Biomass Conversion and Biorefinery
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2022
·
IF 4.05
Gao De,Han Feng,Waterhouse Geoffrey I. N.,Li Yan,Zhang Lili
A series of FeTPP-N/C-X catalysts were successfully prepared by adsorption of Fe tetraphenylporphine (FeTPP) onto a porous nitrogen-doped carbon (N/C) support using an ultrasonication method. The FeTPP-N/C catalysts were then used for the preparation of 5-hydroxymethyl-2-furan acid (HMFCA) by catalytic oxidation of 5-hydroxymethylfurfural (HMF) at 80 °C. The effects of reaction temperature, NaOH dosage, reaction time, and oxygen pressure on HMF conversion and HMFCA yield were systematically investigated. Under optimized testing conditions, a FeTPP-N/C-1 catalyst prepared using equal masses of FeTPP and N/C delivered a HMF conversion in water of 92.4%, with a selectivity to HMFCA of 97.2% over 6 h at an oxygen pressure of 1.0 MPa. Further, the catalyst showed good stability in five consecutive HMF oxidation tests. Based on the catalytic tests, and detailed catalyst characterization studies before and after reaction, a probable reaction mechanism was proposed for the selective oxidation of HMF to HMFCA by the FeTPP-N/C catalysts. Graphical Abstract
A series of FeTPP-N/C
catalysts were successfully prepared by the adsorption of iron
tetraphenylporphine (FeTPP) onto a porous nitrogen-doped carbon (N/C) support
using an ultrasonication method. The FeTPP-N/C catalysts were then used for the
catalytic aerobic oxidation of HMF to HMFCA. Under the optimized reaction conditions (temperature
80 °C, reaction time 6 h, O 2 pressure 1 MPa), a high HMF conversion
of 92.4% and a remarkable HMFCA selectivity of 97.2% were obtained, suggesting
that the developed noble-metal free catalyst has excellent promise for the
synthesis of valuable HMFCA from HMF.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Chengyuan Duan,Yi Feng,Yuming Xie,Meili Ding,Jianfeng Yao
A facile one-step synthetic strategy is proposed here to realize simultaneous amine-functionalized and Fe-doping modification of ZIF-8, aiming to optimize the Lewis acidic and basic properties of ZIF-8 for enhanced CO 2 adsorption and subsequent cycloaddition reaction of CO 2 and epichlorohydrin under solvent-free and relatively mild conditions (0.1 MPa and 80 °C). The obtained Fe-ZIF-8-NH 2 exhibits an improved CO 2 adsorption capacity of 63 mmol/g as compared to that of 18 mmol/g for pristine ZIF-8 and delivers a high catalytic CO 2 cycloaddition efficiency with the yield of target product of 92%, much higher than that of Fe-ZIF-8 (80%), ZIF-8-NH 2 (62%) and pristine ZIF-8 (40%). The improved performance can be attributed to the introduction of abundant –NH 2 groups and Fe-doping that enrich the Lewis acidity and basicity. Moreover, the obtained Fe-ZIF-8-NH 2 also exhibits high chemical stability and satisfactory recycling ability, which makes the obtained sample a promising catalyst for CO 2 capture and utilization.
