CATALYSIS TODAY
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2022
·
IF 6.562
Yiming Ma,Yushuai Sang,Kai Wu,Qingfeng Liu,Hong Chen,Yongdan Li
Low selectivity and complex product distribution are the main challenges for the utilization of lignin. Herein, the selective production of 2-(tert-butyl)-3-methylphenol (TBC), an antioxidant in the polymer industry, from depolymerization of enzymatic hydrolysis lignin (EHL) on a hydrothermally synthesized MoS 2 catalyst is studied. The total aromatic monomer yield is 124.1 mg/g EHL and the selectivity of TBC is up to 40.3 wt% in methanol at 280 °C under 2 MPa H 2 for 6 h. The FT-IR analysis of products reveals that MoS 2 has a high activity for demethylation, dehydroxylation and alkylation, and the dimer conversions reveal that C-O and C-C bonds in EHL are broken with MoS 2 . The guaiacol and its derivants are identified as the intermediate for formation of TBC in EHL depolymerization according to the effect of time on product distribution and monomer conversion.
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Biomass Conversion and Biorefinery
·
2022
·Vol. 13
·期 18
·16887-16898
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IF 4.05
Wang Fei,Lai Jinhua,Liu Zixuan,Wen Sha,Liu Xianxiang
Spinel copper–manganese oxide catalysts were prepared via the co-precipitation method to be used for the catalytic selective oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA). Morphological characterization revealed that the primary particles of the as-synthesized catalysts were irregular nanoparticles aggregated with each other. The effects of reaction conditions such as time, temperature, and the dosage of oxidant on the catalytic activity were investigated. The experimental results show that the CuMn 2 O 4 showed superior catalytic performance in HMF selective oxidation reaction. In the presence of acetonitrile and tert-butyl hydroperoxide as oxidant, the catalytic reaction can achieve complete conversion of HMF, and the FDCA selectivity reached to 96.4%. The catalyst exhibited good recyclability and recoverability in a three-run recycling test. Mechanism studies reveal that Mn 3+ has a significant influence on the catalytic oxidation and the synergistic interaction between Mn and Cu can facilitate the mobility of oxygen thus improving the catalytic activity. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yingshan Zeng,Qiao Yin,Zhi Liu,Hao Dong
The rational utilization of graphitic carbon nitride (g-C 3 N 4 ) and quantum dots (QDs) semiconductors to highlight their merits as efficient photocatalysts remains attractive and challenging. Targeted integration of g-C 3 N 4 and QDs with expanded interfacial contact and multi-channel electron transfer is an effective means to boost the transfer efficiency of photogenerated electrons and achieve prominent photocatalytic activity. In this article, novel attapulgite (ATP)-interpenetrated Bi 2 WO 6 QDs/g-C 3 N 4 nanocomposites (BWQ/g-C 3 N 4 /ATP, designated as BCAs) are successfully fabricated through a simple and effective in situ hydrothermal growth method. The nanorod-structured ATP acts as numerous bridges to intercalate into the interlayers and expands inner space of g-C 3 N 4 . Theoretical calculation results indicate that an interfacial internal electric field (IEF) is formed where electrons transfer from g-C 3 N 4 to Bi 2 WO 6 . Originating from the intact interfacial contact of the expanded g-C 3 N 4 and highly dispersed BWQ with reinforcing electronic transferability of ATP, the optimal sample of BCA5 with higher specific surface area, more active sites and electron transfer channels, and stronger light harvestability, exhibits a nearly-100% degradation of organic contaminant of 2-Mercaptobenzothiazole in water, 35-, 17- and 3-fold rate constant higher than that the pristine g-C 3 N 4 , BWQ and Bi 2 WO 6 /g-C 3 N 4 counterparts, respectively. Various characterization techniques are employed to put forward the mechanisms in depth on MBT degradation route and IEF-induced photocatalytic Z-scheme over the BCA5 under photoexcitation.
