Fundamental Research
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2023
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IF 6.2
Qian Hu,Taoyu Yang,Shanli Wang,Licong Xu,Minghua Wu,Deyou Yu,Kaixing Fu,Jinming Luo
Peracetic acid (PAA) has recently been considered a promising oxidant candidate for heterogeneous Fenton-like reactions; however, the main generation and contribution of organic radicals (R-O•) with unsatisfactory oxidation potential compromises wastewater decontamination efficiency. In this study, we demonstrate the rational design and synthesis of ultrafine FeO x nanocluster-anchored carbonaceous nanosheets (UFe-CN) for altering the PAA activation pathway from R-O• to •OH dominant process via in situ framework collapse carbonization of MIL-53(Fe). The constructed UFe-CN/PAA system effectively accelerated refractory micropollutant ( e.g. , p-nitrophenol (4-NP)) decomposition by the enhanced •OH formation (up to 65.24 μmol L − 1 ) under a wide pH range (3.0–9.0), outperforming the benchmark iron-based catalyst counterparts by 4.2–10.8 times. This outstanding Fenton-like catalytic activity of UFe-CN is primarily attributed to the significant improvement in electron mitigation, ca. 49 times higher than that of its MIL-53(Fe) counterpart, for interface catalysis reactions triggered by iron species cycling. Furthermore, to facilitate adaptive engineering, the organic pollutant removal efficiency could be easily tuned by varying several key treatment factors, including the initial pH, PAA concentration, and UFe-CN dosage. More importantly, the excellent practicality of UFe-CN/PAA was demonstrated by systematically evaluating the impact of the water matrix, catalyst regeneration capability, and wastewater treatment efficiency. Overall, this study provides a significant understanding of •OH-dominated PAA activation and an effective catalyst development paradigm to facilitate the practical application of PAA-based Fenton-like oxidation.
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NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 11
·5546-5554
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IF 3.3
Wenwen Yang,Shan-Shan Xu,Yawen Niu,Yanhui Zhang,Jian-Feng Li,Juan Xu
As a member of the ternary sulfides, CdIn2S4 is a visible light responded catalyst with a band gap of 2.2–2.6 eV, which is suitable for solar spectrum. In this study, a simple two-step solvothermal method was used to construct Ni12P5/In(OH)3/CdIn2S4 composite catalysts with type-II and Z-scheme heterojunctions, and there was a synergy between the two heterojunctions. The Ni12P5/In(OH)3/CdIn2S4 composite catalyst formed a donor-mediator-acceptor system for photogenerated electrons, which greatly improved the separation efficiency of the photogenerated carriers. Moreover, the highest hydrogen production activity achieved by the Ni12P5/In(OH)3/CdIn2S4 composites was 5.75 mmol g−1 h−1, which was 21 times the original CdIn2S4.
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Polymers
·
2023
·Vol. 15
·期 1
·248
·
IF 5
Yao Lu,Xuna Jin,Xiang Li,Minpeng Liu,Baolei Liu,Xiaodan Zeng,Jie Chen,Zhigang Liu,Shihua Yu,Yucheng Xu
Superparamagnetic Fe3O4particles have been synthesized by solvothermal method, and a layer of dense silica sol polymer is coated on the surface prepared by sol-gel technique; then La(OH)3covered the surface of silica sol polymer in an irregular shape by controlled in situ growth technology. These magnetic materials are characterized by TEM, FT-IR, XRD, SEM, EDS and VSM; the results show that La(OH)3nanoparticles have successfully modified on Fe3O4surface. The prepared Fe3O4@La(OH)3inorganic polymer has been used as adsorbent to remove phosphate efficiently. The effects of solution pH, adsorbent dosage and co-existing ions on phosphate removal are investigated. Moreover, the adsorption kinetic equation and isothermal model are used to describe the adsorption performance of Fe3O4@La(OH)3. It was observed that Fe3O4@La(OH)3exhibits a fast equilibrium time of 20 min, high phosphate removal rate (>95.7%), high sorption capacity of 63.72 mgP/g, excellent selectivity for phosphate in the presence of competing ions, under the conditions of phosphate concentration 30 mgP/L, pH = 7, adsorbent dose 0.6 g/L and room temperature. The