CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Zhuozhi Ouyang,Chen Yang,Junheng He,Qian Yao,Bijie Zhang,Hanming Wang,Yu Jiang,Jini Zhou,Yurong Deng,Yanjun Liu,Jingjing Yang,Guining Lu,Zhi Dang
Sulfamethazine (SMT), taken as model compound, have been exposed to a photocatalytic system driven by ultraviolet light (UV) irradiation with Fe(III) and three carboxylic acids (citric, tartaric and malic acid). The kinetic experiments, quenching experiments, electron paramagnetic resonance (EPR), species model theoretical calculation, density functional theory (DFT) and intermediates analyses, were conducted to analyze the formation of reactive oxygen species (ROS) and underlying mechanism of Fe(III)-carboxylate complexes on photocatalytic degradation of SMT. The results indicated the complexes easily induced the degradation under UV irradiation. Enough hydroxyl radicals ( · OH) were produced and the singlet oxygen ( 1 O 2 ) originated from the self-sensitized oxidation. An interaction among ROS, Fe(III)-carboxylate complexes and SMT was firstly proposed. The active sites and groups were characterized through Frontier electron densities (FEDs), Fourier Transform-Infrared (FTIR) and Two-dimensional correlation FTIR spectroscopy (2D-FTIR-CoS) analyses. The transformation pathway mainly included four reactions: hydroxylation, SO 2 extrusion, Smiles-type rearrangement and S-N bond cleavage. The system also had an application potential for removing SMT from practical water.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 28
·15782-15797
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IF 4.22
Jiang Danni,Zhou Yu,Wang Ping,Huang Chao,Zhu Jian,Liu Zhiming
In the MOFs-based composites, the co-catalyst nanoparticles loads tend to agglomerate. In the self-assembly process of MOFs-based composites, the use of acid modulators solved the accumulation of AgI nanoparticles cocatalyst. The active sites of carboxyl groups and mesoporous structure brought by acid modulator provide more loading sites for AgI nanoparticles. The novel AgI/D-MIL-53(Fe) showed good adsorption and photocatalytic performance in the process of removing tetracycline pollutants. Compared to the degradation efficiency of the MIL-53(Fe) with 50.8%, it of AgI/MIL-53(Fe) increased to 85.1% and which further increased to 96.2% by AgI/D-MIL-53(Fe) based on the HCl modulator. On the one hand, it is beneficial for the mesoporous D-MIL-53(Fe) modulated by HCl modulator to disperse the AgI nanoparticles co-catalyst. On the other hand, AgI nanoparticles, as a photosensitive agent, adsorb visible light to generate photogenerated electrons and holes, and electrons rapidly transferred to the heterojunction bridge Ag 0 and then captured by the holes from the D-MIL-53(Fe). The construction of AgI/D-MIL-53(Fe) Z-scheme heterojunction provided favorable conditions for the rapid separation and photogenerated electrons and holes. Finally, ·O 2 − , ·OH and h + as the main active free radicals were driving forces. This study provided more possibilities and opportunities for the construction of mesoporous MOFs-based composites.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shumin Li,Fan Wu,Rongbin Lin,Jin Wang,Chunxia Li,Zhengquan Li,Jun Jiang,Yujie Xiong
Fe-based metal-organic frameworks (MOFs) have shown promising applications in photocatalysis, yet they are incapable of photocatalytic H 2 production due to their inappropriate conduction band (CB) position and large overpotential for H 2 evolution. Herein, we present a facile strategy enabling the photocatalytic H 2 production over Fe-based MOFs through dye sensitization. A combination of characterization techniques with theoretical simulation reveals that dye sensitization can effectively inject energetic electrons into Fe-MOFs and elevate their quasi-Fermi level under light irradiation, overcoming the surface overpotential for H 2 production from water. Furthermore, deposition of Pt nanoparticles on Fe-MOFs can lower the overpotential for H 2 evolution toward further enhanced photocatalytic activity. This work provides insights into MOF band structure engineering at electronic level, and proves a concept that harnesses MOF materials for targeted photocatalytic applications they are originally not fit for.
