Polymers
·
2023
·Vol. 15
·期 13
·2918
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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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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tong Zhang,Yuan Chen,Yurong Zhang,Bin Liu,Yuanyuan Liu,Jianwei Zhao
Cr(VI) and catechol are common pollutants in wastewaters of tannery industry. Cr(VI) reduction by catechol results in accumulation of Cr(V)-complex and toxic o -benzoquinone. Cr(VI) reduction can be enhanced by accelerating the electron transfer from catechol to Cr(VI) using Fe(III). This electron transfer allows the continuous production of reactive oxygen species (ROS) in advanced oxidation processes, which further degrades catechol. However, the effects of catechol on Fe(III)-based Cr(VI) reduction and ROS production are not clear. In this study, the electron transfer pathway between catechol, Fe(III) and Cr(VI) was investigated along with the catechol degradation by ROS. Results show that the process of Cr(VI) reduction follows well a pseudo-second-order kinetic model, and the activation energy decreases by 4189 J/mol after electrons are transferred by Fe(III). Aqueous chromium (50 mg/L) was completely precipitated as Cr(OH) 3 , Fe x Cr 1-x (OH) 3 or Fe(OH) 3 -Cr(OH) 3 at Fe(III) concentration of 10 mmol/L. Residual catechol and Fe(II) in wastewater activated percarbonate, thereby producing OH for over 480 min at pH 3.0 and generating OH and CO 3 − for over 5 min at pH 10.0. Catechol was degraded by these ROS to butenedioic, oxalic, and formic acids, which were then mineralized to H 2 O and CO 2 . Catechol (2 mmo/L) was fully removed from wastewater with TOC removal of 37%, and the degradation was not affected by SO 4 2− and Cl − . This study provides new insights into the removal of pollutants from wastewaters via electron transfer mediated by Fe(III), and may aid in controlling the toxic effects of Cr(VI) and catechol-like organics in natural and engineered aquatic systems.
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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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Nature Communications
·
2022
·Vol. 13
·期 1
·1-9
·
IF 17.694
Zhang Xiaoran,Zhu Xiaorong,Bo Shuowen,Chen Chen,Qiu Mengyi,Wei Xiaoxiao,He Nihan,Xie Chao,Chen Wei,Zheng Jianyun,Chen Pinsong,Jiang San Ping,Li Yafei,Liu Qinghua,Wang Shuangyin
Electrocatalytic urea synthesis emerged as the promising alternative of Haber–Bosch process and industrial urea synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe–Ni pairs can significantly improve the efficiency of electrochemical urea synthesis. Compared with isolated diatomic and single-atom catalysts, the bonded Fe–Ni pairs act as the efficient sites for coordinated adsorption and activation of multiple reactants, enhancing the crucial C–N coupling thermodynamically and kinetically. The performance for urea synthesis up to an order of magnitude higher than those of single-atom and isolated diatomic electrocatalysts, a high urea yield rate of 20.2 mmol h −1 g −1 with corresponding Faradaic efficiency of 17.8% has been successfully achieved. A total Faradaic efficiency of about 100% for the formation of value-added urea, CO, and NH 3 was realized. This work presents an insight into synergistic catalysis towards sustainable urea synthesis via identifying and tailoring the atomic site configurations.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2022
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IF 3.428
Zihao Hu,Huiqi Wu,Fang Zhu,Sridhar Komarneni,Jianfeng Ma
MIL-101(Fe)/Co 3 O 4 composites were synthesized using a facile solvothermal method to establish the superiority of a heterogeneous photochemical catalysis system in the presence of Na 2 S 2 O 8 with visible light irradiation. In the present system, the MIL-101(Fe)/Co 3 O 4 catalyst showed better catalytic performance than the single photocatalytic or chemical catalytic system, implying that the MIL-101(Fe)/Co 3 O 4 catalyst can combine both photocatalysis and chemical catalysis well. When tetracycline (TC) is the target pollutant, the highest degradation efficiency can be achieved within 40 min, reaching to 86 %. Crystallinity, morphology, and elemental valence of the MIL-101(Fe)/Co 3 O 4 composite were explored by using X-ray diffraction (XRD), scanning electron microscopy (SEM) as well as X-ray photoelectron spectroscopy (XPS). From the quenching experiments, it was found that 1 O 2 , SO 4 ‾, OH, and O 2 ‾ make contributions to the effective removal of tetracycline. Apart from that, the recovery and reuse characteristics of MIL-101(Fe)/Co 3 O 4 may facilitate the sustainable wastewater treatment.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Wenjing Zhao,Peng Wang,Fan Zhang,Yinshen Liu,Xuan Jin,Shijun Yuan,Qi Fan,Xing Guo,Qingyu Xu