phosphate adsorption process by Fe3O4@La(OH)3is best described by the pseudo-second-order equation and Langmuir isotherm model. Furthermore, the real samples and reusability experiment indicate that Fe3O4@La(OH)3could be regenerated after desorption, and 92.78% phosphate removing remained after five cycles. Therefore, La(OH)3nanoparticles deposited on the surface of monodisperse Fe3O4microspheres have been synthesized for the first time by a controlled in-situ growth method. Experiments have proved that Fe3O4@La(OH)3particles with fast separability, large adsorption capacity and easy reusability can be used as a promising material in the treatment of phosphate wastewater or organic pollutants containing phosphoric acid functional group.Keywords:superparamagnetic;Fe3O4@La(OH)3inorganic polymer;phosphate adsorption
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Jiajia Wang,Lizhi Wang,Du Zhang,You Wang,Jiawei Li,Fa Zhou,Jianhan Huang,You-Nian Liu
Herein, the covalently connected core–shell metal–organic frameworks (MOFs)@covalent-organic frameworks (COFs) hybrid materials were successfully constructed by coating the stable COF-OH shell on the NH 2 -MIL-125 core. The introduction of the NH 2 -MIL-125 core endowed the hybrid materials with high Brunauer–Emmett–Teller (BET) surface area ( S BET ) and abundant unsaturated metal sites. And the coating of COF-OH shell endowed the hybrid materials outstanding physicochemical stability and visible-light response, and suitable band gaps. Moreover, the thickness of the COF-OH shell was carefully adjusted according to the feeding amount of NH 2 -MIL-125. Impressively, the electron transfer pathway in the formed heterostructure was clarified and it was proven that a type-II heterojunction was generated between the MOFs and the COFs. The formed stable C N covalent bonds in the interfacial layer was beneficial to the photogenerated electron transfer and the electron-hole pairs separation, which greatly enhanced the CO 2 photocatalytic reduction. The product NH 2 -MIL-125@COF-3 exhibited the highest CO yield of 22.93 μmol·g −1 ·h −1 , about 2 times higher than NH 2 -MIL-125 (11.82 μmol·g −1 ·h −1 ) and 3 times greater than COF-OH (7.26 μmol·g −1 ·h −1 ). This work can provide helpful ideas for the careful design of the novel MOFs@COFs hybrid materials as well as useful exploration for the CO 2 photocatalytic reduction.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Tao Luo,Yanan Yuan,Danna Zhou,Liting Luo,Jinjun Li,Feng Wu
In the recent years, sulfite-induced oxidation of various contaminants using oxysulfur radicals (SO 4 − , SO 5 − and SO 3 − ) has been explored to establish novel advanced oxidation processes (AOPs). Although transition metals, such as cupric ions (Cu(II)), have been demonstrated to be capable of activating sulfite (S(IV)), the catalytic mechanism of the specific Cu(II) species is still not very clear. In this work, N-acetyl- para -aminophenol (APAP) was used as a basic substrate to investigate the process, mechanism and stability of the Cu(II)-S(IV) system with low dosages of Cu(II) (0.010 mmol L −1 ) in an alkaline solution (pH 10). The results show that 0.010 mmol L −1 Cu(II) can efficiently activate S(IV) for the oxidation of APAP and other contaminants (e.g., metoprolol, sulfanilamide, aniline, 4-chloroaniline, N,N-dimethylaniline, p -nitrophenol and 3-nitrophenol). Simulation calculations for the distribution of the Cu(II) species and pH-dependence of APAP oxidation in the Cu(II)-S(IV) system showed that Cu(OH) 2 particles are the major active species in the catalysis of S(IV). The surface complexation of S(IV) with the Cu(OH) 2 particles prior to the production of oxysulfur radicals is the basic mechanism of the alkaline Cu(II)-S(IV) system. Radical inhibition with scavengers (ethanol, tert-butyl alcohol or aniline) demonstrates that SO 5 − , SO 4 − and hydroxyl radicals (HO ) are responsible for the contaminant oxidation. Moreover, SO 5 − is believed to be the main active species in the Cu(II)-S(IV) system, which has a second-order rate constant of 2.98 × 10 8 M −1 s −1 with APAP. This work renews our recognition of the Cu(II)-S(IV) system applications and further understanding of the catalytic role of the nascent Cu(OH) 2 particles in the activation of S(IV).
