ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Huiwen Wang,Sihao Wu,Zoujun Peng,Xiulin Wang,Juanhua Lai,Ping Qiu
The quantitative analysis of glyphosate has significant implications for the evaluation of food quality and environmental safety risks. First, copper nanoparticles (Cu NPs) were synthesized using cetyltrimethylammonium bromide (CTAB) as a stabilizing agent, which resolved the limitation associated with atmospheric oxidation of Cu NPs and provided excellent fluorescence stability. Interestingly, the fluorescence of blue-emitting CTAB-Cu NPs was quenched by pH-responsive p-nitrophenol (p-NP) via Förster resonance energy transfer. Herein, a dual read-out sensor based on CTAB-Cu NPs and p-NP was constructed for glyphosate detection. Specifically, acetic acid (HAc) from acetylcholine (ACh) via hydrolysis catalyzed by acetyl cholinesterase (AChE) reduced the pH of the mixed solution and prevented the loss of protons from p-NP, which allowed the fluorescence emission by CTAB-Cu NPs. The presence of glyphosate inhibited the activity of AChE, and the increased pH resulted in proton loss. The fluorescence intensity of CTAB-Cu NPs was quenched, and the solution color changed from colorless to yellow with a UV absorption peak at 400 nm. The sensor can detect ultra-trace levels of glyphosate residues with a limit of detection of 5.43 ng/L. The obtained biosensor was successfully utilized to monitor the degradation of glyphosate in the roots of cabbage and cultivated soil.
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Small
·
2023
·Vol. 19
·期 37
·2301085
·
IF 13.3
Guo Liu,Qi Zeng,Xinyi Sui,Shuhao Tian,Xiao Sun,Qingfeng Wu,Xijuan Li,Yuhao Zhang,Kun Tao,Erqing Xie,Zhenxing Zhang
Polysulfide shuttle effect and sluggish sulfur reaction kinetics severely impede the cycling stability and sulfur utilization of lithium-sulfur (Li-S) batteries. Modulating d-band electronic structures of molybdenum disulfide electrocatalysts via p/n doping is promising to boost polysulfide conversion and suppress polysulfide migration in lithium-sulfur batteries. Herein, p-type V-doped MoS 2 (V-MoS 2 ) and n-type Mn-doped MoS 2 (Mn-MoS 2 ) catalysts are well-designed. Experimental results and theoretical analyses reveal that both of them significantly increase the binding energy of polysulfides on the catalysts’ surface and accelerate the sluggish conversion kinetics of sulfur species. Particularly, the p-type V-MoS 2 catalyst exhibits a more obvious bidirectional catalytic effect. Electronic structure analysis further demonstrates that the superior anchoring and electrocatalytic activities are originated from the upward shift of the d-band center and the optimized electronic structure induced by duplex metal coupling. As a result, the Li-S batteries with V-MoS 2 modified separator exhibit a high initial capacity of 1607.2 mAh g −1 at 0.2 C and excellent rate and cycling performance. Moreover, even at a high sulfur loading of 6.84 mg cm −2 , a favorable initial areal capacity of 8.98 mAh cm −2 is achieved at 0.1 C. This work may bring widespread attention to atomic engineering in catalyst design for high-performance Li-S batteries.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2023
·
IF 2.6
Zhenxing Cai,Pingxin Li,Hui Zhao,Lingyan Wang,Xiaobo Chen,Chaohe Yang
The solubility of cyclohexanone, tert-butanol, and 1,4-dioxane in p-, o-, and m-xylenes and ethylbenzene was measured by a gas chromatography method under an atmospheric environment. The measured data indicated that the solubility of cyclohexanone, tert-butanol, and 1,4-dioxane in the xylenes and ethylbenzene increases with increasing temperature. The experimentally determined solubility results were fitted with the modified Apelblat equation, Van’t Hoff equation, and Wilson model. Among them, the Wilson model was most consistent with the measured solubility results. The dissolution-related thermodynamic properties of cyclohexanone, tert-butanol, and 1,4-dioxane in xylenes and ethylbenzene, including the changes of molar Gibbs free energy, molar enthalpy, and molar entropy, were predicted and analyzed via the correlated Wilson model, which indicates that the dissolution behaviors are spontaneous and endothermic process. The obtained solubility results provide the thermodynamic foundation for the development and upgrading of industrial separation processes related to xylene, ethylbenzene, cyclohexanone, tert-butanol, and 1,4-dioxane.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Liu Jianming,Zhang Han,Xu Yingying,Meng Hao,Zeng An-Ping
The use of gaseous and air-captured CO 2 for technical biosynthesis is highly desired, but elusive so far due to several obstacles including high energy (ATP, NADPH) demand, low thermodynamic driving force and limited biosynthesis rate. Here, we present an ATP and NAD(P)H-free chemoenzymatic system for amino acid and pyruvate biosynthesis by coupling methanol with CO 2 . It relies on a re-engineered glycine cleavage system with the NAD(P)H-dependent L protein replaced by biocompatible chemical reduction of protein H with dithiothreitol. The latter provides a higher thermodynamic driving force, determines the reaction direction, and avoids protein polymerization of the rate-limiting enzyme carboxylase. Engineering of H protein to effectively release the lipoamide arm from a protected state further enhanced the system performance, achieving the synthesis of glycine, serine and pyruvate at g/L level from methanol and air-captured CO 2 . This work opens up the door for biosynthesis of amino acids and derived products from air.
