LANGMUIR
·
2022
·
IF 4.331
Jie Han,Yao Liang,Chengxiu He,Yujia Tong,Weixing Li
A catalytic composite membrane was developed for the enhancement of esterification by lyophilization for the first time. The catalytic composite membrane was composed of a poly(vinyl alcohol) (PVA)-sodium alginate (SA) separation layer and a spongy porous catalytic layer cross-linked by PVA and 4-sulfophthalic acid (SPA). Fourier transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS) results indicated the successful synthesis of the catalytic composite membrane. The membrane properties were evaluated by ethanol dehydration and esterification. The conversion rate of acetic acid reached 95.9% after 12 h. Compared with batch reactions, the conversion rate increased by 24.4%. After five cycles, the membrane still maintained outstanding catalytic activity. The resistance of mass transfer was analyzed, and the results showed that the porous structure reduced the catalytic layer resistance to total resistance from 70.27 to 32.88%. The composite membrane with a spongy porous catalytic layer exhibited superior dehydration and catalytic performance.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
·
IF 4.598
Jie Wei,Yumeng Li,Qingyang Si,Qiao Xiao,Qingmin Chen,Tianhui Jiao,Quansheng Chen,Xiaomei Chen
A label-free, sensitive and reliable electrochemical sensor based on hemin/G-quadruplex (G4) DNAzyme was engineered to determine adenosine triphosphate (ATP) in fish. The nucleic acid sequence (DNA1) including the G4 sequence subunit and anti-ATP aptamer segment is anchored on Au electrodes. The nucleic acid sequence (DNA2) is composed of another G4 sequence fragment and anti-ATP aptamer subunit. The probes DNA1 and DNA2 self-assemble into the active hemin/G4 DNAzyme structure on Au electrodes upon exposure to the target ATP. The determination of the target ATP relied on an increase in the catalytic currents occurring on DNAzyme-anchored electrode via the electrochemical reduction of H 2 O 2 . The proposed strategy enables high-performance and specified determination of the target ATP with a detection limit of 0.04 μmol/L. Specifically, the proposed ATP strategy was further implemented to determine ATP in microorganisms in carp samples. Compared with the classical total viable count (TVC) assay, the proposed ATP assay was feasible to assess the freshness of carp, which expands the applications of hemin/G4 DNAzyme and holds promising potential for freshness assessment in food safety.
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AQUACULTURE
·
2022
·
IF 5.135
Linhan Li,Tao Zhang,Gengrong Zhang,Guoqing Zhou,Fei Yang,Erlong Wang,Tianqiang Liu,Gaoxue Wang
Micropterus salmoides rhabdovirus (MSRV) seriously threats largemouth bass farming in China. Vaccine is a widely-used way to protect against virus infection. However, traditional intramuscular injection is inconvenient, time-consuming, and hard to applicate universally. We employed the naturally biodegradable bacterial nanocellulose (BNC) as effective virus antigen carriers for bath vaccination and improving the largemouth bass immune response. In this study, 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-mediated oxidation of bacterial cellulose (BC) was applied to produce carboxylated BC, which was validated by Fourier transform infrared spectroscopy (FTIR) and elementary analysis. Followed by a controlled sulfuric acid hydrolysis reaction to form carboxylated bacterial nanocellulose (BNC-COOH) with an average size of about 350 nm. Amination reaction was conducted via conjugating the amine groups in MSRV glycoproteins (G) with the carboxyl groups in the BNC-COOH. The prepared bacterial nanocellulose loaded glycoprotein complex (BNCs-G) was used to vaccine largemouth bass via bath immunization. The protective effects were assessed by analyzing MSRV G proteins-specific serum antibody levels and the expression of four immune-related genes ( IgM , IL-12 , TCR , TNF- α, and CD4 ). Results showed that serum antibody levels and the expression of immune-related genes were significantly increased for BNCs-G bath-vaccinated groups (40 mg L −1 ), compared with PBS and the naked G protein groups. After bath immunization for four weeks, fish were challenged with a lethal dose of MSRV. The survival rates for control group (PBS), BNCs group (40 mg L −1 ), the naked G protein groups (40 mg L −1 ) and three BNCs-G groups (10 mg L −1 , 20 mg L −1 and 40 mg L −1 ) were 0%, 0%, 30.0%, 16.7%, 46.7% and 66.7%, respectively. These results indicated that BNCs could be a plausible candidate for the vaccine carrier system, and the BNC loaded glycoprotein showed good immunogenicity.
