TALANTA
·
2022
·
IF 6.556
Chuiyu Zhu,Xiao Tian,Qiuyan Li,Zichang Dai,Lina Wang,Huamin Liu,Chenghong Li,Kashif Rafiq Zahid,Chunmei Wu,Hui Huang,Lichao Fang,Qiyuan Huang,Feixue Liu,Jun Deng,Yan Li,Tao Zeng,Junsong Zheng
Altered DNA methylation in the form of 5-methylcytosine (5-mC) patterns is correlated with disease diagnosis, prognosis, and treatment response. Therefore, accurate analysis of 5-mC is of great significance for the diagnosis of diseases. Here, an efficient enhanced photoelectrochemical (PEC) biosensor was designed for the quantitative analysis of DNA 5-mC based on a cascaded energy level aligned co-sensitization strategy coupling with the bridged DNA nanoprobe (BDN). Firstly, Au nanoparticle/graphite phase carbon nitride/titanium dioxide (AuNPs/g-C 3 N 4 @TiO 2 ) nanocomposite was synthesized through in situ growth of AuNPs on g-C 3 N 4 @TiO 2 surface as a matrix to provide a stable background signal. Next, BDN with a high mass transfer rate synthesized from a pair of DNA tetrahedral as nanomechanical handles was used as a capture probe to bind to the target sequence. The polydopamine nanosphere was applied to load with CdTe QDs (PDANS-CdTe QDs) as a photocurrent label of 5-mC antibodies. When the 5-mC existed, a large number of PDANS-Ab-CdTe QDs were introduced to the electrode surface, the formed CdTe QDs/AuNPs/g-C 3 N 4 @TiO 2 co-sensitive structure could effectively enhance the electron transfer capability and photocurrent response rate due to the effective cascade energy level arrangement, leading to a significantly enhanced photocurrent signal. The proposed PEC biosensor manifested a wide range from 10 −17 M to 10 −7 M and a detection limit of 2.2 aM. Meanwhile, the excellent performance indicated the practicability of the designed strategy, thus being capable of the clinical diagnosis of 5-mC.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yixuan Feng,Haixin Guo,Richard L. Smith,Xinhua Qi
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) was examined as an alternative to thermocatalytic methods in which two-dimensional (2D) cobalt-metal–organic framework (Co-MOF, ZIF-L-Co) nanoplate arrays were prepared on nickel foam (NF) and then transformed into hierarchical porous Co 3 O 4 nanostructures by chemical etching and low temperature annealing to form electrode materials . Hierarchical porous nanoarrays formed during synthesis enlarged the surface area of the as-prepared catalysts introduced a large number of defects and exposed active sites leading to reduced charge diffusion , improved mass transfer and efficient HMF oxidation . Co 3 O 4 /NF electrode materials were able to achieve a current density of 10 mA·cm −2 at an overpotential of 105 mV in 1 M KOH with 10 mM HMF, which was reduced by 175 mV compared with water oxidation. Electrocatalytic oxidation experiments afforded 100 % HMF conversion and 96.7 % FDCA yields with a minimum 96.5 % faradaic efficiency at 1.43 V vs RHE. The proposed MOF-structured synthesis method fundamentally reduces charge diffusion , improves mass transfer of electrodes and is generally applicable to fabrication of hierarchical porous nanostructured materials.
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高影响因子
ENVIRONMENTAL RESEARCH
·
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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高影响因子
ACS Omega
·
2022
·
IF 4.132
Huan Song,Bing Li,Xuezhi Gao,Fenglin Shan,Xiaoxia Ma,Xiaoyan Tian,Xiaoyan Chen
For energetic materials (EMs), the key point of the present research is to improve the energetic property and reduce sensitivity. In this work, two new energetic complexes, Mn(atzc)2(H2O)2·2H2O (1) and Zn(atzc)2(H2O) (2) (Hatzc = 3-amino-1,2,4-triazole-5-carboxylic acid), were synthesized by solvent evaporation and diffusion methods, respectively. The structural analyses illustrate that 1 and 2 exhibit zero-dimensional structural units, which are linked by hydrogen-bonding interactions to give three-dimensional supramolecular architectures. For complexes 1 and 2, the detonation velocities (D) are 10.4 and 10.2 km·s–1 and detonation pressures (P) are 48.7 and 48.6 GPa, respectively. They are higher than most of the reported EMs, which present prominent detonation characteristics. In addition, two complexes can accelerate the thermal decomposition of ammonium perchlorate and exhibit excellent catalytic activity. Therefore, the two complexes can serve as a new class of promising EMs, which have potential application in the design of new high-efficiency solid catalysts.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Kongyan Yang,Feng Zhou,Huixia Ma,Chuntao Liu,Fangwei Ma,Guang Wu
A series of nanocrystalline ZSM-5 zeolites with abundant intercrystalline mesopores was fabricated by a hydrothermal crystallization method without any mesopore template. The ZSM-5 zeolite was characterized by XRD , XRF , N 2 adsorption, NMR, SEM, TEM and NH 3 -TPD and used for the catalytic fast pyrolysis (CFP) of cellulose . The external surface area of the nanocrystalline ZSM-5 zeolite reached 146.6 m 2 /g, larger than the external surface area of conventional ZSM-5 (57.9 m 2 /g). The product yields of the CFP reaction were studied over different Si/Al ratios of nanocrystalline ZSM-5, and the aromatic yield of nanocrystalline ZSM-5 was generally higher than the aromatic yield of conventional ZSM-5. The relationship between the surface area, acid amounts and product yields was established by drawing a linear fitting curve. The results show that both pore structure and acidity have important effects on aromatic yield and coke yield. Aromatics are generated in micropores, and the increase in external surface area caused by reducing the particle size improves the pyrolysis of cellulose to generate bio-oil vapours, which further diffuse into micropores to generate aromatics.
