SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Zhengqing Cai,Yougui Song,Xibiao Jin,Chong-Chen Wang,Haodong Ji,Wen Liu,Xianbo Sun
A highly solar active AgBr/h-MoO 3 composite was constructed by a facile precipitation method, and the charge separation tuning was achieved by photoreduction of AgBr. The photoreduced Ag 0 on AgBr/h-MoO 3 acted as charge transfer bridge to form Z-scheme heterostructure, while the high degree of Ag reduction converted the material into type-II heterostructure. The synthesized optimal material promoted charge separation and visible light activity due to the incorporation of highly solar active AgBr, which showed ca. 2 times activity on trimethoprim (TMP) degradation than h-MoO 3 . The contribution of reactive species on TMP degradation followed the order of O 2 − > 1 O 2 > h + , which agree well with the proposed charge separation mechanism. The photocatalytic degradation mechanism of TMP was proposed based on the radical quenching, intermediate analysis and DFT calculation. The toxicity analysis based on QSAR calculation showed that part of the degradation intermediates are more toxic than TMP, thus sufficient mineralization are required to eliminate the potential risks of treated water. Moreover, the material showed high stability and activity after four reusing cycles, and it is applicable to treat contaminants in various water matrix. This work is expected to provide new insight into the charge separation tuning mechanism for the AgX based heterojunction , and rational design of highly efficient photocatalysts for organic contaminants degradation by solar irradiation.
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Journal of Central South University
·
2020
·Vol. 26
·期 11
·2974-2986
·
IF 1.249
Xu Si-quan,Pan Dong-hui,Xiao Guo-min
With the aim of achieving a high 5-hydroxymethylfurfural (HMF) yield from glucose with H-ZSM-5 catalyst at low cost, three inexpensive biphasic reaction systems, H 2 O—tetrahydrofuran (THF), H 2 O—2-methyltetrahydrofuran (MeTHF) and H 2 O’2-butanol, were discovered and proved to be particularly effective in promoting the formation of HMF from glucose over H-ZSM-5 zeolite. In order to determine the optimal process conditions, the effects of various experimental variables, such as reaction temperature, reaction time, catalyst dosage, volume of organic solvent, as well as inorganic salt type on glucose conversion to HMF in three systems were investigated in detail. It was found that under optimal reaction conditions, H 2 O—THF, H 2 O—2-butanol and H 2 O—MeTHF allowed the glucose dehydration process to achieve HMF yields of up to 61%, 59%, and 50%, respectively. Moreover, in the three biphasic systems, the H-ZSM-5 catalyst was also demonstrated to maintain excellent stability. Thus, the catalytic approach proposed in this paper can be believed to have potential prospects for industrially efficient and low-cost production of HMF.
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Biosensors-Basel
·
2023
·Vol. 13
·期 10
·932
·
IF 5.4
Gang Peng,Mengxue Guo,Yuting Liu,Han Yang,Zuorui Wen,Xiaojun Chen
Hg2+, a highly toxic heavy metal, poses significant environmental and health risks, necessitating rapid detection methods. In this study, we employed an electrochemical aptasensor for rapid and sensitive detection of Hg2+based on DNA strands (H2 and H3) immobilized graphene aerogels-Au nanoparticles (GAs-AuNPs) hybrid recognition interface and exonuclease III (Exo III)-mediated cyclic amplification. Firstly, Gas-AuNPs were modified on the surface of the ITO electrode to form a sensing interface to increase DNA loading and accelerate electron transfer. Then, DNA helper was generated with the addition of Hg2+via Exo III-mediated cycling. Finally, the hairpin structures of H2 and H3 were opened with the DNA helper, and then the methylene blue (MB) functionalized DNA (A1 and A2) combined with the H2 and H3 to form an H-shaped structure. The current response of MB as an electrochemical probe was proportional to the concentration of Hg2+. Under optimal conditions, the aptasensor showed excellent performance for Hg2+, achieving a linear range from 1 fM to 10 nM and a detection limit of 0.16 fM. Furthermore, the aptasensor was used to detect Hg2+in spiked milk samples, achieving a high recovery rate and demonstrating promising application prospects.Keywords:graphene aerogels–Au nanoparticles;Hg2+;H-shaped;aptasensor;milk sample