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高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Mingqi Xu,Dingzhou Liu,Jinghua Yang,Qian Zhu,Yunliang Wang,Jingquan Sha
Study and application of MIL-100(Fe)-based two-dimensional graphene oxide (GO) nanocomposite was limited because the nucleation of the spherical structure of MIL-100(Fe) on GO along different directions hindered the formation of MOF-100(Fe). To address this issue, MIL-100(Fe)/three-dimensional graphene (3DG) nanocomposites (abbreviated as MIL-3DG-n, n = 25, 50, 75, and 100) were successfully fabricated via in situ growth of MIL-100(Fe) on 3DG matrixes in this work because the unique structure of 3DG can avoid the attachment with MIL-100(Fe) on nucleation sites along multiple directions, resulting in their ideal combination. The prepared MIL-3DG nanocomposites exhibited higher peroxidase-like catalytic activities than pure MIL-100(Fe), and MIL-3DG-75 exhibited the best peroxidase-like activities for detecting xanthine with the detection limit of 0.0014 μM in the linear range of 0–200 μM to date, to the best of our knowledge, which is attributed to the higher affinity of MIL-3DG-75 nanocomposite to peroxidase substrates o-phenylenediamine (OPD) and H2O2, confirmed by the Michaelis–Menten kinetics (Vm: 49.5 × 10–8 M s–1 for H2O2, 18 × 10–8 M s–1 for OPD, Km: 0.029 mM for H2O2, 0.011 mM for OPD). Owing to the high catalytic efficiency of the MIL-3DG-75 nanocomposite, a rapid and efficient strategy for the sensitive colorimetric detection of xanthine was established.
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高影响因子
ANALYST
·
2021
·Vol. 146
·期 20
·6187-6192
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IF 4.616
Guihua Zhang,Xinyi Zou,Hua Li,Yi He
Triacetone triperoxide (TATP) explosives, a popular choice for terrorists, have been used in many violent terrorist attacks all over the world. However, simple, rapid, and on-site detection methods of TATP are still lacking. Herein, we present a visual colorimetric method for on-site and rapid detection of TATP based on a Fe(II)-promoted thermal decomposition process of TATP. We discovered that TATP can be decomposed into H2O2 under heating conditions, and it reacts with Fe2+ to produce hydroxyl radicals (˙OH) and Fe3+via the Fenton reaction. The resulting ˙OH and Fe3+ further oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to a yellow oxidized product (oxTMB). These reaction processes remarkably promote the chemical equilibrium shift and decrease the activation energy. Using the TATP-Fe2+-TMB ternary chromogenic system, the present colorimetric assay for TATP shows a dynamic range of 0.5–30 μM with a low detection limit of 0.12 μM. Additionally, common substances (e.g., inorganic salts, small organic substances, and polymers) do not interfere with TATP detection. This assay can be used for analyzing TATP in real water and camouflage samples. Furthermore, a test-paper-based method was also successfully developed for visual, rapid and on-site detection of TATP.
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 29
·期 3
·4461-4473
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IF 4.223
Shao Jiang,Zhang Yi,Liu Zongtang,Fei Zhenghao,Sun Yufeng,Chen Ziyan,Wen Xiaoju,Shi Weizhong,Wang Dandan,Gu Chenggang
Organic palygorskite (OP)–supported Pd/Fe nanoparticles composite (OP-Pd/Fe) was prepared by stepwise reduction method. The removal capacity of 4,4′-dibrominated diphenyl ether (BDE15) by OP-Pd/Fe was compared with other various materials. For better understanding the possible mechanism, the synthesized and reacted OP-Pd/Fe materials were characterized by TEM, SEM, XRD, and XPS, respectively. The effects of major influencing parameters on the degradation of BDE15 were also studied. Benefit from the synergistic effect of the carrier and bimetallic nanoparticles, BDE15 could be completely debrominated into diphenyl ether (DE) under suitable conditions. A two-stage adsorption/debromination removal mechanism was proposed. The degradation of BDE15 with OP-Pd/Fe was mainly stepwise debromination reaction, and hydrogen transfer mode was assumed as the dominated debromination mechanism. The removal process fitted well to the pseudo first-order kinetic equation. The observed rate constants increased with increasing Pd loading and OP-Pd/Fe dosage while decreased with increasing initial BDE15 concentration, the tetrahydrofuran/water ratio, and the initial pH of the solution. The work provides a new approach for the treatment of PBDEs pollution.
