CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Bin Han,Yuanfang Lin,Yu Luo,Weizhen Liu,Xueming Liu,Zonglin Weng,Xinwen Ou,Zhang Lin
Low-crystalline ultrathin nanosheets (UNSs) hold great potential for efficient photoreduction of anthropogenic CO 2 , while developing green synthetic methodologies and elucidating the structure-performance relationship remain significant challenges. Here, via a CaO-mediated strategy , we demonstrate a facile strategy for the large-scale production of low-crystalline Ni(OH) 2 UNSs from industrial wastes. The resultant Ni(OH) 2 UNSs deliver a superior CO formation rate of 9.2 μmol h −1 with a high selectivity of 93.1 % in low-concentration CO 2 (10 %), which remarkably outperforms that of Ni(OH) 2 NSs with high crystalline. Experimental and theoretical investigations demonstrate that the boosted performance originates from the fully exposed oxygen vacancies and low-coordination Ni sites, which facilitates the separation of photogenerated charge pairs and the adsorption and activation of diluted CO 2 . This work demonstrates a sustainable strategy for the large-scale synthesis of low-crystalline layered metal hydroxides, paving new avenues for the high-value utilization of industrial wastes in mitigating climate change.
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Nature Communications
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2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Liu Heming,Xie Ruikuan,Luo Yuting,Cui Zhicheng,Yu Qiangmin,Gao Zhiqiang,Zhang Zhiyuan,Yang Fengning,Kang Xin,Ge Shiyu,Li Shaohai,Gao Xuefeng,Chai Guoliang,Liu Le,Liu Bilu
Constructing stable electrodes which function over long timescales at large current density is essential for the industrial realization and implementation of water electrolysis. However, rapid gas bubble detachment at large current density usually results in peeling-off of electrocatalysts and performance degradation, especially for long term operations. Here we construct a mechanically-stable, all-metal, and highly active CuMo 6 S 8 /Cu electrode by in-situ reaction between MoS 2 and Cu. The Chevrel phase electrode exhibits strong binding at the electrocatalyst-support interface with weak adhesion at electrocatalyst-bubble interface, in addition to fast hydrogen evolution and charge transfer kinetics. These features facilitate the achievement of large current density of 2500 mA cm −2 at a small overpotential of 334 mV which operate stably at 2500 mA cm −2 for over 100 h. In-situ total internal reflection imaging at micrometer level and mechanical tests disclose the relationships of two interfacial forces and performance of electrocatalysts. This dual interfacial engineering strategy can be extended to construct stable and high-performance electrodes for other gas-involving reactions.
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高影响因子
Journal of Central South University
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2022
·Vol. 29
·期 9
·2980-2990
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IF 2.392
Wang Zhen-yu,Li Cong,Huang Ying-de,He Zhen-jiang,Yan Cheng,Mao Jing,Dai Ke-hua,Zheng Jun-chao
With increasing demand on energy density of lithium-ion battery, wide electrochemical window and safety performance are the crucial request for next generation electrolyte. Gel-electrolyte as a pioneer for electrolyte solidization development aims to solve the safety and electrochemical window problems. However, low ionic conductivity and poor physical performance prohibit its further application. Herein, a fast-ionic conductor (Li 2.64 (Sc 0.9 Ti 0.1 ) 2 (PO 4 ) 3 ) (LSTP) was added into poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) base gel-electrolyte to enhance mechanical properties and ionic conductivity. Evidences reveal that LSTP was able to weaken interforce between polymer chains, which increased the ionic conductibility and decreased interface resistance during the cycling significantly. The obtained LiFePO 4 /hybrid gel-electrolyte/Li-metal coin cell exhibited excellent rate capacity (145 mA·h/g at 1 C , 95 mA·h/g at 3 C , 28 °C) which presented a potential that can be comparable with commercialized liquid electrolyte system.