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ChemCatChem
·
2022
·Vol. 15
·期 1
·e202201234
·
IF 5.497
Lu Lin,Guikai Zhang,Liqun Kang,Tao Yu,Yang Su,Guang Zeng,Shengqi Chu,Wenhao Luo
Graphical Methane oxidation : Highly dispersed mononuclear Fe species encapsulated by ZIF-8 (Fe-ZIF-8) afford an optimal turnover rate of ∼45 mol C1 mol Fe −1 h −1 and a formic acid selectivity of ∼97 % in the direct methane oxidation at 323 K. The direct catalytic oxidation of methane into C1 oxygenates is a promising approach for methane valorization. However, the difficulties in CH 4 activation and inhibition of over-oxidation hinder the development of efficient catalysts for this transformation. Herein, highly dispersed Fe species confined by ZIF-8 are developed for the direct transformation of methane into value-added C1 oxygenates with H 2 O 2 as oxidant at 323 K. The as-obtained Fe-ZIF-8 can afford an optimal turnover rate (TOR) of ∼45 mol C1 mol Fe −1 h −1 . Note that the selectivity to HCOOH is ∼97 %, outstanding among the reported Fe-based heterogeneous catalysts. Combined analysis of X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, ultraviolet-visible diffuse reflectance spectroscopy and 57 Fe Mössbauer spectroscopy suggests that the catalytically active sites in Fe-ZIF-8 are mononuclear six-coordinated Fe 3+ species. The confinement of mononuclear Fe species within a porous metal-organic framework material can provide an exquisite, enzyme-like performance for highly selective oxidation of methane towards formic acid under mild conditions.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2022
·
IF 8.91
Fang Guo,Yaoyin Lou,Qun Yan,Jianglei Xiong,Jiahao Luo,Chikang Shen,Dimitris V. Vayenas
For the efficient removal of the bio-refractory organic pollutants in the electronic industry wastewater, the Ni–Fe (oxides) modified three-dimension (3D) particle electrode was applied in electro-Fenton system (3D/EF), where iron ions were released from anode and deposited onto algal biochar (ABC) to prepare composite catalyst during reaction process. Firstly, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and Brunauer-Emmett-Teller (BET) analysis were applied to confirm successful fabrication of the 3D particle electrode materials . Secondly, COD removal efficiency could reach about 80%, which was about 20% higher than that in 2D/EF system, under the optimized conditions as 2.0 g/L of Ni-ABC particle electrodes, initial pH of 3, 100 mL/min of aeration intensity and 20 mA/cm 2 of applied current density. Thirdly, characterized using three-dimensional fluorescence spectroscopy and GC-MS analysis, it seemed that most of the macromolecular substances could be degraded, whereas mono-2-ethylhexyl phthalate (MEHP) was identified as the most abundant and representative compound. Finally, possible degradation pathway of MEHP in 3D/EF system was proposed including dealkylation, cleavage of C–O bond, and demethylation. Therefore, this study provides a new strategy in designing EF system employing bimetal doped biochar composite for an efficient elimination of organic pollutants within electronic industry wastewater.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Xiaojuan Feng,Yanlong Shi,Jingmei Liang,Wei Li,Xuyuan Gou
Exploring high activity, stable and low-cost electrocatalysts are of great importance for high-efficient hydrogen production via water splitting. Herein, a cactus-like Fe, P co-doped CoNi-S array was constructed via facile hydrothermal reaction and subsequently sulfuration and phosphorization process. Benefiting from the strong synergistic effects of different components, high conductivity of bimetallic sulfide, 3D cactus-like architecture with rich channels for mass/charge transport, and Fe and P co-doping with electron structure regulation, the as-prepared Fe, P-NiCo 2 S 4 /NF presents superior electrocatalytic activity with low overpotentials of 139 and 290 mV to drive the current density of 10 and 40 mA cm −2 for HER and OER, respectively. Meanwhile, it also manifests the distinguished durability for over 60 h in alkaline media. Notably, when integrating in a two-electrode electrolytic cell with Fe, P-CoNi-S, a reduced operation voltage of 1.55 V is required to reach 10 mA cm −2 , which is superior to precious metal-based Pt/C/NF//RuO 2 /NF counterparts. Impressively, it can also be driven by sustainable solar and thermal energies motivated Stirling engine. This work offers a universal strategy for designing high-activity and durable electrocatalysts by dual doping heteroatoms and synergistic interface engineering.
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FUEL
·
2022
·
IF 8.035
Chenxi Lu,Yuanzhuo Zhou,Liangzhi Li,Hongwei Chen,Lishi Yan
Catalytic production of 5-hydroxymethylfurfural (5-HMF) from glucose is a promising routine for generation of varied value-added chemicals. Herein, Mixed-Metal metal–organic frameworks (MOFs)–Fe/MIL-101(Cr) and MIL-101(Cr, Fe) obtained from post-synthesis modification and one-pot synthesis approach respectively were applied for catalytic converting glucose to 5-HMF. The synthesized Mixed-Metal MOFs were characterized by PXRD, SEM, N 2 adsorption–desorption analysis, TGA, XPS and NH 3 -TPD. Cr-and Fe-containing Mixed-Metal MOFs Fe/MIL-101(Cr) and MIL-101(Cr, Fe) presented synergistic effect with enhanced catalytic ability for glucose transformation to 5-HMF compared with typical single-metal MOFs and sulfonic acid-functionalized MOFs. Moreover, these two Mixed-Metal MOFs also presented better thermal stability than single-metal MOFs like MIL-101(Cr). Fe/MIL-101(Cr) was found to possess higher catalytic performance than MIL-101(Cr, Fe). 55.8 % 5-HMF yield was obtained with Fe/MIL-101(Cr) at 170 °C for 2 h in DMSO/water system. In addition, Fe/MIL-101(Cr) demonstrated desired recyclability for five times without incredible loss in its activity. This study provides a Mixed-Metal strategy on MOFs for improving catalytic efficiency of glucose conversion to 5-HMF.
