N-C (0.81 V) counterparts. Moreover, the Pt, Fe, Co/N-C catalyst demonstrated much-improved cycling stability and methanol tolerance.Keywords:oxygen reduction reaction;electrocatalysts;single atom;ternary metal;kinetics
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Polymers
·
2023
·Vol. 15
·期 13
·2918
·
IF 5
Cheng Tang,Tao Hu,Chengzhen Du,Ziqin Liao,Wenyan Cheng,Fen Wang,Xiaoli Hu,Kunpeng Song
A Fe-N conjugated organic polymer (SMP-Fr-Py) was prepared from ferrocene and pyrrole using a Scholl coupling reaction, which significantly improved the performance of Cr(VI) removal compared to the polymer (HCP-Fr-Py) prepared by adding the cross-linker formaldehyde dimethyl acetal (FDA). The results showed that at a pH of 2 and at 25 °C, the removal of Cr(VI) reached 90% for SMP-Fr-Py and only 58% for HCP-Fr-Py after 20 min of reaction. Subsequently, 99% and 78% were achieved after 120 min of reaction, respectively. The test results showed that the removal reaction followed a pseudo-second-order kinetic model. The removal efficiency decreased with increasing solution pH and initial Cr(VI) concentration, but increased with increasing SMP-Fr-Py dosage, reaching three cycles. The characterization of the reaction complexes and measurements of Cr species conversion revealed the near absence of Cr(VI) species in the solution. Approximately 38% of Cr(VI) was found to be adsorbed on the material surface, with another fraction present in solution (24%) and on the material surface (38%) in the form of Cr(III). The overall study showed that the direct connection of ferrocene and pyrrole in SMP-Fr-Py through C-C bonding increased the conjugated structure of the polymer backbone, which facilitated electron transfer and transport. Furthermore, the Fe-N elements worked synergistically with each other more easily, which improved the removal performance of Cr(VI) and provided a reference for the subsequent work.Keywords:organic polymers;Fe-N co-doping;Cr(VI) removal;conjugate structure
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Jingjuan Lai,Fengyu Guo,Li Wang,Chunxia Zhao,Dong Xiang,Hui Li,Bin Wang,Peng An,Zhenyu Li,Hongwei Zhou,Yuanpeng Wu
With the acceleration of the industrial process, oil-water separation is an urgent problem for oil spill accidents and wastewater treatments. Exploiting superhydrophobic materials applied in harsh environments and remote drives remains a significant challenge in solving oil moisture problems. An alternative strategy to solve this problem has been demonstrated by decorating poly lauryl methacrylate (LMA) on Fe foam via the solution polymerization method. The as-prepared Fe foam possesses good superhydrophobicity (>150°) under broad pH (1 < pH < 12) and a wide temperature range (−55°C-180 °C). Furthermore, outstanding separation efficiency (>99.1%), high cycle stability (>50 times), and high oil flux (63.7–114.6 kL m −2 h −1 ) against diverse oil/water mixtures can be realized under gravity. Interestingly, oil harvesting capacity above or beneath the water can be realized by remote magnetic driving as well.
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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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Journal of Materiomics
·
2023
·
IF 9.4
Ying Wang,Li Jin,Shiyang Hua,Zhe Zhao,Zhijia Xiao,Chunyan Qu,Jiayuan Huang,Gaoshan Huang,Xinyi Ke,Zihan Lu,Ji Tan,Xuanyong Liu,Yongfeng Mei
Precise assembly of active component with sophisticated confinement in electrocatalyst are promising to increase the active site exposure for enhanced hydrogen evolution reaction (HER). Here, PCN-333 films with mesopores are firstly assembled on titanium carbide MXene with the assistance of atomic layer deposited oxide nanomembrane. With the whereafter pyrolysis process, the composite is converted to N-doped porous carbon multi-layer containing Fe nanoparticles. The strong confinement of Fe active particle in carbon as well as great contact between metal and carbon effectively enhance active site exposure. Furthermore, this multi-layer porous structure provides high specific surface area and plentiful mesopores for electrolyte penetration. Due to the structural advantage, the composite can be well functioned in both acid and alkaline electrolytes with excellent HER performance, e.g. , low overpotential/Tafel slope. The present work may have great potential in developing high efficiency transition-metal based electrocatalysts.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Mengting Zhu,Ruli Xu,Xueyang Wang,Jie Liu Qianli Zhang,Jie Wei
Four Fe-based metal-organic frameworks (MIL-101(Fe), MIL-53(Fe), MIL-88(Fe), and MIL-100(Fe)) were synthesized using a solvothermal method, and further characterized by X-ray diffraction, Fourier transforms infrared spectroscopy, Scanning electron microscopy, and X-ray photoelectron spectroscopy. The synthesized Fe-MOFs were used to fabricate the modified carbon paste electrodes (CPE) for simultaneous detection of hydroquinone and catechol. Among the MILs (Fe) modified CPEs, MIL-101(Fe)/CPE exhibited extraordinary electrochemical sensitivity because of MIL-101 (Fe)’s excellent conductivity. The oxidation potential separation of hydroquinone and catechol achieved 190 mV. Compared with CPE, the oxidation currents of hydroquinone and catechol at MIL-101/CPE were 10-fold higher and the reduction currents were 5-fold higher. The linear range was 2 - 90 μM for hydroquinone and 2 - 100 μM for catechol, and the detection limit was 0.58 μM and 0.62 (S/N = 3) μM for hydroquinone and catechol. Furthermore, the application of MIL-101 (Fe)/CPE has been validated in an actual river water sample with the satisfied recoveries of 90.21 - 102.36% and 91.11 - 102.19% for hydroquinone and catechol, respectively.
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Journal of Environmental Chemical Engineering
·
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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FIBERS AND POLYMERS
·
2023
·Vol. 24
·期 6
·1983-1994
·
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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ENVIRONMENTAL TECHNOLOGY
·
2023
·
IF 2.8
Yi Ding,Min Zhang,Sijie Zhou,Linbei Xie,Ao Li,Ping Wang
Ferrous iron (Fe(II)) reacts with peroxymonosulphate (PMS) to form active oxidants that can degrade refractory organic pollutants. However, the conversion rate of Fe(III) to Fe(II) is slow, which limits its actual application. In the study, the effect of fulvic acid (FA) on the degradation of dimethyl phthalate (DMP) by Fe(II)/PMS was investigated. Moreover, the degradation process of DMP was predicted by the preliminary identification of active free radicals and intermediates. As expected, FA gave rise to a higher concentration of Fe(II) than that in Fe(II)/PMS to enhance the removal of DMP in Fe(II)/PMS system. The precipitate, involved in FA and iron, was an important composite to promote the degradation of DMP in the system. Also, the response surface methodology (RSM) was applied to model and optimize the degradation conditions of DMP. The highest removal efficiency (85.70%) was obtained at pH = 3.86, [PMS] = 0.96 mM, [FA] = 11.44 mg/L and [DMP] = 5 µM. The results of free radical quenching experiments and EPR showed that •OH and SO4•− were the main active radicals in this system. The degradation intermediates of DMP were monomethyl phthalate (MMP), phthalic acid and benzoic acid. Discoveries of this study had raised the current understanding of the application of FA keeping the cycles of Fe(II)/Fe(III) for peroxymonosulphate activation, which could afford valuable information for the degradation of organic pollutants by FA/Fe(II)/PMS.
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