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Green Energy & Environment
·
2019
·
IF 0
Xiaolan Deng,Yuqi Jiang,Zengxi Wei,Minglei Mao,Ramyakrishna Pothu,Hongxia Wang,Caiyun Wang,Jinping Liu,Jianmin Ma
Increasing the energy density, power density as well as widening the operation voltage are essential to electrochemical capacitors to meet the practical energy demands. Herein, a novel flexible quasi-solid-state dual-ion asymmetric supercapacitor (ASC) with Ni(OH) 2 and Nb 2 O 5 nanosheets directly grown on stainless steel mesh is developed. In the dual-ion ASC, Nb 2 O 5 negative and Ni(OH) 2 positive electrodes react with Li + and OH − respectively in alkaline gel electrolyte to store energy, which is quite different from conventional alkali metal ion SCs and alkaline SCs. The as-assembled flexible device has an extended working voltage of 1.7 V and delivers a capacity of 5.37 mAh cm −2 , a maximum energy density and power density of 0.52 mWh cm −3 and 170 mW cm −3 , respectively. The device maintains around 60% capacity retention after long cycling up to 1000 cycles. Moreover, our device can light up a LED light efficiently upon fast charging. The proposed quasi-solid-state dual-ion ASC has potential applications in future portable electronics and flexible energy storage devices.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2018
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IF 2.829
Jinqiong Xu,Tingting Chen,Xiujuan Qiao,Qinglin Sheng,Tianli Yue,Jianbin Zheng
A novel non-enzymatic electrochemical sensor based on gold nanoparticles/nicke hydroxide nanosheet (AuNPs/Ni(OH) 2 NS) nanocomposite was successfully fabricated and further used for glucose sensing. The morphology and composition of AuNPs/Ni(OH) 2 NS were characterized by scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and X-ray diffraction. The electrochemical properties were evaluated through cyclic voltammetry and amperometric methods. The AuNPs/Ni(OH) 2 NS/GCE exhibited wide linear range (0.002–6.0 mM), a low detection limit (0.66 μM) and good reproducibility and stability. The sensor was successfully employed for glucose detection in food samples for which the sensor displayed high performance with excellent reproducibility and recovery in complex food materials.
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CHEMOSPHERE
·
2019
·
IF 5.108
Jian Lu,Qi Sun,Jun Wu,Guangcan Zhu
Techniques for reutilization of the discarded bischofite are limited while efficient recovery of the Mg(OH) 2 nanoparticles from water during the synthesis and reuse processes is a challenge. In this study, the Fe 3 O 4 @Mg(OH) 2 core-shell magnetic nanoparticles were firstly prepared from discarded bischofite and used as catalyst for improving the ozonation of metronidazole (MNZ). The removal rate constant of MNZ increased by 694.7% using Fe 3 O 4 @Mg(OH) 2 . Compared with the Mg(OH) 2 control, the MNZ removal rate constant of Fe 3 O 4 @Mg(OH) 2 treatment was almost tripled. The persistent high catalytic activity of the Fe 3 O 4 @Mg(OH) 2 catalyst was observed since the MNZ removal rate constant decreased by just 13.2% in the third reuse run. The Fe 3 O 4 @Mg(OH) 2 primarily enhanced ozone decomposition through producing hydroxyl radicals . The MNZ removal rate constant increased from 0.075 min −1 to 0.643 min −1 as catalyst dose increased from 0 to 0.6 g L −1 while it decreased by 96.0% when its initial concentration increased from 10 to 200 mg L −1 . The maximum removal rate constant was observed at 25 °C when temperature increased from 15 °C to 35 °C. The Cl − , HCO 3 − , SO 4 2− , Ca 2+ , Mg 2+ ions could jeopardize MNZ degradation. The antibacterial activity of MNZ was eliminated after catalytic ozonation while the mineralization efficiency was almost doubled. The nitro group reduction and the cleavage of hydroxyethyl bond were two main transformation pathways of MNZ. These findings suggest that Fe 3 O 4 @Mg(OH) 2 nanoparticle made from discarded bischofite is the promising catalyst for the ozonation of antibiotics in the terms of water purification practice and reutilization of the bischofite.