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Shiyue Hu,Junhong Liu,Xuanlan Luo,Qiqi Shen,Yu Qin,Haikun Hu,Jinhai Yuan,Shuangkou Chen,Di Xu
Currently, photocatalytic degradation is a fascinating technology due to its capability to treat escalating environmental problems by degrading chemicals like dyes and pharmaceuticals from wastewater. Herein, the hexagonal prism GQDs/h-MoO 3 composite photocatalyst was fabricated through a facile hydrothermal approach. The synthesized samples were identified by XRD , SEM, FT-IR, XPS , UV-Vis DRS , and PL technologies to study the crystal structure, morphology, surface chemical composition , and optical properties . The preparation circumstances of binary compounds, such as different GQDs (Graphene quantum dots) loading amounts, precursor solution pH, hydrothermal temperature, and hydrothermal time were optimized, also, and the photocatalytic activity of materials is determined by photodegradation of Methylene Blue in this approach, which systematically investigated the impact of operational conditions on the efficiency of the photocatalytic reaction. The results revealed that 10GQDs/h-MoO 3 has the best photocatalytic performance among competitors, which exhibited a high photodegradation efficiency (85.58%) of MB, and the rate was approximately 2.13 times greater than pristine h-MoO 3 . Moreover, the PL and EIS measurements proved the outstanding separation and migration ability of the photo-excited carriers of composite, which was attributable to the fact that GQDs can serve as electron transporters and acceptors to induce electron-hole separation efficiently. Finally, the free radical scavenging experiments confirmed that the primary active species was h + in the photocatalytic process, as well as a potential explanation for the improved photocatalytic activity of GQDs/h-MoO 3 photocatalysts was proposed.
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Materials
·
2023
·Vol. 16
·期 14
·4979
·
IF 3.4
Wen Zhong,Jiazhi Dong,Siqiang Chen,Zhe Tong
The synergistic effect of different types of solid particles in liquid lubricants is of great interest. In this work, g-C3N4nanosheets were initially prepared using a calcination method and then as-prepared, and h-BN were used as lubricating additives to the white oil. A comparison between the mixed additives and the single g-C3N4or h-BN additives revealed that the base oil with the addition of g-C3N4and h-BN showed the best lubricating properties. The results show a 12.3% reduction in friction coefficient, resulting in a 68.6% reduction in wear rate compared to the white oil when filled with 0.5 wt% g-C3N4and h-BN (1:1 by weight). Moreover, the addition of g-C3N4and h-BN improves the high-temperature lubrication properties of the white oil. However, the friction coefficient and wear rate increase with increasing oil temperature. The large contact area between g-C3N4and its sliding counterpart and the strong adhesive force between h-BN and its sliding counterpart improve the film formation efficiency, leading to enhanced tribological properties under oil lubrication conditions.
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ACTA MATERIALIA
·
2023
·
IF 9.4
Ruineng Ruan,Haibo Xiao,Wenjing Dong,Zhanghong Yu,Xunying Wang,Baoyuan Wang,Chen Xia,Hao Wang
Fast ionic transportation is in high demand for developing low-temperature solid oxide fuel cells (LT-SOFCs). Facing this challenge, a new H + /O 2− /Li + triple conductor is designed in this study from a lithium-metal oxide, spinel Li 4 Ti 5 O 12 (LTO). First-principle calculation based on density functional theory (DFT) reveals the proton transport barrier in LTO can be as low as 0.37 eV while the barrier for oxygen ion transportation is 0.94 eV. Using the designed LTO as the electrolyte and a typical cathode of lithium-ion battery, LiNi 0.8 Co 0.15 Al 0.05 O 2-δ , as the symmetrical electrodes, an all-lithium-metal-oxides-based LT-SOFC is constructed. High performance is achieved by the SOFC at 550–425 °C, i.e. 625 mW cm −2 at 550 °C, and a low activation energy of 0.60 eV is found with respect to the ionic conductivity of LTO at 550–475 °C. Further study confirms the dual O 2− /H + conduction of LTO via the application of proton and oxygen ion filters as well as the transference number test. Additionally, particular attentions are paid to the transport behavior of Li + in the cell via a charging process study and from XRD results. The possible contribution of triple conduction on fuel cell performance is discussed. This work demonstrates the great promise of triple H + /O 2− /Li + conducting lithium-metal oxides for LT-SOFC electrolyte development.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Zihao Cui,Qianqian Zhang,Hui Fu,Qihao Liu,Xiaolei Liu,Yaqiang Wu,Peng Gao,Zeyan Wang,Zhaoke Zheng,Hefeng Cheng,Yuanyuan Liu,Ying Dai,Baibiao Huang,Peng Wang