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Congcong Ji,Hongyu Wang,Shiqin Sun,Qi Li,Ji-Jun Zou,Shitao Yu,Huibing Shi,Genkuo Nie,Shiwei Liu
2-Ethylanthraquinone is frequently used for producing bulk consuming chemicals. However, the synthesis of 2-ethylanthraquinone is still restricted by expensive raw materials, complex preparation process and poor-cycling catalyst. Herein, a one-pot method is developed to synthesize 2-ethylanthraquinone using phthalic anhydride and ethylbenzene as feedstock by combination of acylation and dehydration over a Sc-modified Hβ catalyst. Sc-modified Hβ was prepared via impregnation and catalyzed conversion of phthalic anhydride about 58.8% and 2-ethylanthraquinone selectivity up to 78.5% which is better than the results by other metals-modified Hβ zeolites. By adjusting Sc loading amount in Hβ, more acids are created especially strong Lewis acid and an appropriate synergistic effect of Lewis/Bronsted acids is obtained for cascade reactions of acylation and dehydration. Then, the reaction conditions were investigated and the catalyst can be reused in 4 runs. This work provides a green and simple way for 2-ethylanthraquinone synthesis.
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ChemElectroChem
·
2022
·Vol. 9
·期 2
·e202101523
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IF 4.782
Junye Zhang,Hao Guo,Fan Yang,Mingyue Wang,Tingting Zhang,Hao Zhang,Wu Yang
Graphical Ni-MOF derived CMs@Ni(OH) 2 /NiSe with a core-shell structure was designed. The obtained core-shell nanostructure material possesses a high contact area, excellent synergistic effect and can provide more reactive active sites. The application of Ni-MOF in supercapacitors has received widespread attention, but its poor conductivity and bad stability hinder its application. Therefore, Ni-MOF derived CMs@Ni(OH) 2 /NiSe with a core-shell structure was designed. Here, carbon microspheres (CMs) were explored as the conductive substrate to enhance the stability and in situ prepared Ni-MOF was anchored on the surface of CMs. Then, alkali-treatment and selenylation were carried out on CMs@Ni−MOF to improve stability and conductivity. The obtained core-shell nanostructure material possesses a high contact area, excellent synergistic effect and can provide more reactive active sites. The prepared CMs@Ni(OH) 2 /NiSe shows a higher specific capacitance (2106 F g −1 ) and excellent cycling performance with a capacitance retention of 95 % after 30000 cycles. Furthermore, the assembled CMs@Ni(OH) 2 /NiSe//AC device delivers a high energy density of 70.84 Wh kg −1 at the power density of 756.8 W kg −1 and maintains 100 % of the initial capacitance after 40000 cycles.
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INORGANIC CHEMISTRY
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2022
·
IF 5.436
Lixiong Qian,Lei Yao,Yunpeng Liu,Hao Wang,Jiajun Zhong,Chao Liu,Guang Mo,Xueqing Xing,Zhongjun Chen,Zhonghua Wu
The formation mechanism of nanoparticles is of great significance for the controllable synthesis, structural design, and performance optimization of nanomaterials. In this paper, an economical hydrothermal method was used to synthesize zinc oxide (ZnO) nanorods. X-ray diffraction, X-ray absorption fine structure, and small-angle X-ray scattering techniques were used to probe the structural changes. Scanning electron microscopy and high-resolution transmission electron microscopy were used to observe the morphologies of the products. A self-designed in situ temperature–pressure sample cell was used to control the hydrothermal conditions. The results demonstrate that an unknown intermediate phase, Zn(HCO3)2·H2O, was first formed at 50 °C, having a morphology of nanoflakes with a average thickness of about 35 nm. The intermediate phase Zn(HCO3)2·H2O was determined to have a monoclinic structure with space group P1211 and the following lattice parameters: a = 11.567 Å, b = 3.410 Å, c = 5.358 Å, β = 96.0011°, and Z = 2. After a hydrothermal temperature of 140 °C, CO2 and H2O were evaporated from the Zn(HCO3)2·H2O intermediate product and the ZnO nanorods with a wurtzite structure were formed. The final ZnO nanorods have an average diameter of about 45 nm and an average length of about 2 μm. The axial direction of the ZnO nanorods is the [001] crystallographic direction. By virtue of understanding the formation mechanism, this work is helpful for the controllable synthesis of ZnO nanoparticles.