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ChemPlusChem
·
2022
·Vol. 87
·期 10
·e202200312
·
IF 3.21
Yujun Wang,Rongxiu Tu,Chuantao Hou,Zonghua Wang
Graphical A porous Fe−N−C aerogel catalyst was synthesized by pyrolysis of porous metal-organic aerogels. The Fe−N−C aerogel shows enhanced catalytic performance for oxygen reduction reaction (ORR) under alkaline condition. The markedly enhanced ORR performance for Fe−N−C aerogel can be assigned to the synergistic catalytic effect between Fe−N catalytic sites and graphitized carbon and excellent mass transport due to the unique hierarchically porous architecture. Synthesis of Fe−N−C electrocatalysts by pyrolysis of porous materials has been shown to be a promising pathway for the oxygen reduction reaction (ORR). Metal-organic aerogels (MOAs) with unique micropores and mesopores should provide an excellent precursor for Fe−N−C electrocatalysts. This work reports a Fe−N−C aerogel synthesized by pyrolysis of MOA. The Fe−N−C aerogel shows excellent ORR performance in alkaline condition with an onset potential of 0.96 V (vs. RHE) and a limiting current density of 5.02 mA cm −2 . The markedly enhanced ORR performance for Fe−N−C aerogel can be assigned to the synergistic catalytic effect between Fe−N catalytic sites and graphitized carbon and excellent mass transport due to the unique hierarchically porous architecture. In addition, satisfactory durability and methanol tolerance were obtained, demonstrating a promising material for ORR.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Xudong Zhao,Xiangxi Wang,Lei Chen,Xianglong Kong,Zhi Li,Ying Zhao,Zhuoyan Wu,Tingyu Wang,Zhiliang Liu,Piaoping Yang
Exploring low-cost and high-activity transition metal-based electrocatalysts for oxygen evolution reaction (OER) is critical toward mass hydrogen generation by water splitting. Herein, a cheap Fe element doped flower-like nickel sulfides catalyst (Fe-NiS/NiS 2 ) is designed and synthesized through facile electrostatic adsorption and sulfuration methods. It is investigated that the Fe doping effectively induces the lattice contraction of nickel sulfides and regulates the phase composition and heterogeneous interfaces, thus enabling high intrinsic OER activity. The Fe-NiS/NiS 2 catalyst shows a high electrochemically active surface area of 150 cm 2 , a small overpotential of 361 mV at 100 mA cm −2 and a low Tafel slope of 61.5 mV dec -1 . Furthermore, the Fe-NiS/NiS 2 exhibits a very excellent structure and performance stability without current attenuation for 24 h at 1.50 V versus reversible hydrogen electrode. This work provides an important insight for the exploitation of low-cost and high-performance OER catalysts with cheap Fe element doping metal sulfides.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Ming Xiao,Ruixue Li,Jinglin Yin,Junhui Yang,Xinyu Hu,Hongbo Xiao,Wenlei Wang,Ting Yang
The treatment of arsenite pollution in water has always been concerned. Oxidation of high toxic As(III) to relatively low toxic As(V) by efficient photocatalytic oxidation technology is a research hotspot. This paper is focused on the active photocatalyst of TiO 2 @Fe 3 O 4 composites synthesized by a simple hydrothermal method for the efficient photocatalytic oxidation of As(Ⅲ). The successful construction of Ti–O–Fe interface bonds between TiO 2 and Fe 3 O 4 significantly promoted the transfer efficiency of photo-generated carriers, and further rapidly improved the photocatalytic oxidation efficiency of As(Ⅲ). The application results showed that the constructed TiO 2 @Fe 3 O 4 photocatalyst with 0.10 g Fe 3 O 4 (TF-0.10) could complete the transformation from As(Ⅲ) (10,000 μg/L) to As(Ⅴ) within 4 min with a high oxidation ratio of 100% and maintained the good properties with unchanged crystal structure after five cycles. Furthermore, the photocatalytic properties of TiO 2 @Fe 3 O 4 composites were still stable under different pH values. Electron paramagnetic resonance (EPR) consequence displayed that the superoxide radical (‧O 2 — ) and hole (h + ) were the main intermediate product in the arsenic photocatalytic oxidation system, and hydroxyl radical (‧OH) had little effect on this oxidation system. The possible mechanism of As(Ⅲ) photocatalytic conversion was further explored based on the results of the data analysis. Furthermore, this work provides a potential new idea for the practicability of efficient photocatalytic arsenic oxidation.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Zhiwen Gan,Tian Zhang,Xuanxuan An,Qin Tan,Shujun Zhen,Xiaoli Hu