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Analytical Methods
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2022
·Vol. 14
·期 48
·5091-5099
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IF 3.532
Yue Sun,Zihao Xie,Fubin Pei,Wei Hu,Shasha Feng,Qingli Hao,Bing Liu,Xihui Mu,Wu Lei,Zhaoyang Tong
The rapid spread of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) seriously threatened global public health. Establishing a rapid and sensitive diagnostic test for early detection of the SARS-CoV-2 nucleocapsid protein is urgently required to defend against the pandemic. Herein, an enhanced lateral flow immunoassay (LFIA) was fabricated by trimetallic Au@Pd@Pt core–shell nanozymes for detection of the SARS-CoV-2 nucleocapsid protein. The Au@Pd@Pt nanozymes (Au@Pd@Pt NZs) synthesized via a one-pot method, with a dendrite morphology and uniform particle size, showed excellent peroxidase-like activity. Due to the perfect enzyme-like catalytic activity toward 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H2O2), the catalytic signal could be generated even by a tiny amount of Au@Pd@Pt NZs accumulated on the test strip. Therefore, rapid detection with higher sensitivity was achieved. The Au@Pd@Pt NZs-based LFIA provided a quantitative range of 0.05–100 ng mL−1 with a limit of detection of 0.037 ng mL−1, which was 17-fold lower than the LFIA without enhancement. The average recoveries from spiked samples were in the range of 92.5–107.9% with relative standard deviations all less than 4%, indicating the reliability and repeatability of the proposed LFIA. Additionally, the proposed LFIA could report results within 30 min using a microplate reader. In conclusion, the Au@Pd@Pt NZs-LFIA is a rapid, simple, and sensitive method for detecting the SARS-CoV-2 nucleocapsid protein.
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高影响因子
Journal of Tissue Engineering and Regenerative Medicine
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2022
·Vol. 16
·期 12
·1223-1237
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IF 4.323
Zecheng Li,Shi Cheng,Ang Li,Chengchao Song,Anlong Jiang,Fangxing Xu,Hui Chi,Jinglong Yan,Guanghua Chen
The microenvironment in the healing process of large bone defects requires suitable conditions to promote osteogenesis and angiogenesis. Coaxial electrospinning is a mature method in bone tissue engineering (BTE) and allows functional modification. Appropriate modification methods can be used to improve the bioactivity of scaffolds for BTE. In this study, coaxial electrospinning with QK peptide (a Vascular endothelial growth factor mimetic peptide) and BMP-2 peptide–DFO (BD) was performed to produce double-modified PQBD scaffolds with vascularizing and osteogenic features. The morphology of coaxially electrospun scaffolds was verified by scanning electron microscopy (SEM) and transmission electron microscopy. Laser scanning confocal microscopy and Fourier transform infrared spectroscopy confirmed that BD covalently bound to the surface of the P and PQ scaffolds. In vitro, the PQBD scaffold promoted the adhesion and proliferation of bone marrow stromal cells (BMSCs). Both QK peptide and BD showed sustainable release and preservation of biological activity, enhancing the osteogenic differentiation of BMSCs and the migration of human umbilical vein endothelial cells and promoting angiogenesis. The combined ability of these factors to promote osteogenesis and angiogenesis is superior to that of each alone. In vivo, the PQBD scaffold was implanted into the bone defect, and after 8 weeks, the defect area was almost completely covered by new bone tissue. Histology showed more mature bone tissue and more blood vessels. PQBD scaffolds promote both angiogenesis and osteogenesis, offering a promising approach to enhance bone regeneration in the treatment of large bone defects.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Zuqin Duan,Qian Lei,Wenhui Wu,Honglin Chen
Hydrogen release from formic acid is a significant energy supply route. However, the current catalysts suffer from low catalytic efficiency and stability. Herein, a porous N-doped carbon material with high N content (16.87%) and a large surface area (1544 m 2 ·g −1 ) were designed using a 2-dimensional metal-organic framework and etching agent potassium chloride . Due to its high N content and large surface area, ultrafine Pd particles are uniformly distributed on the porous N-doped carbon support, which effectively enhances excellent reactivity and enables a TOF value of 2365 h −1 under additive-free conditions. The research also revealed that the strong interaction between Pd particles and pyridinic-N species can significantly slow metal agglomeration. Hence, the Pd/NC ZIF-L (KCl) displayed good activity even after 10 cycling experiments, and it is a particularly competitive catalyst for hydrogen release from formic acid.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Kai Zhang,Meina Yang,Helin Sun,Xueyin Wang,Hao Li,Jinxiang Han,Zhongwen Zhang
