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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高影响因子
Materials
·
2021
·Vol. 14
·期 11
·2741
·
IF 3.623
Pengcheng Lv,Ruihong Meng,Zhongyang Mao,Min Deng
In this study, the hydrated sodium aluminosilicate material was synthesized by one-step hydrothermal alkaline desilication using fly ash (FA) as raw material. The synthesized materials were characterized by XRD, XRF, FT-IR and SEM. The characterization results showed that the alkali-soluble desilication successfully had synthesized the sodium aluminosilicate crystalline (N-A-S-H) phase of sodalite-type (SOD), and the modified material had good ionic affinity and adsorption capacity. In order to figure out the suitability of SOD as an adsorbent for the removal of ammonium and phosphorus from wastewater, the effects of material dosing, contact time, ambient pH and initial solute concentration on the simultaneous removal of ammonium and phosphorus are investigated by intermittent adsorption tests. Under the optimal adsorption conditions, the removal rate of ammonium was 73.3%, the removal rate of phosphate was 85.8% and the unit adsorption capacity reached 9.15 mg/L and 2.14 mg/L, respectively. Adsorption kinetic studies showed that the adsorption of ammonium and phosphorus by SOD was consistent with a quasi-secondary kinetic model. The adsorption isotherm analysis showed that the equilibrium data were in good agreement with the Langmuir and Freundlich model. According to thermodynamic calculations, the adsorption of ammonium and phosphorus was found to be a heat-absorbing and spontaneous process. Therefore, the preparation of SOD by modified FA has good adsorption properties as adsorbent and has excellent potential for application in the removal of contaminants from wastewater.Keywords:N-A-S-H;sodalite;simultaneous removal;ammonium;phosphorus
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Materials
·
2020
·Vol. 13
·期 10
·2340
·
IF 3.057
Yongzhe Fan,Huazhen Yang,Haisheng Fan,Qi Liu,Chuang Lv,Xue Zhao,Mingxu Yang,Jianjun Wu,Xiaoming Cao
The hexagonal boron nitride (h-BN) nanosheets modified by silane coupling agent (KH560) were doped into acrylic acid coating on the surface of galvanized steel to improve its corrosion resistance. H-BN nanosheets modified by KH560 were prepared and characterised by scanning electron microscopy, transmission electron microscopy, atomic force microscopy, X-ray diffraction, and Fourier-transform infrared spectroscopy. The corrosion resistance of the acrylic acid coatings was measured by electrochemical testing. The results show that the corrosion current density of the coating with modified h-BN nanosheets was reduced from 2.2 × 10−5A/cm2to 2.3 × 10−7A/cm2compared with the acrylic acid coating. The impedance of the composite coating with modified h-BN is 4435 Ω·cm2, higher than the BNNS coating (2500 Ω·cm2) and the acrylic acid coating (1500 Ω·cm2). This is due to the physical barrier and electrical insulation properties of the hexagonal boron nitride (h-BN) nanosheets.Keywords:hot-dip galvanized steel;boron nitride nanosheet;corrosion resistance;acrylic coating
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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
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2023
·Vol. 13
·期 10
·932
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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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MACROMOLECULAR CHEMISTRY AND PHYSICS
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2023
·Vol. 224
·期 23
·2300304
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IF 2.5
Mingzhao Li,Jia Wang,Anjun Qin,Ben Zhong Tang
Hyperbranched polymers have been widely applied in various fields because of their good solubility, high reactive end groups, and low viscosity, etc. Therefore, it is of great importance to develop new strategies to build multifunctional hyperbranched polymers with novel architectures. In this work, a C(sp 3 )─H activation-based polymerization of internal alkynes and bifunctional secondary amines is successfully established, and multifunctional hyperbranched polyamines (hb-PAs) with 100% E -isomers and high molecular weights ( M w up to 76 500) are prepared in good yields (up to 82%). The hb-PAs containing tetraphenylethylene moiety show unique aggregation-enhanced emission properties and can be used for explosive detection with a low limit of detection (9.14 × 10 −8 m ). Notably, the hb-PAs display high refractive indices (up to 1.7607) that can be further modulated to 1.7825 by the coordination of its peripheral ethynyl group with metallic cobalt. Moreover, the hyperbranched structure endows the hb-PAs with much better properties than their linear counterparts, such as higher photoluminescence quantum yields and refractive indices. In addition, the hb-PAs can be modified by a C(sp 3 )─H activation reaction of internal alkynes and alcohols. This work not only prepares a series of functional nitrogen-containing hyperbranched polymers but also promotes the application of C(sp 3 )─H activation in polymer chemistry.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Junyong He,Ya Yang,Peidong Hong,Yulian Li,Chao Xie,Zijian Wu,Minqiang Li,Lingtao Kong