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ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Haochen Qi,Zhiwen Hu,Zhongliang Yang,Jian Zhang,Jie Jayne Wu,Cheng Cheng,Chunchang Wang,Lei Zheng
The pandemic caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) has lasted for almost 2 years. Stemming its spread has posed severe challenges for clinical virus detection. A long turnaround time, complicated operation, and low accuracy have become bottlenecks in developing detection techniques. Adopting a direct antigen detection strategy, we developed a fast-responding and quantitative capacitive aptasensor for ultratrace nucleocapsid protein detection based on a low-cost microelectrode array (MEA) chip. Employing the solid–liquid interface capacitance with a sensitivity of picofarad level, the tiny change on the MEA surface can be definitively detected. As a result, the limit of detection reaches an ultralow level of femtogram per milliliter in different matrices. Integrated with efficient microfluidic enrichment, the response time of this sensor from the sample to the result is shortened to 15 s, completely meeting the real-time detection demand. Moreover, the wide linear range of the sensor is from 10–5 to 10–2 ng/mL, and a high selectivity of 6369:1 is achieved. After application and evaluation in different environmental and body fluid matrices, this sensor and the detection method have proved to be a label-free, real-time, easy-to-operate, and specific strategy for SARS-CoV-2 screening and diagnosis.
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高影响因子
Biosensors-Basel
·
2021
·Vol. 12
·期 1
·13
·
IF 5.519
Tao Peng,Xueshima Jiao,Zhanwei Liang,Hongwei Zhao,Yang Zhao,Jie Xie,You Jiang,Xiaoping Yu,Xiang Fang,Xinhua Dai
The coronavirus disease 2019 (COVID-19) pandemic caused by severe acute respiratory coronavirus 2 (SARS-CoV-2) is still raging all over the world. Hence, the rapid and sensitive screening of the suspected population is in high demand. The nucleocapsid protein (NP) of SARS-CoV-2 has been selected as an ideal marker for viral antigen detection. This study describes a lateral flow immunoassay (LFIA) based on colloidal gold nanoparticles for rapid NP antigen detection, in which sensitivity was improved through copper deposition-induced signal amplification. The detection sensitivity of the developed LFIA for NP antigen detection (using certified reference materials) under the optimized parameters was 0.01 μg/mL and was promoted by three orders of magnitude to 10 pg/mL after copper deposition signal amplification. The LFIA coupled with the copper enhancement technique has many merits such as low cost, high efficiency, and high sensitivity. It provides an effective approach to the rapid screening, diagnosis, and monitoring of the suspected population in the COVID-19 outbreak.Keywords:SARS-CoV-2;nucleocapsid protein;signal amplification;copper deposition
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Shuai Li,Ruilin Tang,Chuan Hu,Xiaobin Niu,Liping Wang
As a promising cathode material for high-performance lithium-ion batteries, olivine LiFe 1-x Mn x PO 4 (0 < x < 1, LFMP) combines the high safety of LiFePO 4 and the high energy density of LiMnPO 4 . During the charge-discharge process, poor interface stability of active materials leads to capacity decay, which prevents its commercial application. Here, to stabilize the interface, a new electrolyte additive potassium 2-thienyl tri-fluoroborate (2-TFBP) is developed to boost the performance of LiFe 0.3 Mn 0.7 PO 4 at 4.5 V vs. Li/Li + . Specifically, after 200 cycles, the capacity retention remains at 83.78% in the electrolyte containing 0.2% 2-TFBP while the capacity retention without 2-TFBP addition is only 53.94%. Based on the comprehensive measurements results, the improved cyclic performance is attributed to that 2-TFBP has a higher highest occupied molecular orbit (HOMO) energy and its thiophene group can be electropolymerized above 4.4 V vs. Li/Li + for generating uniform cathode electrolyte interphase (CEI) with poly-thiophene, which can stable materials structure and suppress the decomposition of electrolytes. Meanwhile, 2-TFBP both promotes the deposition/exfoliation of Li + at anode-electrolyte interfaces and regulates Li deposition by K + cations through the electrostatic mechanism. This work presents that 2-TFBP has a great application prospect as a functional additive for high-voltage and high-energy-density lithium metal batteries .