Cation-disordered rock-salt cathodes have attracted extensive attention due to their high capacity and energy density . However, the excessive redox reaction of O 2- causes a severe impairment of Ni capacity and the release of O 2 , leading to the poor cycle stability and voltage decay for Li-Ni-Nb-O cathodes. In our work, the oxyfluoride compounds Li 1.23 Ni 0.3 Nb x Fe y O 2- z F z with various doping concentrations of Fe and F are successfully synthesized by solid state reaction using high-energy ball milling. Apart from observing the plateau at around 4 V with the redox reaction of Ni, a new plateau at approximately 2.6 V is observed due to the redox reaction of Fe. The doping of Fe on Nb increases the discharge capability and the co-doping of F on O further improves cycle stability. With the optimized doping amount of Fe ( y = 0.16) and F ( z = 0.15), Li 1.23 Ni 0.3 Nb 0.30 Fe 0.16 O 0.85 F 0.15 can deliver a discharge capacity of 347.1 mAh/g at a current density of 20 mA/g after the activation process in subsequent cycles. After 20 cycles at 20 mA/g, the capacity retention is 181.6 mAh/g, and after 100 cycles at 50 mA/g, the discharge capacity remains 102.2 mAh/g.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 46
·17787-17794
·
IF 4.569
Pengjun Li,Zili Li,Xirui Miao,Haoting Hou,Mao Wang,Xudong Yang
It has become a significant problem to develop and improve carbonized polymer dot (CPD)-based fluorescence sensors with environmental detection features. In this study, fluorescent “turn on” sensors of CPDs were prepared by a one-step hydrothermal method using o-phenylenediamine (o-PD) and ferric chloride (FeCl3) as raw materials. Fe-doped CPDs exhibited excellent fluorescence properties, stability, and the sensitive and selective “turn on” detection of hydrazine hydrate (N2H4·H2O). In this detection system, Fe3+ acts as an effective fluorescence inhibitor that inhibits the yellow fluorescence emission from CPDs, while Fe3+ is reduced upon the addition of the N2H4·H2O reducing agent. The fluorescence intensity of CPDs gradually increased with the increasing concentration of N2H4·H2O, while the limit of detection (LOD) could reach 0.168 μM. In addition, CPD-based polyvinyl alcohol (CPDs@PVA) films were also prepared, which still maintained excellent sensitivity to N2H4·H2O. The results show that CPDs and their composite films can detect N2H4·H2O with good detection performance.
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Chenguang Wang,Chengyan Wen,Zheng Liang,Zhipeng Tian,Qian Jiang,Yuhe Liao,Xunzhu Jiang,Lungang Chen,Qiying Liu,Longlong Ma,Michiel Dusselier
Direct conversion of syngas to aromatics has great potential to decrease fossil fuel dependence. Here, a unique structured hybrid catalyst composed of Fe 3 O 4 nanoparticles intimately dispersed inside an acidic zeolite is developed. 1 to 4 nm sized Fe 3 O 4 nanoparticles end up evenly dispersed in an acidic and slightly mesoporous Al-ZSM-5 based on Fe 3 O 4 restructuring during co-hydrothermal synthesis using organosilane modification. A very high aromatic productivity of 214 mmol aromatics h −1 g Fe −1 can be obtained with a remarkable 62% aromatic selectivity in hydrocarbons. This catalyst has excellent sintering resistance ability and maintains stable aromatics production over 570 h. The synthetic insights that postulate a mechanism for the metastable oxide-zeolite reorganization during hydrothermal synthesis could serve as a generic route to sinter-resistant oxide-zeolite composite materials with uniform, well-dispersed oxide nanoparticles in close intimacy with - and partially confined in - a zeolite matrix.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Wenjuan Wang,Yanfang Huang,Junpeng Zuo,Lulu Kou,Bingbing Liu,Hu Sun,Guihong Han
Microfine metal–organic frameworks (MOFs) are promising adsorbents for water treatment, but their commercial applicability is severely constrained by poor separability. Herein, we designed a feasible bubble flotation strategy for achieving the effective separation of oxyanions-loaded Fe-MOF particles in the solution after adsorption, by modifying the particle interface properties and introducing bubbles mineralization. The results showed that the separation of P(V), Mo(VI) and W(VI) oxyanions-loaded Fe-MOF could be completely achieved under optimum conditions. FTIR, XPS and DFT analyses revealed that the particle size and hydrophobicity of oxyanions-loaded Fe-MOF increased by sodium dodecyl sulfate (SDS) collector via chemisorption and electrostatic interactions. The collision and attachment models analysis of bubbles with particles demonstrated that the separation efficiencies of collector modified oxyanions-loaded Fe-MOFs were significantly enhanced with increasing bubble mineralization. EDLVO theoretical calculations and bubble-particle carrying ability analysis demonstrated that the gravitational interactions between oxyanions-loaded Fe-MOF particles and particles/bubbles were intensified by the collector. The gravitational interaction further induced particle aggregation and enhanced the carrying capacity of individual bubbles. This work provides a feasible strategy for the removal of oxyanions and the separation of oxyanions-loaded microfine Fe-MOF in the adsorption process.