Using Peptide nucleic acid (PNA), this work provides a unique approach for controlling CRISPR/Cas13a activity by RNA Inhibitory PNA (RIP). This method reduces the action of CRISPR/Cas13a by inhibiting the binding of crRNA to CRISPR/Cas13a, which was subsequently utilized to detect metalloproteinase-2 (MMP-2) activity. We carefully constructed a PNA sequence that includes a peptide sequence (Gly-Pro-Leu-Gly-Val-Arg-Gly) that is particularly cleaved by MMP-2 in the middle. When MMP-2 is not present in the system, the PNA/crRNA complex reduces crRNA binding to CRISPR/Cas13a, hence inhibiting CRISPR/Cas13a cleavage activity. When MMP-2 is present in the system, it cleaves the peptide sequence (Gly-Pro-Leu-Gly-Val-Arg-Gly) selectively and so prevents PNA from binding to crRNA, enabling crRNA to reach the "free" form. Then, in the presence of an RNA activator, crRNA may bind to CRISPR/Cas13a and stimulate its activity. CRISPR/Cas13a triggered in this manner may precisely cleave the DNA sequence containing modified -UU- bases on the electrode surface . Thus, the ferrocene (Fc) is changed away from the electrode surface at one end of the DNA , enabling for the recovery of the Electrochemiluminescence (ECL) signal from the two-dimensional material transformed on the electrode surface. As a result, MMP-2 activity was detected utilizing this technique of inhibiting crRNA activity with a detection limit of 15.56 fM. Our suggested method of inhibiting CRISPR/Cas13a activity via PNA has a broad variety of potential therapeutic applications in gene editing and the development of CRISPR/Cas13a-based biosensors.
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ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Mingyu Li,Yuhan Ma,Jingjing Jiang,Tianren Li,Chongjun Zhang,Zhonghui Han,Shuangshi Dong
Heterogeneous photo-Fenton technology has drawn tremendous attention for removal of recalcitrant pollutants. Fe-based metal-organic frameworks (Fe-MOFs) are regarded to be superior candidates in wastewater treatment technology . However, the central metal sites of the MOFs are coordinated with the linkers, which reduces active site exposure and decelerates H 2 O 2 activation. In this study, a series of 2, 5-dioxido-1, 4-benzenedicarboxylate (H 2 DOBDC)-functionalized MIL-100(Fe) with enhanced degradation performance was successfully constructed via solvothermal strategy. The modified MIL-100(Fe) displayed an improvement in photo-Fenton behaviors. The photocatalytic rate constant of optimized MIL-100(Fe)-1/2/3 are 2.3, 3.6 and 4.4 times higher compared with the original MIL-100(Fe). The introduced H 2 DOBDC accelerates the separation and transfer in photo-induced charges and promotes Fe(II)/Fe(III) cycle, thus improving the performance. •OH and •O 2 − are main reactive radicals in tetracycline (TCH) degradation. Dealkylation, hydroxylation, dehydration and dealdehyding are the main pathways for TCH degradation.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
·
IF 6.633
Wang Jun,Zhu Tianlong,Deng Ziwen,Liu Haicheng,Huang Chunxiang,Li Na,Sun Xueni,Shao Hui,Qi Lv
Isobaric vapour-liquid equilibrium (VLE) data for binary systems containing methyl chloroacetate (MC) + methyl 2-chloropropionate (M2C), MC + methyl dichloroacetate (MDC), and M2C + MDC at 101.33 kPa and the saturated vapour pressure data of these components were measured by using a modified Othmer still. The VLE data showed that these binary systems were all slightly positive deviation solutions compared with the ideal system. Herington area and point tests were used to confirm the thermodynamic consistency for these binary systems, and the results showed good thermodynamic consistency. The interaction energy ( E inter ) between these components was calculated by molecular simulation to explain the normal boiling point and VLE behavior. The simulation results showed weak hydrogen bonds between these chlorinated esters. In addition, the binary VLE experimental data were correlated by the Wilson, NRTL, and UNIQAC models. The correlated results agreed well with the experimental values.