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CHEMOSPHERE
·
2023
·
IF 8.8
Xuan Zhang,Keke Geng,Ningning Wu,Gang Hu,Ben Fan,Jian He,Wenjing Qiao
4-Chloro-2-methylphenoxyacetic acid (MCPA) is a widely used herbicide across the world. MCPA is persistent and easily transports into anoxic environment, such as groundwater, sediments and deep soils. However, little research on anaerobic microbial degradation of MCPA was carried out. The functional microorganisms as well as the catabolic pathway are still unknown. In this research, an anaerobic MCPA-degrading bacterial consortium was enriched from the river sediment near a pesticide-manufacturing plant. After about 6 months’ acclimation , the MCPA transformation rate of the consortium reached 4.32 μmol g −1 day −1 , 25 times faster than that of the original sludge . 96% of added MCPA (2.5 mM) was degraded within 9 d of incubation. Three metabolites including 4-chloro-2-methylphenol (MCP), 2-methylphenol (2-MP) and phenol were identified during the anaerobic degradation of MCPA. An anaerobic catabolic pathway was firstly proposed: firstly, MCPA was transformed to MCP via the cleavage of the aryl ether, then MCP was reductively dechlorinated to 2-MP which was further demethylated to phenol. The 16S rRNA gene amplicon sequencing revealed a substantial shift in the bacterial community composition after the acclimation. SBR1031, Acidaminococcaceae , Aminicenantales , Syntrophorhabdus , Acidaminobacter , Bacteroidetes_vadinHA17 , Methanosaeta , Bathyarchaeia , KD4-96, Anaeromyxobacter , and Dehalobacter were significantly increased in the enriched consortium after acclimation, and positively correlated with the anaerobic degradation of MCPA as suggested by heat map correlation analysis. This study provides a basis for further elucidation of the anaerobic catabolism of MCPA, and contributes to developing efficient and low-cost anaerobic treatment technologies for MCPA pollution.
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DALTON TRANSACTIONS
·
2023
·
IF 4
Yuanlei Huang,Mengdi Lv,Binglian Guo,Guojing Hu,Yong Qian,Zhi Su,Xuling Xue,Hong-Ke Liu
Breast cancer (BC) is one of the most common malignant tumors and often accompanied by inflammatory processes. Inflammation is an essential component of the tumor microenvironment, which might influence tumor proliferation and metastasis. Herein, three metal–arene complexes MA-bip-Ru, MA-bpy-Ir, and MA-bpy-Ru were prepared by tethering the non-steroidal anti-inflammatory drug meclofenamic acid (MA). Among them, MA-bip-Ru and MA-bpy-Ir showed lower cytotoxicity towards cancer cells, but MA-bpy-Ru showed significantly high selectivity and cytotoxicity towards MCF-7 cells through the autophagic pathway and exhibited no toxicity against normal HLF cells, showing potential for selective treatment of tumor cells. MA-bpy-Ru could also effectively destroy the 3D multicellular tumor spheroids, demonstrating its potential for clinical application. Besides, MA-bip-Ru, MA-bpy-Ir, and MA-bpy-Ru exhibited anti-inflammatory properties superior to MA, notably downregulating the expression of cyclooxygenase-2 (COX-2) and inhibiting the secretion of prostaglandin E2 in vitro. These findings demonstrated that MA-bpy-Ru was capable of intervening in inflammatory processes and showed the potential of MA-bpy-Ru to act as a selective anticancer agent, thus presenting a new mechanism of action for metal–arene complexes.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
He Liu,Jiahao Liang,Xiaodong Du,Rui Wang,Ting Tang,Xueqin Tao,Hua Yin,Zhi Dang,Guining Lu
Organophosphorus esters (OPEs), one kind of the emerging contaminants with high frequency of detection, is rather refractory in natural environment, thus posing great threat to human health. This study investigated the feasibility and mechanism of tris(2-chloroethyl) phosphate (TCEP) degradation in thermally activated persulfate (TAP) system. Influence of impact factors, such as PDS dosage, temperature, initial pH, and presence of natural water matrix (Cl − , NO 3 − , H 2 PO 4 − , NH 4 + , humic acid), were evaluated. Results showed that 100% degradation of TCEP can be achieved in TAP system in 40 min at 60 °C. SO 4 ·− as the dominant oxidant for TCEP degradation was proved by quenching experiment and verified by EPR analysis. Alkaline condition exerted great inhibitory effect by affecting the constituents of oxidative radicals. It is suggested that Cl − and H 2 PO 4 − at lower dosages promoted the degradation by stimulating ·OH production and forming oxidative radicals with better selectivity . Intermediates identified by high resolution mass spectrometer was suggested less toxic than TCEP by ECOSAR program. Meanwhile, the illustrated oxidation mechanism mainly involved radical attack at C Cl bond and cleavage of C O bond, as further confirmed by frontier electron density calculation and wavefunction analysis. Moreover, cyclic degradation of TCEP indicated the constant release of SO 4 ·− in 450 min, suggesting high efficiency and stability of PDS in TAP system. Four selected OPEs achieved complete removal in TAP system and their degradation discrepancy was further discussed based on the distinctive structures. Altogether, TAP technology can be used as an efficient method in TCEP removal with great potential for application.
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