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 97
·期 7
·1900-1908
·
IF 3.709
Yanjie Wu,Huiping Zhang,Ying Yan
BACKGROUND Cu-ZSM-5 was prepared on paper-like sintered stainless steel fibers (PSSF) by ion-exchange method for the catalytic wet peroxide oxidation (CWPO) of phenol in a fixed bed reactor. The prepared Cu-ZSM-5/PSSF catalyst was characterized by scanning electron microscope (SEM), Brunner−Emmet−Teller (BET), X-ray diffraction (XRD), Fourier Transform InfraRed (FT-IR), Ultraviolet–visiblespectroscopy (UV–vis) and X-ray photoelectron spectroscopy (XPS). RESULTS The XRD results showed that the ZSM-5 membrane was loaded well over PSSF with good crystallinity, even after the process of ion-exchange. The UV–vis inferred that isolated copper was the predominant species over ZSM-5 pores of the catalyst. Then, the effects of different catalyst bed heights, reaction temperatures, and feed flow rates on catalytic performance were investigated to obtain optimum reaction conditions. CONCLUSIONS Finally, the catalytic reaction kinetics analysis over Cu-ZSM-5/PSSF catalyst were carried out with the Power-rate Law Kinetic model. The experimental results showed that the reaction order was the first-order reaction, and the activation energy of the oxidation reaction was Ea = 72.9 kJ/mol. The initial oxidation rate equation (−r A0 = 5.36 × 10 8 e −72 994/RT C A ) was obtained for phenol degradation using Cu-ZSM-5/PSSF catalyst. © 2022 Society of Chemical Industry (SCI).
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高影响因子
FUEL
·
2022
·
IF 8.035
Linjie Guan,Chengming Huang,Dingmei Han,Binbin He,Linhua Zhu,Dedong He,Yi Mei,Yun Zu
A series of HZSM-5 zeolites are fabricated to make it cross-link with an external ultrathin siliceous layer by chemical liquid deposition and the corresponding thickness is measured by TEM and XPS analysis. In situ FTIR experiments disclose that the external surface acidic sites of HZSM-5 zeolite can be covered even by siliceous monolayer (0.7 ∼ 1.3 nm, HZ5-S1). In comparison to parent HZSM-5, the catalytic cracking performance of n-butane over the modified zeolites are evidently enhanced. In particular, the n-butane conversion rate per Brønsted acid site over the HZ5-S2 (16.02 min −1 ) at 550 °C is 2.82 times than that over the HZSM-5 (5.68 min −1 ). Meanwhile, the diffusion properties of n-butane over the zeolites are quantified by in situ FTIR spectroscopic analysis. Negative correlation between steady-state diffusivity and n-butane conversion rate per Brønsted acid site can be found, which unravels the origin of the progressive decrease in the catalytic stability. Under comparable conditions, more advantages can be greatly achieved by HZ5-S1 catalyst in the catalytic activity and the yields to light olefins due to the benign diffusivity and the elimination of external surface acidic sites. This study can provide a guidance for the understanding of diffusion intensification and the rational design of superior catalyst for the catalytic cracking reactions of alkanes.
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
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2022
·Vol. 48
·期 3
·983-1001
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IF 3.134
Zhang Dawei,Ren Lu,Liu Ailing,Zhang Yumin,Lv Yang,Gu Qiang
Abstract An efficient synthesis of 1,3,5-trisubstituted-1 H -pyrazoles was developed via cyclocondensation in 78–92% yields starting from α , β -unsaturated aldehydes/ketones with substituted phenylhydrazine using vitamin B 1 as a catalyst, and was characterized by HR-MS, FT-IR, 1 H NMR and 13 C NMR spectroscopy. The reaction has simple operation, metal-free catalysis, acid or base free catalysis. As a green catalyst, vitamin B 1 was found to possess favorable catalytic activity and reusability for the condensation reaction. 1,3,5-trisubstituted-1 H -pyrazole shows from orange-red to cyan in different solvents when the electron withdrawing group is attached to acetophenone (taking compound 5i as an example). Compound 5i as a metal ion fluorescent probe has excellent selectivity for Ag + detection. The crystal structure of the compound 3-(4-chlorophenyl)-1,5-diphenyl-4,5-dihydro-1 H -pyrazole ( 5b ) in the orthorhombic space group Pca 21 was presented and formed racemic crystals. Graphical abstract
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Qian Zhu,Yan Zhuang,Hongqing Zhao,Peng Zhan,Cong Ren,Changsheng Su,Wenqiang Ren,Jiawen Zhang,Di Cai,Peiyong Qin
The selective oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) is an important reaction for renewable biomass building blocks. Compared with thermal catalytic processes, photocatalytic production of DFF from HMF has attracted tremendous attention. Herein, the MoS 2 /CdIn 2 S 4 (MC) flower-like heterojunctions were prepared and considered as photocatalysts for selective oxidation of HMF into DFF under visible-light irradiation in aqueous solution. Results demonstrated MoS 2 in MC heterojunction could promote the separation of photoexcited electron-hole pairs, while the amount of MoS 2 dropping was proved influenced on the photocatalytic performance. 80.93% of DFF selectivity was realized when using 12.5% MC as photocatalyst. In addition, the MC catalyst also showed great potential in transformation of other biomass derived benzyl- and furyl-alcohols. The catalytic mechanism suggested that · O 2 - was the decisive active radical for HMF oxidation. Therefore, the MC heterojunction could be applied in photocatalytic conversion of biomass to valuable chemicals under ambient condition.