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2022
·
IF 6.633
Yameng Wan,Haixia He,Pengshuai Zhang,Fanfan Li,Xiaoqiang Gao,Yanxun Li
Solubility behavior as a significant molecular property should be known in the field of crystal form screening, dosage form along with separation and purification in the pharmaceutical industry. In this research work, solubility data of 2-chloronicotinamide (2-CNA) in ten pure solvents including methanol (MeOH), ethanol (EtOH), ethylene glycol (EG), 2-methoxyethanol (EGME), 2-ethoxyethanol (EGEE), methyl acetate (MeAc), water, 1,4-dioxane (Diox), N,N-dimethylformamide (DMF) and N,N-dimethylacetamide (DMAC) within the range of 278.15/288.15 K to 323.15 K was experimentally determined by laser monitoring method at 0.1 MPa. Solubility of 2-CNA presented a positive correlation with temperature, and increased with incremental temperature. The result was indicative of a common tendency: DMAC > DMF > EGME > EGEE > EG > MeOH > Diox > EtOH > MeAc > water. The solvation free energy, molecular electrostatic potential surface (MEPS) and Hirshfeld surface were used to study the intermolecular interactions. Moreover, six mathematical models namely “Margules, UNIQUAC, NRTL, Wilson, NRTL-SAC and Jouyban model” were utilized to correlate solubility data of 2-CNA in mono-solvents. UNIQUAC model could provide maximum regression accuracy in correlation with solubility data among six models in terms of average relative deviation (ARD) and root mean square deviation (RMSD). Finally, thermodynamic parameters obtained from UNIQUAC equation indicated that all dissolution and mixing process were always entropy-increasing, endothermic and spontaneous.
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高影响因子
INORGANICA CHIMICA ACTA
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2022
·
IF 3.118
Yuwei Dong,Jialin Ma,Zhou Yu,Xinxin Liu,Zhen Zhao
Herein, we report a reversible and easy assembled fluorometric probe (4-(quinolin-2-ylmethylene)aminoanisole, QMAA ) for the highly selective and sensitive detection of cadmium ion (Cd 2+ ) in DMF solution with PBS buffer (0.01 M, pH = 7.30). The strong fluorescence response of QMAA to Cd 2+ along with a bright blue fluorescence was mainly ascribed to the formation of the complex QMAA–CdCl 2 . The results show that the complexation can inhibit the C N isomerisation and photo–induced electron transfer (PET), and further lead to the occurrence of chelation fluorescence enhancement. The 1:1 stoichiometry of the complex between QMAA and cadmium ion was studied by fluorescence titration, Job’s plot analysis, 1 H NMR, FT–IR, and ESI–MS data, and was further confirmed by the single crystal structure of the complex QMAA–CdCl 2 . Density functional theory (DFT) calculations have verified the mechanism of fluorescence enhancement. In addition, the limit of detection of QMAA for Cd 2+ was as low as 0.1547 µM (at 10 –7 M level), which was lower than the acceptable limit of Cd 2+ level in drinking water defined by World Health Organization. The analog experiments about nature contamination of Cd 2+ in real samples were finished.
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Food Biophysics
·
2022
·Vol. 17
·期 4
·495-507
·
IF 3.34
Ghide Michael Kidane,Li Kai,Wang Jianhua,Abdulmalek Saadiah A.,Yan Yunjun
1,3-Dioleoyl-2-palmitoyl glycerol (OPO)-supplemented infant formulas mimic the nutritional properties of human milk, and thus are the best nutritional alternatives to breast feeding. Herein, structured triacyl glycerides rich in sn-1,3 oleic acid (OA) and sn-2 palmitic acid (PA) are synthesized via a new strategy by employing Rhizomucor miehei lipase (RML) adsorbed on magnetized multiwalled carbon nanotubes (mMWCNT) and synthesizing OPO-rich fats in a two-step enzymatic acidolysis. The results showed that the immobilized lipase (mMWCNT-COOH-RML) exhibited improved pH and thermal stability, and it could be separated conveniently from the reaction system via an external magnetic field. It also possessed a much better performance in catalysis of tripalmitin (PPP) with OA to synthesize OPO-rich fats in a two-step enzymatic acidolysis. Under optimized conditions, the content of palmitic acid at the sn-2 position and incorporation of OA at the sn-1,3 positions respectively reached 92.93% and 57.82%. mMWCNT-COOH-RML also exhibited better reusability and catalytic activity than the conventionally used commercial Lipozyme RM IM. The results indicate the employed new strategy for synthesis of OPO-rich fats has a prosperous potential in the application of infant formula formulations.
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