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International Journal of Environmental Research and Public Health
·
2022
·Vol. 19
·期 22
·14835
·
IF 4.614
Jinkai Shu,Bozhi Ren,Wei Zhang,An Wang,Sen Lu,Shuyu Liu
Modified Shell Powder/La-Fe-TiO2(La-Fe-TiO2@MSP) composites were fabricated using the sol-gel method and characterized by SEM, XRD, UV-vis DRS and photocurrent techniques, and their physicochemical and optical properties were analyzed. The effects of various factors on the photocatalytic degradation of pyridine and its reaction kinetics were investigated by batch experiments using pyridine, a typical nitrogen-containing heterocyclic compound in coal chemical wastewater, as the target removal species. The pyridine degradation rate of 80.23% was obtained for 800 mg/L composite solution by photocatalytic oxidation of 50 mg/L pyridine wastewater for 180 min at 35 °C, pH = 8 and light intensity of 560 W. The photocatalytic degradation performance was optimal. The quenching experiments determined that the active species of photodegradation were mainly hole and hydroxyl radicals, and the photocatalytic degradation mechanism was analyzed in this way.Keywords:La-Fe-TiO2@MSP;photocatalysis;pyridine;reaction kinetics
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FUEL
·
2022
·
IF 8.035
Hui Li,Tianyu Wang,Yangyang Wang,Fengsheng Liu,Yan Li,Yunpu Wang,Min Guo,Guoning Li,Xiaoling Ma
Sulfated metal oxides are widely used in catalyzing esterification for biodiesel production due to their low corrosivity and easy separation. While, the catalytic stability is still a challenge on account of active site leaching during successive batch experiments. To this end, the typical metal organic frameworks, MIL-100(Fe) doped with Co was adopted to load ammonium sulfate ((NH 4 ) 2 SO 4 ) for stable heterogeneous acid preparation, which was employed to catalyze the esterification of methanol and oleic acid. Influence of preparation factors of (NH 4 ) 2 SO 4 loading amount and activation temperature on catalytic activity were initially evaluated. Furthermore, to elucidate the effect of Co doping, catalysts were characterized by TG, XRD, FTIR, nitrogen adsorption–desorption, Py-FTIR, XPS, SEM and NH 3 -TPD. Results indicated that the maximum esterification conversion of 92.56 % was achieved by MS(Fe/Co) with molar ratio of methanol to oleic acid of 8:1 and catalyst amount of 8 wt% at 70 °C in 2 h. In comparison to MS(Fe), Co doping significantly improved the stability, where the catalytic activity of MS(Fe/Co) was increased by 20 % at the fifth cycle. The activation energy and pre-exponential factor of esterification catalyzed by MS(Fe/Co) were also calculated as 42.06 kJ/mol and 5.24 × 10 5 min −1 . This study provides a feasible way to enhance the catalytic stability of heterogeneous acid for biodiesel production.
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RENEWABLE ENERGY
·
2022
·
IF 8.634
Ying Li,Shengli Niu,Yanan Hao,Wenbo Zhou,Jun Wang,Jiangwei Liu
In this work, the catalytic performance of the mesoporous SrTi 1- x Fe x O 3 ( x = 0.05, 0.10, 0.15 or 0.20) for biodiesel production from palm oil with a high acid value is investigated. The physicochemical properties of the catalysts are revealed by various characterization methods, including XRD , N 2 adsorption-desorption, XPS , Raman, EPR, SEM-EDS, and CO 2 /NH 3 -TPD. Fe doping results in many oxygen vacancies in the perovskite structure , which increases the electron density of the active sites on the surface and promotes the polarization of the perovskite structure, thus improving the catalytic activity of the catalyst. The most oxygen vacancies and the best catalytic performance are observed in the SrTi 0.85 Fe 0.15 O 3 catalyst, where the FAME yield of 97.52% is achieved with the catalyst concentration of 5 wt % and methanol to oil molar ratio of 18:1 at 150 °C for 3 h. Meanwhile, the catalyst maintains a FAME yield of 83.59% for the fourth reused cycle. Also, the catalyst exhibits strong resistance to FFAs, where the FAME yield is still 93.58% even with oleic acid addition of 12 wt % to show the capability in catalyzing the simultaneous esterification and transesterification .
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