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高影响因子
Materials Today Sustainability
·
2023
·
IF 7.8
Z. Hao,Q. Zhao,Y. Wang,H. Lu,X. Liu,Q. He,T. Wang,J. Wang,J. He,W. Wang
The complete removal of harmful phenolic contaminants from water remains huge challenge because of the lack of cost-effective and powerful adsorbents. Herein, a sustainable nitrogen self-doped biochar (named KBC750N) with large specific surface area (1398.44 m 2 /g), high adsorption capacity (606.06 mg/g) and removal ratio (99.99%) for p -nitrophenol (PNP) in real waters (Seawater, Yangtze River water , and Yellow River water) was prepared from a naturally abundant protein-rich psammophyte Caragana korshinskii (CK) by a facile one-step pyrolysis process . The in-situ nitrogen-doped biochar shows much better adsorption removal efficiency of 99.99% toward PNP than expensive commercial adsorbents (only 77.52%). The biochar still keeps high adsorption efficiency after reused more than five times. Site energy distribution analysis revealed that the biochar captures PNP mainly through n–π and π–π electron-donor–acceptor interactions among the electron-rich functional groups (N-containing moieties, –COOH, and –OH), graphite carbon, and PNP. Density functional theory (DFT) calculations confirmed that the nitrogen site in biochar helps to strengthen its adsorption capability to PNP. This work provides a sustainable platform for the development of high-performance, cost-effective materials for efficient elimination of organic pollutants from water.
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JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Qingqin Sun,Xu Fu,Peiru Wang,Kunlan Li,Ligang Wei,Shangru Zhai,Qingda An
The oxidative depolymerization of alkali lignin (AL) catalyzed by copper-containing imidazolium-based ionic liquids ([C 4 C 1 im]CuCl 3 ) was investigated with CH 3 OH-H 2 O (9/1, v/v) as solvent under an initial oxygen pressure of 1.5 MPa at 150 °C for 3 h. Compared with other transition-metal chlorides and metal-containing ionic liquids (ILs), [C 4 C 1 im]CuCl 3 presented a relatively remarkable catalytic capacity for AL oxidative depolymerization due to the cooperative effects of [C 4 C 1 im] + and CuCl 3 − . [C 4 C 1 im]CuCl 3 molar concentration ( x McIL ) greatly influenced AL conversion and product selectivity. The highest AL conversion of 70.4% was achieved at x McIL = 0.18 mol.%. For the obtained small-molecule products, the highest selectivity of p -hydroxybenzaldehyde reached 51.3% at x McIL = 0.72mol.% (corresponding yield of 103.6 mg·g −1 ). The inter-unit linkages of lignin were effectively cleaved in the oxidative depolymerization catalyzed by [C 4 C 1 im]CuCl 3 , and the H unit in lignin was preferentially destroyed. The molecular interactions and microenvironment of [C 4 C 1 im]CuCl 3 –solvent (CH 3 OH-H 2 O) system were investigated with x McIL varied from 0.05 mol.% to 5.12 mol.% by using attenuated total reflectance-infrared spectroscopy and molecular-dynamics method, respectively. The catalytic properties of [C 4 C 1 im]CuCl 3 strongly depended on the interactions of [C 4 C 1 im]CuCl 3 and solvent molecules with changes in microstructure organization. The optimum catalytic capacity of [C 4 C 1 im]CuCl 3 was obtained when the ion pair formed through hydrogen bonding at x McIL = 0.18–0.36 mol.%. The solvation of solvent molecules on CuCl 3 − and the formation of ionic cluster with the hydrogen-bonding self-association of [C 4 C 1 im]CuCl 3 were unfavorable for the oxidative depolymerization of lignin.