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Molecular Catalysis
·
2022
·
IF 5.089
Jie Xu,Jiusheng Shi,Jingyu Wang,Lihui Zhang,Yujie Wang
Depolymerizing lignin to prepare aromatic high-value chemicals is beneficial to solve the problem of energy shortage and waste of resources. However, cleavage of lignin C C bonds still faces greater challenges due to the recalcitrance of C C bonds in lignin. Photocatalysis is considered to be a promising way to break lignin C C bonds under mild conditions. Here, the micellar aqueous medium (SDS) composed of sodium lauryl sulfonate and water was prepared. 1, 2-Diphenylethanol (lignin model compound, Dpol) and dioxanesolv poplar lignin can be well dispersed in SDS-8 (mass fraction of 0.08% for sodium lauryl sulfate). Photocatalyst g-C 3 N 4 can efficiently break the lignin C C bonds in SDS-8 and very high photocatalytic efficiency can be obtained. A small amount of acetic acid can further improve photocatalytic efficiency. The main products produced by photocatalytic breaking lignin C C bonds are benzaldehyde and benzoic acid. The mechanism of photocatalytic cleavage of lignin C C bonds mainly follows a photogenerated electron-hole coupled redox mechanism. Thereinto, the hydrogen provided by SDS-8 has powerfully promoted photocatalytic efficiency. Our work provides a new direction for photocatalytic cleavage of lignin C C bonds into aromatic high-value chemicals.
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Nanomaterials
·
2022
·Vol. 12
·期 18
·3089
·
IF 5.719
Li Tan,Yiming Chen,Didi Li,Shaobin Wang,Zhimin Ao
An in situ photo-Fenton system can continuously generate H2O2by photocatalysis, activating H2O2in situ to form strong oxidizing ·OH radicals and degrading organic pollutants. A WSe2/g-C3N4composite catalyst with WSe2as a co-catalyst was successfully synthesized in this work and used for in situ photo-Fenton oxidation. The WSe2/g-C3N4composite with 7% loading of WSe2(CNW2) has H2O2production of 35.04 μmol/L, which is fourteen times higher than pure g-C3N4. The degradation efficiency of CNW2 for phenol reached 67%. By constructing an in situ Fenton-system, the phenol degradation rate could be further enhanced to 90%. WSe2can enhance the catalytic activity of CNW2 by increasing electron mobility and inhibiting the recombination of photogenerated electron–hole pairs. Moreover, the addition of Fe2+activates the generated H2O2, thus increasing the amount of strong oxidative ·OH radicals for the degradation of phenol. Overall, CNW2 is a promising novel material with a high H2O2yield and can directly degrade organic pollutants using an in situ photo-Fenton reaction.Keywords:WSe2/g-C3N4;visible light;in situ photo-Fenton;phenol degradation
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 101
·期 4
·2199-2211
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IF 2.5
Zheng Zeng,Haikuan Yuan,Jie Lu
Graphene oxide (GO) has extensive applications in membrane-based separations, but its dispersion in the membrane has always been a problem due to the presence of π–π interactions in GO nanosheets. In this study, a grafting reaction was designed by using poly (vinyl alcohol) (PVA) for GO grafting modification and poly (vinyl alcohol)-g-graphene oxide (PVA-g-GO) nanocomposites were synthesized. The grafting material to GO was the same as the basic separation polymer material. PVA-g-GO showed better dispersibility and hydrophilicity than GO, and a series of composite membranes were prepared using a polyacrylonitrile (PAN) ultrafiltration (UF) membrane as a substrate. PVA-g-GO nanocomposites and membranes were characterized by using X-ray diffraction (XRD), thermogravimetric analysis (TGA), Fourier-transform infrared spectroscopy (FTIR), water contact angle, scanning electron microscopy (SEM), etc. The addition of PVA-g-GO improved both the separation performance and anti-swelling property of the composite membrane, and the PVA-g-GO/PVA/PAN composite membrane loaded with 2 wt.% PVA-g-GO obtained a high flux of 4.46 kg/m 2 · h and a high rejection of 99.99% when dehydrating 3.5 wt.% NaCl solution at 30°C by pervaporation.