Herein, a facile anti-solvent preparation strategy is proposed to fabricate lead-free halide perovskite Cs 3 Bi 2 Br 9 with TiO 2 , which boosts photocatalytic activation of C(sp 3 )−H bonds in toluene oxidation . TiO 2 not only works as nucleation center to reduce the particle size of perovskite, but could form type II heterojunction with Cs 3 Bi 2 Br 9 , thus improving the photocatalytic performance of the TiO 2 /Cs 3 Bi 2 Br 9 composite. Under AM 1.5 G simulated sunlight irradiation, the optimal TiO 2 /Cs 3 Bi 2 Br 9 composite exhibits both high production rate (9692.5 μmol g −1 h −1 ) and selectivity (91 %) of benzaldehyde product. As verified by in-situ ESR, in-situ FT-IR and DFT calculations, •O 2 − and h + are demonstrated to be the main active species in this process. This work provides a new insight into the design of high-performance lead-free perovskite photocatalysts for organic synthesis.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ziwei Qin,Yi Yang,Qingli Tian,Hao-Yang Mi,Heng Li,Runhao Guo,Ying Wang,Chuntai Liu,Changyu Shen
Developing protective materials with intelligent and stimuli-responsive properties is indispensable for safety protection. However, combining contradictory characteristics into a single polymer is challenging, such as high mechanical strength, impact protection, and self-healing properties. Herein, a strain-hardening supramolecular polyurethane nanocomposite (SPN) with high mechanical strength and unique impact protection characteristics is synthesized by incorporating quadruple hydrogen bonds (H-bonds), disulfide bonds, and modified silica nanoparticles into polyurethane elastomer. Benefiting from the dynamic break and re-form characteristic of quadruple H-bonds and the stress dissipation behavior of nanoparticles, SPN exhibits high energy absorption efficiency and impact protection properties. During the drop ball striking test, the impact energy absorption efficiencies reached 90%, and the buffer time of impact was significantly longer than common buffering materials. The SPN exhibited excellent stretchability and self-healing ability, ascribing to disulfide metathesis and H-bonds association. Moreover, the prepared SPN could be easily processed through a hot press and showed negligible creeping. The developed SPN could serve as a novel self-standing impact protective material that offers promising prospects in sports, transportation, and aerospace fields.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Qiuxia Zou,Hongshen He,Jie Xie,Shibo Han,Weijie Lin,Ajoy Kanti Mondal,Fang Huang
In this study, Sn modified molecular sieves with Lewis (L) acid center and Al modified molecular sieves with Brönsted (B) acid center were prepared by post-synthesis method. They were applied to the catalytic pyrolysis of Kraft lignin for the preparation of bio-oil. The acid properties of acid modified zeolites were systematically investigated by XRD, SEM, EDS and Py-FT-IR, and the bio-oil is analyzed by heteronuclear single quantum coherent nuclear magnetic resonance (HSQC-NMR). By separating L acid and B acid from zeolite molecular sieves, the conformational relationships between these two acids on the oxygen-containing functional groups in Kraft lignin bio-oil are investigated separately. The results show that acid modified molecular sieves’ L acid and B acid can effectively improve the cleavage of aromatic C-O bonds including methoxy and ether bonds. The L acid of Sn modified molecular sieve tends to break the O-C 4 bond and the natural methoxy bond, while the B acid of Al modified molecular sieve generates aliphatic hydrocarbon intermediates and phenolic compounds by breaking the C β -O bond and rearranging the methoxy bond. By chemical characterization of the acid modified molecular sieves and the bio-oil, the conformational relationship between the L acid and B acid of zeolite molecular sieves on the deoxygenation efficiency of Kraft lignin pyrolysis bio-oil is established.