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高影响因子
JOURNAL OF POLYMER RESEARCH
·
2023
·Vol. 30
·期 5
·1-15
·
IF 2.8
Bai Xiaodong,Li Ke,Hu Hua,Yan Yancheng,Luo Yumei
A new anionic polymer poly(acrylamide-co-N-vinylpyrrolidone-co-sodium p-styrene sulfonate) (abbreviated as PANS) is synthesized by using acrylamide(AM), N-vinylpyrrolidone(NVP) and sodium p-styrene sulfonate(SSS) as monomers and used as filter loss agents. The optimal synthesis process conditions are explored by orthogonal experiments: molar ratio is AM:NVP:SSS = 3.5; 2; 1, the monomer concentration is 35 wt%, the initiator concentration is 0.40 wt%, the reaction temperature is 45 °C, and the reaction time is 4 h. Fourier infrared spectroscopy(FTIR)and nuclear magnetic resonance hydrogen spectroscopy( 1 HNMR) hydrogen spectroscopy are used to characterize it. Through thermogravimetric analysis(TG) testing, its temperature resistance is tested, and it is found that it has good thermal stability before 350 °C. The performance test is carried out using American Petroleum Institute(API) evaluation criteria, and it is found that the filter loss before aging is 7.5 mL under 2 wt% addition, and only 8 mL after aging. At the same time, after the addition of PANS, the salt resistance of drilling fluid after high temperature aging is improved, and the filtration loss after aging is only 8.25 mL under the addition of 12 wt% NaCl, while the filtration loss after aging is 8.2 mL under the addition of CaCl 2 at 3 wt%. Through Zeta potential and particle size analysis, after adding PANS, the particle size of clay particles can be greatly reduced after aging, and the zeta potential value of drilling fluid is optimized under calcium salt contamination.
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INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Haoran Yuan,Chengyu Li,Rui Shan,Jun Zhang,Yong Chen
In the present study, selective transformation of waste cassava residues into aromatics via catalytic pyrolysis over as-prepared La and P modified ZSM-5 was systematically investigated, especially in the aspects of product regulation and kinetic analysis. Comprehensive physicochemical characterizations were undertaken for unveiling the essential structural properties of La and P modified ZSM-5. The introduction of La and P species significantly enriched the Lewis and Brønsted acid sites in ZSM-5, thus facilitating the directional pyrolysis of waste cassava residues into aromatics. Higher apparent activation energy for aromatics formation from waste cassava residues pyrolysis in the presence of La and P modified ZSM-5 might be due to the fact that the catalytic pyrolysis belonged to diffusion-controlled gas-solid reaction. In comparison with that of the parent ZSM-5, LaP 2 /ZSM exhibited better performance towards aromatics formation in waste cassava residues pyrolysis, wherein the relative content of aromatics reached 83.3% at a temperature of 650 °C. Gratifyingly, the relative content of aromatics was increased to 90.5% for the catalytic pyrolysis of acid pretreated cassava residue, in the case of LaP 1 /ZSM catalyst.
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CANCER LETTERS
·
2023
·
IF 9.7
Ruikun Lin,Lei Zhang,Biwei Ye,Yanan Wang,Yi-Dong Li,Hsu Jason,Wenzhen Liu,Ping Hu,Jincan Chen,Zhe-Sheng Chen,Zhuo Chen
P-glycoprotein (P-gp/ABCB1)-mediated multidrug resistance (MDR) in cancers severely limit chemotherapeutic efficacy. We recently reported that phosphatidylinositol-3-kinase (PI3K) 110α and 110β subunits can be novel targets for reversal of P-gp mediated MDR in cancers, and BAY-1082439 as an inhibitor specific for PI3K 110α and 110β subunits could reverse P-gp-mediated MDR by downregulating P-gp expression in cancer cells. However, BAY-1082439 has very low solubility, short half-life and high in-vivo clearance rate. Till now, nano-system with the functions to target PI3K P110α and P110β and reverse P-gp mediated MDR in cancers has not been reported. In our study, a tumor targeting drug delivery nano-system PBDF was established, which comprised doxorubicin (DOX) and BAY-1082439 respectively encapsulated by biodegradable PLGA-SH nanoparticles (NPs) that were grafted to gold nanorods (Au NRs) modified with FA-PEG-SH, to enhance the efficacy to reverse P-gp mediated MDR and to target tumor cells, further, to enhance the efficiency to inhibit MDR tumors overexpressing P-gp. In-vitro experiments indicated that PBDF NPs greatly enhanced uptake of DOX, improved the activity to reverse MDR, inhibited the cell proliferation, and induced S-phase arrest and apoptosis in KB-C2 cells, as compared with free DOX combining free BAY-1082439. In-vivo experiments further demonstrated that PBDF NPs improved the anti-tumor ability of DOX and inhibited development of KB-C2 tumors. Notably, the metastasis of KB-C2 cells in livers and lungs of nude mice were inhibited by treatment with PBDF NPs, which showed no obvious in-vitro or in-vivo toxicity.