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高影响因子
Applied Sciences-Basel
·
2022
·Vol. 12
·期 8
·3769
·
IF 2.838
Wei Ma,Dong Ye,Haining Wang
Herein, a series of Co-Fe mixed oxide modified ZSM-5 adsorbents were synthesized using the ultrasonic-assisted impregnation method for the capture of elemental mercury. In comparison with other samples, Co4Fe1-ZSM-5 produced a relatively better performance, with the removal efficiency of around 96.6% Hg0and the adsorption capacity of around 901.63 ug/mg Hg0achieved at 120 °C. The interaction between CoOxand FeOximproved the reducibility of oxygen species, thus promoting the oxidation of Hg0. Among a variety of other gas components, O2and NO exerted a positive effect on Hg0, which improved its removal to a certain extent. By contrast, SO2caused an adverse effect on the capture of Hg0, which could be reversed to some degree by the introduction of 5% O2. After five cycles, the mercury removal efficiency of Co4Fe1-ZSM-5 remained above 90%, suggesting excellent recyclability. Finally, XPS analysis was conducted to reveal that Mars–Maessen mechanisms are dominant in the process of mercury adsorption.Keywords:Hg0adsorption;ZSM-5;cobalt oxide;iron oxide;regeneration
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 97
·期 7
·1822-1832
·
IF 3.709
Yongwei Ma,Xiangxiang Zhao,Hui Shao,Jianfeng Yao
BACKGROUND Fluoride ions can form corresponding complexes with transition metal elements (Co, Ti, V, Cr, Mn, Fe, Ni, Cu, etc.), so it is easier to synthesize heteroatomic molecular sieves in a fluorine-containing system than in a fluorine-free system. RESULTS In this paper, a hierarchical CoAPO-5 molecular sieve was synthesized in a fluorine system, and the effects of different fluorine resources on its synthesis were investigated. The CoAPO-5 samples were characterized by X-ray diffraction, scanning electron microscopy, N 2 adsorption–desorption and temperature-programmed desorption of NH 3 . CONCLUSION The results showed that, compared with other fluorine resources, the sample D-AFI-1 synthesized with HF possessed more acid sites, which appeared to be more attractive for oxidative desulfurization. The central composite design of response surface methodology was applied to design experimental schemes employing D-AFI-1 as catalyst. The volume ratio of oxidant/fuel, extractant/fuel and the mass ratio catalyst/fuel were screened out as the significant factors after the investigation of single factors. The quadratic model of the three significant factors and desulfurization rate was established. On the basis of optimizing the reaction conditions, oxidant/fuel volumetric ratio, catalyst/fuel mass ratio and extractant/fuel were 0.07 mL mL −1 , 0.01 g g −1 and 1.65 mL mL −1 , respectively, the desulfurization rate was 85.0%, which was consistent with the predicted value of the model (83.7%). © 2022 Society of Chemical Industry (SCI).
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
He Han,Anfeng Zhang,Limin Ren,Xiaowa Nie,Min Liu,Yi Liu,Chuan Shi,Hong Yang,Chunshan Song,Xinwen Guo
Shape-selective alkylation of toluene with methanol is one of the most attractive promising synthetic routes to para -xylene. To date, modified ZSM-5 zeolites are considered to be one of the best candidate catalysts for this reaction. Although the para -selectivity could be tuned to approaching 100% by modification of the zeolite and optimization of reaction conditions, at present, there is still a lack of effective means to inhibit the rapid deactivation of the catalysts due to coke formation. In this work, a coke-resistant (Pt + Ni)/ZSM-5 zeolite with excellent stability for shape-selective alkylation of toluene with methanol to para -xylene is developed. The pore structure and acid properties of the zeolite are effectively tuned to ensure high para -selectivity. Meanwhile, the co-existence of Pt and Ni species in this catalyst plays the critical role in inhibiting coke formation, as the two species concurrently impede the formation of olefins, the main coking precursors, via two distinctive mechanisms.
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