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ChemSusChem
·
2019
·Vol. 12
·期 16
·3871-3877
·
IF 7.804
Dan Wu,Xing Yu,Xinqing Chen,Gan Yu,Kun Zhang,Minghuang Qiu,Wenjie Xue,Chengguang Yang,Ziyu Liu,Yuhan Sun
Graphical Stacks on ! H-type MFI zeolite catalysts with a unique stacked structure are synthesized in a one-pot procedure in the presence of NH 4 F with the help of zeolite confinement through a solvent-free route without further ion-exchange procedures. The catalysts display excellent catalytic performance in methanol-to-gasoline reactions. H-type aluminosilicate zeolites are extensively used as solid-acid catalysts and support materials in industrial catalysis. However, the conventional synthesis methods involving hydrothermal syntheses and ion-exchange processes suffer from severe water pollution and toxic gas emissions. Herein, H-type MFI zeolite catalysts with a unique stacked structure were directly synthesized in the presence of NH 4 F and with the help of zeolite confinement through a solvent-free route without further ion-exchange procedures. A range of ex situ and in situ characterization procedures were used to provide evidence of the simultaneous use of pre-made ZSM-5 and NH 4 F as a confined Al source and mineralizer, respectively. The confined zeolite framework of ZSM-5 prevented the formation of AlF x species between NH 4 F and Al atoms, ensuring that the prepared samples had desirable acidic properties. Moreover, the resulting morphology could be controlled by using different silica substrates. The obtained H-type MFI zeolites showed excellent catalytic performance in methanol-to-gasoline reactions owing to their unique structure and directly exposed acidic sites. The developed one-pot strategy provides an alternative method for the facile synthesis of H-type zeolites with defined morphology.
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EUROPEAN POLYMER JOURNAL
·
2025
·
IF 6.3
Zhen Huang,Shimin Geng,Yizhen Chen,Ying Li,Mingen Fei,Renhui Qiu,Tingting Chen,Wendi Liu
Traditional polyurethane hot-melt adhesives often fall short in achieving high bonding strength and recyclability, and their dependence on non-renewable resources poses a significant hurdle for sustainable development. In this study, a palm oil-based diethanolamide (POEA) containing a long aliphatic chain was synthesized to develop comb thermoplastic polyurethane hot-melt adhesives (POPUs) with high biobased content, superior adhesion strength, and reusability. The microphase separation structure of POPUs was manipulated through the incorporation of dangling fatty acid chains and hydrogen bonds, resulting in the adhesives with excellent mechanical properties, with an optimum tensile strength of 5.37 MPa and an elongation at break of 282 %. As a hot-melt adhesive, it achieved a maximum lap-shear strength of 7.34 MPa on steel and maintained an average strength of 95 % of its initial value across multiple bonding cycles. Moreover, its lap-shear strengths with wood and glass remained at 6.57 MPa and 3.57 MPa respectively, fully meeting the requirements for interior decoration. Additionally, it was unexpectedly discovered that the adhesives possessed fluorescence characteristics, which can be applied in fields such as cultural relic restoration and anti-counterfeiting.
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JOURNAL OF MATERIALS SCIENCE
·
2014
·Vol. 49
·期 22
·7730-7741
·
IF 2.305
Luo Yan-Ling,Huang Rui-Juan,Xu Feng,Chen Ya-Shao
pH-Sensitive biodegradable polymethacrylic acid- block -polylactic acid- block -polymethacrylic acid (PMAA 2 - b -PLA- b -PMAA 2 ) H-type multiblock copolymers were synthesized by atom transfer radical polymerization. The copolymer structure and molecular weight were characterized by FT-IR, 1 H NMR, and gel permeation chromatography. The physicochemical characterization revealed that the copolymers could spontaneously form spherical core–shell micelles in aqueous solution, with critical aggregation concentration of about 19.7–32.5 mg L −1 and the hydrodynamic diameters below 200 nm. Z eta potentials measurements disclosed that the copolymer micelles were negatively charged due to ionized carboxyl groups in various PBS solutions. The H-type block copolymer micelles exhibited pH- sensitivity, as expected; and the hydrophobic anticancer drugs, 10-hydroxycamptothecin, and paclitaxel, had faster release rate in PBS solution of pH 5.6–7.4 than in PBS of pH 1.4, which was important for applications in the therapy of small intestine cancers. The copolymer micelle aggregates were proved to be biodegradable, and the degradation rates changed with copolymer compositions and environmental media. The micelle drug formulation indicated pH-dependent cytotoxicity and was thus capable of effectively killing the intestinal cells while avoiding doing harm to stomach. The biodegradable pH-sensitive PMAA 2 - b -PLA- b -PMAA 2 H-type copolymer micelles can be used as water-insoluble drug targeting release carriers for targeted treatment of intestine cancers.
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