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高影响因子
Small
·
2023
·Vol. 19
·期 30
·2300770
·
IF 13.3
Shilin Zhang,Qingjie Wang,Peng Zhang,Jie Wang,Yue Li,Chang Lu,Muhammad Tariq Sarwar,Xiongbo Dong,Qihang Zhao,Aidong Tang,Liangjie Fu,Huaming Yang
To achieve a high separation efficiency of photogenerated carriers in semiconductors, constructing high-quality heterogeneous interfaces as charge flow highways is critical and challenging. This study successfully demonstrates an interfacial chemical bond and internal electric field (IEF) simultaneously modulated 0D/0D/1D-Co 3 O 4 /TiO 2 /sepiolite composite catalyst by exploiting sepiolite surface-interfacial interactions to adjust the Co 2+ /Co 3+ ratio at the Co 3 O 4 /TiO 2 heterointerface. In situ irradiation X-ray photoelectron spectroscopy and density functional theory (DFT) calculations reveal that the interfacial Co 2+ O Ti bond (compared to the Co 3+ O Ti bond) plays a major role as an atomic-level charge transport channel at the p-n junction. Co 2+ /Co 3+ ratio increase also enhances the IEF intensity. Therefore, the enhanced IEF cooperates with the interfacial Co 2+ O Ti bond to enhance the photoelectron separation and migration efficiency. A coupled photocatalysis-peroxymonosulfate activation system is used to evaluate the catalytic activity of Co 3 O 4 /TiO 2 /sepiolite. Furthermore, this work demonstrates how efficiently separated photoelectrons facilitate the synergy between photocatalysis and peroxymonosulfate activation to achieve deep pollutant degradation and reduce its ecotoxicity. This study presents a new strategy for constructing high-quality heterogeneous interfaces by consciously modulating interfacial chemical bonds and IEF, and the strategy is expected to extend to this class of spinel-structured semiconductors.
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Materials Today Chemistry
·
2023
·
IF 7.3
H. Chai,R. Li,L. Gao,H. Niu,J. Jin
The phase interface properties of the p-n junction may profoundly affect its photoelectrochemical (PEC) water oxidation performance. Here, we introduced a non-conjugated polymer functional layer (poly(diallyl-dimethylammonium chloride, PDDA) between the interfaces of the p-n junction (Co 3 O 4 /Gd–Fe 2 O 3 ) to tune the interfacial properties . First, the PDDA modulates the band structure so that the composite photoanode (Co 3 O 4 /PDDA/Gd–Fe 2 O 3 ) has an enlarger band bending than the p-n junction. Then, PDDA passivates the surface trap, which synergizes with Co 3 O 4 to provide more active sites for water oxidation. Furthermore, PDDA improves the PEC water oxidation kinetics. Specifically, PDDA extracts holes and adsorbs water oxidation reactants, thus it efficiently transfers photogenerated holes to Co 3 O 4 , promoting the water oxidation reaction in the positive direction. With these positive modulations, PDDA can further enhance the PEC water oxidation performance of the p-n junction. This conceptual work provides insight into the role of the non-conjugated polymer in PEC water splitting .
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Journal of Materials Research and Technology-JMR&T
·
2023
·
IF 6.4
Hongyuan Zhao,Meimei Guo,Fang Li,Yu Zhou,Gan Zhu,Yunhang Liu,Qiwen Ran,Fuquan Nie,Volodymyr Dubovyk
The efficient and accurate detection of gallic acid (GA) is particularly important for human health. Herein, a simple and low-cost ultrasonic-assisted strategy was proposed for the preparation of multifunctional nanocomposite of Super-P carbon black (SPCB) nanoparticles and mesoporous silica nanoparticles (MSNs), which was used to modify the glassy carbon electrode (GCE) for the fabrication of GA electrochemical sensor (SPCB@MSNs/GCE). SPCB with pearl-chain nanostructure presented an interconnected highly conductive carbon network, which significantly improved the charge transfer efficiency. MSNs with spherical morphology and mesoporous structure exhibited uniform particle dispersion and high active surface area, which remarkably improved the surface accumulation effect of sensing electrode towards GA. Moreover, the excellent electrical conductivity of SPCB compensated for the non-conductive property of MSNs. Under the optimized condition, the electrochemical response of SPCB@MSNs/GCE sensor had a good linear relationship with GA concentration (0.5–10 μM), and the corresponding limit of detection could reach up to 4.911 nM. The fabricated nanohybrid sensor showed good reproducibility, repeatability and anti-interference property. Moreover, the satisfactory GA recoveries and RSD values were achieved for the electrochemical detection of GA in tea samples. This work provides an important reference for the highly sensitive analysis of GA in the field of food safety.
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