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高影响因子
JACS Au
·
2021
·
IF 0
Yang Wu,Chunlei Pei,Hao Tian,Tao Liu,Xianhua Zhang,Sai Chen,Quan Xiao,Xianhui Wang,Jinlong Gong
The suppression of methane and coke formation over Ni-based catalysts for low temperature ethanol steam reforming remains challenging. This paper describes the structural evolution of Fe-modified Ni/MgAl2O4 catalysts and the influence of iron species on methane and coke suppression for low temperature ethanol steam reforming. Ni–Fe alloy catalysts are gradually oxidized by water to generate Ni-rich alloy and γ-Fe2O3 species at steam-to-carbon ratio of 4. The electron transfer from iron to nickel within Ni–Fe alloy weakens the CO adsorption and effectively alleviates the CO/CO2 methanation. The oxidation capacity of γ-Fe2O3 species promotes the transformation of ethoxy to acetate groups to avoid methane formation and the elimination of carbon deposits for anticoking. Ni10Fe10/MgAl2O4 shows a superior performance with a highest H2 yield of 4.6 mol/mol ethanol at 400 °C for 15 h. This research could potentially provide instructions for the design of Ni-based catalysts for low-temperature ethanol steam reforming.
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PubMed
RENEWABLE ENERGY
·
2021
·
IF 8.001
Hui Li,Junchi Wang,Xiaoling Ma,Yangyang Wang,Guoning Li,Min Guo,Ping Cui,Wanpeng Lu,Shoujun Zhou,Mingzhi Yu
Solid catalyst loss is inevitable by using the traditional separation methods of centrifugation or filtration. To this end, the carbonized MIL−100(Fe) is used to support ammonium sulfate ((NH 4 ) 2 SO 4 ) for synthesizing magnetic solid acid on the purpose of biodiesel production . Influence of preparation factors of loading amount, activation temperature, and activation time on catalytic activity are initially evaluated. With that, the prepared catalyst (CIS) is comprehensively investigated to obtain the optimal esterification parameters for biodiesel production . Moreover, characterizations of TG, XRD, BET, SEM, EDS, FTIR, py−FTIR, VSM, XPS, and Hammett indicator are conducted to elucidate the structure−function relationship between physicochemical property and catalytic activity . Results indicated the CIS is a superparamagnetism material with the saturated magnetism of 22 emu/g, which could be easily recovered from mixture with external magnet. Furthermore, the maximum conversion of 95.68% is obtained with mild conditions: molar ratio of methanol/oleic acid of 8:1 and catalyst amount of 8 wt% at 70 °C for 2 h. Negligible impact is detected for CIS with presence of 5 wt% water content, even with 20 wt% water content, the conversion of 85.88% is still achieved.
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高影响因子
ACS ES&T Engineering
·
2021
·
IF 0
Ying Liu,Yulin Yang,Wei Miao,Ningjie Du,Dandan Wang,Hehe Qin,Shun Mao,Kostya Ken Ostrikov
Electro-Fenton (EF) is one of the promising clean and renewable technologies for organic pollutant control. However, insufficient hydrogen peroxide (H2O2) generation and the subsequent hydroxyl radicals (•OH) conversion still prevent the wide applications of EF. Herein, we report a Ce-doped vertically aligned α-FeOOH nanoflakes anchored on a carbon felt (CF) cathode for EF operation. In this system, a high concentration H2O2 (113.6 mg/L on 4 cm2 cathode) is generated in 60 min, and being efficiently catalyzed to •OH by virtue of the active nanoedge (1.6 nm thickness) of Ce-doped α-FeOOH. The •OH production rate is calculated as high as 4.2 mM/W/cm2/min, which is ∼6.6-fold higher compared with the unmodified CF electrode. Moreover, this novel cathode achieves a complete removal (100% removal rate) of ultrahigh concentration chloramphenicol (1.1 mM, 355 mg/L) in 8 h and a high mineralization rate (94%) in 29 h in a scaled-up EF system. Density functional theory calculations (DFT) reveal that the Ce doping in α-FeOOH greatly promotes the conversion of H2O2 into •OH. This study not only offers a novel cathode structure for EF process but also opens radically new prospects for applied environmental catalysis.