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Micro & Nano Letters
·
2022
·Vol. 17
·期 11
·259-271
·
IF 0.98
Yunting Wang,Qing-an Qiao,Honglan Cai,Juan Jin,Hongwei Gao,Yanbin Xu
g-C 3 N 4 was employed as a modified substance for modification engineering of wurtzite-ZnS photocatalysts to overcome its limited light response and stability. The g-C 3 N 4 /ZnS (CNZS) photocatalyst was synthesized by solvothermal reaction of g-C 3 N 4 , thiourea and zinc acetate. The results show that wurtzite-ZnS spheres were loaded on the surface of g-C 3 N 4 with well uniformed size. The photocatalytic activity of the catalyst was determined by the degradation of MB and Rh.B under visible light. The degradation rates of Rh.B and MB by CNZS were 96% and 97%, much better than that of pure ZnS. The addition of g-C 3 N 4 promoted the visible light response of wurtzite-ZnS and inhibited the recombination of photogenerated electrons with holes. The density functional theory (DFT) results indicated that the components of both valence band and conductive band were changed for the CNZS system. Compared to pure ZnS, the band gap of CNZS was decreased about 0.5 eV, and the work function calculations were in good agreement with the experimental results. As a result, the heterostructure of CNZS made it beneficial to the electron transfer from g-C 3 N 4 (2p of N) to ZnS (3p of S) and absorption edge has been extended to about 600 nm.
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Biomaterials Science
·
2022
·Vol. 10
·期 15
·4284-4292
·
IF 7.59
Ruixia Liu,Tingting Ding,Pingping Deng,Xiaofan Yan,Fuquan Xiong,Jienan Chen,Zhiping Wu
This work was carried out in order to broaden the application field of lignin and improve its additional value. The degraded deep eutectic solvent lignin-grafted poly(N-vinyl caprolactam) (DES-lignin-g-PNVCL) was synthesized by using modified DES-lignin and NVCL via activators regenerated by electron transfer-atom transfer radical polymerization (ARGET-ATRP). Aspirin was coated with DES-lignin-g-PNVCL through self-assembly by an ethanol/water anti-solvent method to obtain lignin thermosensitive polymer nanoparticle coated aspirin (aspirin@LTNP). X-ray electron spectroscopy (XPS), elemental analysis, scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), dynamic light scattering (DLS), and ultraviolet visible spectroscopy (UV) were used to characterize the composition, structure and morphology of DES-lignin-g-PNVCL and aspirin@LTNP. The releasing behavior of aspirin@LTNP at different temperatures and pH values was investigated. The safety was evaluated by cytotoxicity tests. The results indicated that aspirin@LTNP was mainly accumulated by the hydrophobic effect and π–π interaction in the process of self-assembly, and its morphology was an ellipsoid stacked layer by layer. The aspirin@LTNP hydrophilic chains were increased and had externally hydrophilic and internally hydrophobic structures. The particle size decreased slightly during the self-assembly process. The red-shift occurred at the π–π interaction wavelength of the lignin aromatic ring, which indicated a physical coating process. The coating rate of aspirin@LTNP was 88.87%. Aspirin@LTNP showed an obvious temperature response; the 96 h cumulative release rate at the LCST was 73.75 ± 1.16%, while the 96 h cumulative release rate above the LCST was 28.10 ± 0.92%. The 96 h cumulative release rate was 63.21 ± 0.57% at pH = 1.5 and 49.56 ± 0.48% at pH = 7.4. The dosage of aspirin@LTNP used in the experiment was safe. This study provided a strategy for drug coating and controlled release.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xinran Li,Shuohan Li,Jian Xu,Lanxin Wang,Kaiwei Liang,Huihui Zhang,Xuelian Yu,Zhongwei Liu
Photoconversion of CO 2 into fuel is critical for realizing a net-zero emission future, but it remains an open challenge due to the unsatisfactory light absorption and photogenerated carriers’ separation efficiency of catalysts. In this work, upon in situ thermal polymerization method, the nanodiamond (ND) are homogeneously and solidly modified on the defective graphitic carbon nitride (g-C 3 N 4 ) surface. Under visible light irradiation, the ND/g-C 3 N 4 (NH) exhibits excellent CO 2 photocatalytic performance with a CO yield of 10.98 μmol/h (18.6 times higher than bulk g-C 3 N 4 ), predominant performance in the selectivity of CO and cyclic stability. The improved CO 2 photoreduction ability was sourced from the synergetic effect of nitrogen vacancies engineering and ND decoration, which also significantly improved visible light absorption capacity and facilitated electron transport pathways, and promoted the separation and transfer of charge carriers efficiently.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xiaohui Zhan,Junyan Liu,Yue Zhao,Yanping Sun,Rui Gao,He Wang,Huixiang Shi