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JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 21
·15118-15129
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IF 2.993
Liu Hao,Xu Jü,Liu Guanxi,Wang Meiri,Li Jing,Liu Yuanyuan,Cui Hongtao
Herein, a facile sol–gel strategy for building the ordered interpenetrating network of Ni(OH) 2 and reduced graphene oxide (rGO) was proposed. In this strategy, rGO nanosheets were homogeneously fixed inside composite utilizing the pores of Ni(OH) 2 gel as template, forming rGO-interpenetrated gel network. It was found that the rGO nanosheets could effectively reduce the internal resistant of composites and provide mechanical support for the gel network of Ni(OH) 2 . Therefore, the composite presented high electrochemical performance, especially high-rate performance, due to the interpenetrating of rGO nanosheets plus the supplementary role of acetylene black. It had high specific capacitance of 2163 F g −1 at low current density of 2.9 A g −1 and 733 F g −1 at high current density of 86.8 A g −1 .
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JOURNAL OF NANOPARTICLE RESEARCH
·
2018
·Vol. 20
·期 6
·1-9
·
IF 2.127
Wu Xiang-Feng,Li Hui,Su Jun-Zhang,Zhang Jia-Rui,Feng Yan-Mei,Pan Jun-Cheng,Zhang Ying,Sun Li-Song,Zhang Wei-Guang,Sun Guo-Wen
The In 2.77 S 4 microspheres had been firstly fabricated by using polyethylene glycol (PEG) as the morphological modifier and then used to hybridize with In(OH) 3 nanocubes by a simply depositional method. The structure, optical properties, morphology, chemical compositions, and charge carrier behaviors of the as-prepared In 2.77 S 4 /In(OH) 3 composites were characterized, respectively. The methyl orange, tetracycline, rhodamine B, and Cr(VI) dilute solution were selected to evaluate their photocatalytic activities. Experimental results showed that In(OH) 3 nanocubes could improve the photocatalytic activity and recyclability of the In 2.77 S 4 microspheres under the visible light irradiation. With the usage of In(OH) 3 increased, the photocatalytic efficiency of the hybrids was firstly increased and then decreased. When the mass ratios of In 2.77 S 4 to In(OH) 3 were 6:2, it reached the maximum of 100% in 15 min for methyl orange, obviously higher than 67.4% of In 2.77 S 4 and 1.1% of In(OH) 3 . Meanwhile, it could also oxidize 85.6% of tetracycline in 20 min, 97.8% of rhodamine B in 7.5 min, and reduce 92.9% of Cr(VI) in 30 min under the visible light irradiation. Moreover, it could still degrade 91.7% of methyl orange solution after 3 cycles, which was much higher than 40.7% of In 2.77 S 4 microspheres. In addition, the possible mechanism of enhancing photocatalytic properties was proposed.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2018
·
IF 3.909
Haifeng Hu,Liu Yang,Zhen Lin,Xiaotong Xiang,Xiancai Jiang,Linxi Hou
A novel magnetic bioadsorbent beads composed of Fe 3 O 4 , chitosan, and Al(OH) 3 (Fe 3 O 4 /CS/Al(OH) 3 ) was synthesized by a modified solvothermal and in-situ reaction. The composite adsorbent was characterized by Fourier-transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, energy dispersive X-ray spectroscopy, and vibrating sample magnetometer, respectively. Adsorption toward F − onto Fe 3 O 4 /CS/Al(OH) 3 was investigated as a function of Fe 3 O 4 concentration, initial solution pH, adsorbent dosage, initial fluorion concentration, co-existing ions in water and initial temperature. The addition of Fe 3 O 4 could enhance the adsorption properties of CS/Al(OH) 3 . The saturated adsorption capacity of magnetic Fe 3 O 4 /CS/Al(OH) 3 calculated from the Langmuir isotherm model was 76.63 mg/g at 298 K. The adsorption isotherm of F − followed Langmuir isotherm model and the adsorption kinetics fitted better to the pseudo-second order kinetic model. The influence of temperature confirmed that the adsorption was spontaneous and endothermic. The magnetic Fe 3 O 4 /CS/Al(OH) 3 beads could be easily separated from water under a low magnetic field.