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WATER RESEARCH
·
2021
·
IF 11.236
Jia Deng,Enlai Gao,Feng Wu,Zhixiong You,Xiaozhong Li,Shuxian Gao,Li-Zhi Huang
Atomic hydrogen (H•) is highly reactive for the hydrodechlorination of trichloroethylene (TCE). In this work, we found that the coprecipitation of Ni 2+ and Fe 2+ at neutral pH led to an unprecedented catalytic generation of H•. The generated H• effectively dechlorinate TCE to nontoxic ethylene and ethane, and Fe 2+ is the only electron donor. The abundant adsorbed H• produced with a Ni/Fe ratio of 0.4 enhances hydrogen evolution reaction causing a low efficiency for hydrodechlorination. In contrast, the active absorbed H• is generated in the crystal lattice of Ni-Fe hydroxides with a Ni/Fe ratio of 3.0 causing highly efficient hydrodechlorination of TCE. This work not only reveals the mechanism of catalytic hydrodechlorination by Ni-Fe hydroxides at neutral pH, but also provides a novel approach to detoxify TCE in contaminated water using facile precipitated Ni-Fe hydroxides.
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高影响因子
POLYMER INTERNATIONAL
·
2021
·Vol. 71
·期 2
·169-174
·
IF 2.99
Yinyan Chen,Yiban Wu,Yifan Zhu,Saiqi Tian
Rhodamine salicylaldehyde was synthesized, and its structure was determined using Fourier transform infrared spectroscopy, 1 H NMR analysis as well as electrospray ionization mass spectrometry. Then a fluorescent polyurethane foam was obtained via incorporation of the prepared rhodamine salicylaldehyde, and the fluorescence sensing behavior for Fe 3+ was systematically investigated. Results showed that the fluorescent polyurethane foam produced higher fluorescence in the presence of Fe 3+ in pure water, due to the coordination for Fe 3+ binding leading to ring-opened amide form. The limit of detection was calculated to be 1.64 × 10 −6 mol L –1 . This fluorescent polyurethane foam can also recognize Fe 3+ with good selectivity. © 2021 Society of Industrial Chemistry.
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高影响因子
FUEL
·
2021
·
IF 6.609
Mingquan Li,Aqsa Noreen,Yajie Fu,Cederick Cyril Amoo,Yujia Jiang,Xu Sun,Peng Lu,Ruiqin Yang,Chuang Xing,Shurong Wang
Directly synthesizing olefins from syngas using metal-zeolite composite catalysts has engrossed a lot of attention recently. Fe-based catalysts will be the most promising industrial candidates due to cost and availability constraints. In this work, we investigate the characteristics and Fischer-Tropsch activity of a novel Fe@Na-ZSM-5 composite for one-step conversion of syngas to higher olefins (C 5+ ). The in-situ crystallization mechanism induced Na in the ZSM-5 as a Fe-based promoter which realized 52.5 % selectivity for gasoline of which ∼ 70% were olefins. Additionally, the promotion by the Na ions enhanced the formation of Fe 5 C 2 phases which in turn favored C–C coupling, high gasoline and olefins selectivity. Na type zeolite (Na-Zeolite) offers a novel Na electron promoter, which participate immensely in the development of heterogenous catalyst and functional materials.
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高影响因子
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