Numerous ratiometric fluorescence nanozyme sensors are developed, though, fluorescence-scattering ratiometric sensors based on nanozymes are hardly reported. First-order scattering (FOS) could be quenched due to inner filter effect of quenchers on scattering signals. Meanwhile, Second-order scattering (SOS) depended on FOS. Based on the principle, we designed a novel nanozyme sensor by coupling fluorescence (FL) and SOS. Specifically, Fe-N-C nanozyme (Fe-HCNP) was fabricated by doping Fe into carbon-nitrogen polymers via formamide condensations . Fe-HCNP possessed robust oxidase-like activity, effectively transforming O 2 into ·O 2 - and ·OH. Then, Fe-HCNP and o-phenylenediamine (OPD) severed as a hybrid system to construct an FL-SOS ratiometric sensor for ascorbic acid (AA). Fe-HCNP with large size possessed strong SOS. After being added into the Fe-HCNP/OPD system, AA could fast be oxidized to dehydroascorbic acid (DAA) due to Fe-HCNP as oxidase mimics. Subsequently, fluorescent quinoxaline derivative (DFQ) was produced after condensation reactions between DAA and OPD, causing an increase in fluorescence. Meanwhile, the intensity of FOS was reduced because FOS peaks of Fe-HCNP overlapped absorption bands of DFQ, causing a decrease in SOS. The FL-SOS ratiometric sensor for AA showed outstanding advantages of high specificity and fast. Overall, this work provided a new strategy for nanozyme ratiometric sensors.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Mingzhe Li,Wenli Yao,Min Yu,Changduo Sun,Xinquan Deng,Fengjuan Chen,Lei Zhou,Yian Zheng
Hydrogels possess 3D network with abundant reactive groups, and can bind with active metal ions within their confined 3D structure for fabricating functional materials . In this study, a chitosan grafted polyacrylic acid (CTS-g-PAA) hydrogel was prepared for loading Fe 2+ , which was then converted into magnetic Fe@C via subsequent pyrolysis process . In Fe@C activated peroxymonosulfate (PMS) (Fe@C/PMS) system, the degradation behaviors of ciprofloxacin (CIP) were systematically investigated, including influencing parameters, reactive oxygen species (ROSs), degradation mechanism and potential eco-toxicity of degradation intermediates. The results showed that CTS-g-PAA supported, in-situ derived magnetic Fe@C had not only stable catalytic ability at pH 3.0–9.0, but also high degradation efficiency in the presence of inorganic Cl − and HCO 3 − (5–20 mM) as well as organic humid acid (10 and 20 mg/L). Under the optimized conditions, the degradation efficiency of CIP could reach to 96.84 % within 1 h. In Fe@C/PMS system, the main ROSs involved free radicals SO 4 •− , •OH, O 2 •− and non-free radical 1 O 2 . Through free radical quantitative experiments, the concentration of SO 4 •− and •OH at 60 min was determined respectively to be 11.84 µM and 0.14 µM, proving the dominant role of SO 4 •− . By HPLC-MS analysis, the degradation products were proposed via four degradation pathways, including hydroxylation, defluorination and decarboxylation, as well as the ring opening of quinolone and piperazine. Finally, the potential eco-toxicity of CIP and its degradation intermediates was evaluated by using ECOSAR method based on quantitative structure–activity relationships analysis.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Wenzhi Tang,Yangchun Qi,Xuewei Yang,Jianlong Wang,Zhonghong Li
A multi-channel colorimetric device was developed for the low-cost and simultaneous determination of three important parameters in wine safety and quality— total iron (Fe), methanol (MeOH), and total phenols. The detection was performed by assembling light-dependent resistors and light-emitting diodes in a 3D printed chamber, which measured colorimetric signals horizontally transmitting through the microwells of an 8-well strip. This device demonstrated linear relationships (R 2 greater than 0.99) for all analytes with detection limits of 0.04 mg/L, 2.26 mg/L, and 3.40 mg/L for Fe, MeOH, and total phenols, respectively. Wine sample measurements showed that the multi-channel device was as accurate as the professional spectrophotometer and could simultaneously provide the three target concentrations to facilitate the analysis. With the merits of low fabrication cost and ease of use, this device could be used as a general platform for multiple-target detection, demonstrating great potential for application in food analysis.
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