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Chemistry Central Journal
·
2017
·Vol. 11
·期 1
·1-8
·
IF 2.442
Xie Yulu,Li Xican,Xu Jieying,Jiang Qian,Xie Hong,He Jianfeng,Chen Dongfeng
Background
Suoyang originates from a psammophyte named Cynomorium songaricum Rupr and has been known as a phenolic-antioxidant-enriched traditional Chinese herbal medicine. The present study attempted to investigate the protective effect of phenolic antioxidants in Suoyang towards •OH-mediated MSCs and then further discusses the chemical mechanisms.Methods The lyophilized aqueous extract of Suoyang (LAS) was prepared and characterized using HPLC. Then, two phenolic antioxidant references, epicatechin and luteolin-7-O-β-D-glucoside, along with LAS, were investigated for their effects on the viability of •OH-treated MSCs using the 3-(4, 5-dimethylthiazol-2-yl)-2,5-diphenyl (MTT) assay. The comparison and mechanistic chemistry of epicatechin and luteolin-7-O-β-D-glucoside were further explored using various antioxidant assays, including PTIO•-scavenging, FRAP (ferric ion reducing antioxidant power), ABTS+•-scavenging, and DPPH•-scavenging. Their Fe2+-binding capacities were also compared using ultraviolet (UV) spectra.Results The HPLC analysis indicated that there are 8 phenolic antioxidants in LAS, including epicatechin, luteolin-7-O-β-D-glucoside, gallic acid, protocatechuic acid, catechin, isoquercitrin, phlorizin, and naringenin. The MTT assay revealed that epicatechin could more effectively increase the survival of •OH-treated MSCs than luteolin-7-O-β-D-glucoside. Similarly, epicatechin exhibited higher antioxidant abilities than luteolin-7-O-β-D-glucoside in the DPPH•-scavenging, ABTS+•-scavenging, FRAP, and PTIO•-scavenging assays. In the Fe2+-binding assay, luteolin-7-O-β-D-glucoside gave a stronger UV peak at 600 nm, with ε = 2.62 × 106 M−1 cm−1, while epicatechin produced two peaks at 450 nm (ε = 8.47 × 105 M−1 cm−1) and 750 nm (ε = 9.68 × 105 M−1 cm−1).Conclusion As two reference antioxidants in Suoyang, epicatechin and luteolin-7-O-β-D-glucoside can enhance the viability of •OH-damaged MSCs. Such a beneficial effect may be from their antioxidant effects, including direct-antioxidant and indirect-antioxidant (i.e., Fe2+-binding) processes. In the direct-antioxidant process, proton (H+), one electron (e), or even hydrogen-atom (•H) transfer may occur to fulfill radical-scavenging (especially •OH-scavenging); in this aspect, epicatechin is superior to luteolin-7-O-β-D-glucoside due to the presence of more phenolic –OHs. The additional –OHs can also be responsible for the better cytoprotective effect. In terms of indirect-antioxidant potential, however, epicatechin is inferior to luteolin-7-O-β-D-glucoside due to the absence of a hydroxyl-keto moiety. These findings will provide new information about medicinal psammophytes for MSC transplantation.
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