The use of peroxymonosulfate (PMS) activation to eliminate organic contaminants is a promising technology to purify water owing to its strong reactivity. However, because of the existed rate limiting step, the performance of PMS activation was restrained and required external energy consumption. Therefore, a new strategy was proposed to solve this problem by preparing catalysts with abundant electron-rich sites and electron traps to accelerate PMS activation. In this research, a novel MnCeO x -H catalyst with rich surface oxygen vacancies was firstly synthesized to accelerate the transfer of electrons among the catalysts, oxidant and pollutants. The contaminants were rapidly eliminated in the MnCeO x -H/PMS system, while the reaction rate constant of MnCeO x -H/PMS system was 30 times higher than that of CeO 2 /PMS system. The surface oxygen vacancies were able to adsorb and trap PMS, then the free electrons of oxygen vacancies would reduce PMS and produced HO•, 1 O 2 and SO 4 •- , while 1 O 2 played a major role. The contaminants which acted as electron-donors in this system were adsorbed at Mn, Ce sites, achieving effective conversion recycling of Ce(IV)/Ce(III), Mn(III)/Mn(II) and Mn(IV)/Mn(III). This discovery is believed to inaugurate a novel way for designing powerful electron-rich sites and electron traps to accelerate PMS activation for contaminants degradation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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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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JOURNAL OF MEMBRANE SCIENCE
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2023
·
IF 9.5
Shiwei Tian,Yaqi Zhang,Qiankun Sha,Tian Yang,Yan Huang,Xingxiang Zhang,Wei Wang,Na Han
Highly efficient treatment of oil-water emulsions in severe environments (organic solvents, strong acids) is recognized as a challenging subject. Polyphenylene sulfide (PPS) is an ideal membrane material with superior thermal stability as well as chemical resistance that is expected to settle this challenge. However, the hydrophobicity of PPS (h-PPS) membrane inherently prevents its efficient treatment of oil-in-water (O/W) emulsions. In this study, superhydrophilic modification of PPS substrates was achieved by in situ electrostatic self-assembly of hydrophilic Zr-MOFs to obtain UiO-66-NH 2 @h-PPS membranes. The introduction of UiO-66-NH 2 crystals constructed the micro/nanoscale hierarchical structure for the substrate, which transforms the PPS substrate from a hydrophobic to a superhydrophilic state (water droplets require only 0.6 s to be completely immersed in the membrane). Meanwhile, the UiO-66-NH 2 @h-PPS membranes gain under-water superhydrophobicity (the under-water oil contact angle exceeds 150° for toluene, hexane , dichloromethane , and carbon tetrachloride , of which toluene reaches 163.1°), thereby improving wettability selectivity and decreasing oil adhesion, permitting the fabricated UiO-66-NH 2 @h-PPS membranes to effectively separate different types of O/W emulsions. The UiO-66-NH 2 @h-PPS membranes acquire excellent permeate fluxes (for the surfactant-free toluene-in-water emulsion, it reaches up to 7638.1 L m −2 h −1 ) and separation accuracy (99.1% oil rejection). Moreover, the UiO-66-NH 2 @h-PPS membrane exhibited outstanding harsh environment resistance. Interestingly, the combination of UiO-66-NH 2 and h-PPS substrate was applicable to degrade the organic compound in water, and the degradation efficiency of the methylene blue achieved 85.7% under visible light within 120 min. In summary, loading Zr-MOFs onto h-PPS substrates provides a novel strategy for the efficient treatment of wastewater under complex conditions with great potential for practical applications.
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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
·
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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