In this study, we designed and synthesized Mn III with tunable spin state in g-C 3 N 4 through one-step calcination of Mn-MOF. The Mn atoms were induced into the six-fold cavity of the g-C 3 N 4 lattice and formed Mn-N 6 coordination. Mn-MOF served as the source of Mn. The collapse of Mn-MOF effectively promoted the stripping of stacked layers in g-C 3 N 4 and increased the atomic loading. The Mn-N coordination induced impurity energy levels which effectively regulated Mnx-CN's bandgap structure and accelerated the migration and separation of carriers. The O 2 − was activated to 1 O 2 by the energy released from the high-spin Mn III transferred ground state. The H 2 production of Mn 10 -CN (13479.19 µmol·g −1 ·h −1 ) is ∼32.2 times that of CN under visible light irradiation and with a remarkable apparent quantum yield (AQY) of 12.23% at 420 nm. The rates of TC degradation and Cr (VI) reduction achieved 0.059 and 0.18 min −1 , respectively. In addition, the practical application conditions and catalytic mechanism of Mnx-CN were explored. This work demonstrates the connection of the spin state of metal with the photocatalytic activity, providing an efficient photocatalytic system that can be used for solar-chemical energy conversion and pollution remediation, and presenting a new approach for modifying the g-C 3 N 4 -based catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Qi Yin,Hao Zhou
Water pollution has received much attention and constructing efficient catalysts to photodegrade the pollutants is a promising method. Herein, we reported that a novel composite catalyst, NaNb x Ta 1−x O 3 /g-C 3 N 4 , exhibited high efficiency to degrade the model pollutant, methylene blue (MB), in ultraviolet light. The optimal catalyst was NaNb 0.75 Ta 0.25 O 3 /g-C 3 N 4 (1:9), which degraded 99.6% of MB (10 mg/L) after 180 min of reaction. The superior photocatalytic activity was attributed to the formation of the Z-scheme heterojunction, which could suppress the recombination of the photogenerated electron-hole pairs and protect the high redox potentials simultaneously. Hydroxyl radicals ( . OH) and superoxide radicals ( . O 2 - ) were found to be the dominant active free radicals in the reaction process and a possible photocatalytic mechanism over the catalyst was proposed accordingly. This work provides an efficient direction to fabricate composite photocatalysts and helps to overcome the shortcomings of a single catalyst.
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RSC Advances
·
2021
·Vol. 11
·期 49
·30503-30509
·
IF 3.361
Xiupei Yang,Lin Zhang,Dan Wang,Qian Zhang,Jie Zeng,Run Zhang
Developing a new photocatalyst for fast and highly efficient organic dye degradation plays an essential role in wastewater treatment. In this study, a photocatalyst graphite phase carbon nitride (g-C3N4) containing nitrogen defects (CN) is reported for the degradation of rhodamine B (RhB). The porous g-C3N4 photocatalyst is facilely synthesized through a polycondensation method and then characterized by X-ray diffraction (XRD), infrared spectroscopy (FT-IR), field emission scanning electron microscopy (FESEM), N2 isotherm adsorption line, and X-ray photoelectron spectroscopy (XPS). The photocatalytic activity of the g-C3N4 is evaluated through the degradation of RhB under visible light irradiation. The results show that photocatalytic activity of the nitrogen-defective g-C3N4 can be improved by optimizating washing conditions, including washing temperature, washing dosage, drying time, and drying temperature. With the prepared nitrogen-defective g-C3N4, decolourization of RhB is able to be completed within 20 minutes, in which the degradation rate is 1.7 times higher than that of bulk g-C3N4. Moreover, the nitrogen-defective g-C3N4 has high stability and reusability in the degradation of RhB. Photocatalytic degradation mechanism investigations by ultraviolet-visible absorption spectroscopy, radical trapping experiments and high-performance liquid chromatography (HPLC) reveal that RhB achieved complete mineralization through the photocatalytic degradation reaction mediated by superoxide radicals (˙O2−). This work thus provides a new approach for the preparation of photocatalysts for organic pollutants treatment in wastewater samples.
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