JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Lu Qi,Peng Zheng,Zhen Zhao,Aijun Duan,Chunming Xu,Xilong Wang
The intrinsic kinetics of hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene (4,6-DMDBT) over mesoporous CoMoS 2 /ZSM-5 (CoMoS 2 /MZSM-5) was investigated by comparing the commercial CoMoS 2 /γ-Al 2 O 3 . A pseudo-first-order kinetic model considering the direct desulfurization (DDS) and two detailed partial and full hydrogenation pathways was formulated with simple power law rate equations. The apparent rate constants of five lumped reactions on CoMoS 2 /MZSM-5 are 2–4 times larger than those of CoMoS 2 /γ-Al 2 O 3 . With both catalyst system, the pre-exponential factor plays a dominant role in the reaction rate of DDS pathway showing equally high activation energies. The apparent activation energies show a critical effect on the reaction rate of two hydrogenation and subsequent desulfurization reactions. Furthermore, the Delplot analysis was applied to identify the reaction sequence of product formation and verify the reaction network. The HDS performance and reaction rates of individual reaction steps can be rationally linked to the morphology and available content of CoMoS phase as identified by HRTEM and XPS characterization. Thus, multi-stacked MoS 2 nanocrystallites on CoMoS 2 /MZSM-5 provide more available sulfur vacancies to facilitate the DDS pathway, and catalyze efficiently the hydrogenation and subsequent desulfurization with the synergy of brim sites and sulfur vacancies.
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 12
·3817-3825
·
IF 6.177
Zhefei Zhao,Tianyang Guo,Xingyu Luo,Xuetao Qin,Lingxia Zheng,Li Yu,Zhuoqing Lv,Ding Ma,Huajun Zheng
Bimetallic-sites construction and coordination species tuning are considered as effective strategies to improve electrocatalytic performance of 5-hydroxymethylfurfural (HMF) oxidation. However, it remains a challenging issue to clarify the roles of dual-sites and coordinating anions through optimized electronic structure. Herein, hierarchical NiCo-based sulfide (NiCo–S) nanosheets are reported to disclose the composition-dependent activity at the atomic level. X-ray absorption spectroscopy (XAS) evaluates the tuned electronic configuration. Electrochemical experimental and theoretical results manifest that Ni–Co dual sites synergistically participate in HMF oxidation, where Co sites promote the transformation of the aldehyde (CHO) group to the carboxyl group with the strong diatomic adsorption (O and C atoms) on the CHO group of HMF, while Ni sites speed up the reaction rate of 2,5-furandicarboxylic acid (FDCA) generation. Meanwhile, the coordinating S species also contributes to the formation of strong diatomic adsorption with the CHO group of HMF, and a larger density of state (DOS) of NiCo–S at the Fermi level demonstrates a higher conductivity for carrier transfer compared with NiCo–O. All the above studies confirm the effects of the Ni–Co dual-sites and S coordination on accelerating reactions and lowering energy barriers, thus facilitating the catalytic activity (98.0% selectivity and 97.1% yield for FDCA) with rapid reaction kinetics and low onset potential (1.2 V vs. RHE).
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 14
·6756-6764
·
IF 3.925
Boyong Ye,Wenyang Zhang,Ruru Zhou,Yuanyuan Jiang,Zixin Zhong,Zhaoyin Hou
The dehydration of fructose to 5-hydroxymethylfurfural (5-HMF) is a crucial step in the biorefinery process, and finding a recyclable solid-acid catalyst and green solvent remains a challenge. In this work, a mesoporous sulfonated high-crosslinked polymer (abbreviated as SHCP) was synthesized following a facile route and used in the dehydration of fructose to 5-HMF in different solvents. The structure and properties of SHCP were characterized using N2 adsorption–desorption, XRD, Raman, SEM, TEM, FTIR, 13C CP/MAS NMR and XPS techniques. It was confirmed that SHCP possesses high surface area, uniform mesoporous and abundant sulphonic groups, and it can promote the dehydration of fructose to 5-HMF under mild reaction conditions. At the same time, the performance of SHCP in different solvents was tested in detail, it was found that SHCP exhibited similar initial activity in 1,4-dioxane/H2O mixture as that in dimethyl sulfoxide (DMSO), while the stability of SHCP in 1,4-dioxane/H2O mixture was enhanced obviously compared with that in DMSO. The reason for the deactivation of SHCP in different solvents was discussed, and it was disclosed that a small amount of water in DIO could depress the oligomerization of 5-HMF and enhance the stability of SHCP.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yang Wang,Yafei Wen,Yun Qu,Zhichao Pei,Yuxin Pei
Nitric oxide (NO)-mediated gas therapy (GT) and alkyl radical (R•) therapy (ART) are emerging cancer therapy modes, and multi-mode therapy has been recognized as an attractive strategy for enhancing anti-cancer efficacy. In this work, a thermal-responsive R• initiator 2,2′-azobis[2-(2-imidazolin-2-yl)propane] dihydrochloride (AIBI)-loaded glycol-targeting NO nanogenerator was constructed by first the covalent conjugation of thermal-responsive NO donor of S-nitrosothiols (RSNO) on the surface of mesoporous silica-coated gold nanorods ( [email protected] ), then the coating of a supramolecular complex of amino pillar[5]arene (NP5) and galactose derivative (G), and finally the loading of AIBI. The glycol-targeting NO nanogenerator demonstrated specific targeting ability to HepG2 cells owing to the recognition between galactose residues and asialoglycoprotein receptors (ASGPR). Specially, upon 808 nm near-infrared (NIR) irradiation, the AIBI-loaded NO nanogenerator generated hyperthermia to achieve photothermal therapy (PTT), and further GT and ART resulted from the thermal responsiveness of RSNO and AIBI, respectively. In vitro experiments revealed that the AIBI-loaded glyco-targeting NO nanogenerator had good biocompatibility and exhibited effective inhibition to the proliferation of HepG2 cells. This work provides a novel way to supramolecular hybrid drug delivery systems for triple-mode targeting therapy of PTT/GT/ART.
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PubMed
高影响因子
ANALYST
·
2022
·Vol. 147
·期 8
·1598-1610
·
IF 5.227
Huizhen Deng,Jie Zhao,Shifan Zhao,Shuai Jiang,Guofeng Cui
Developing an accurate, sensitive, and efficient portable device for simultaneous detection of disease-related biomolecules is an attractive challenge for point-of-care testing (POCT). In this work, we introduced a novel graphene-based electrochemical flow analysis device (GEFAD), which combined a 3D-printed flow cell with a three-electrode system based on a gold nanoparticle-modified graphene (AuNPs@Gr) working electrode to simultaneously detect depression-related biomolecules: dopamine (DA), 5-hydroxytrypserotonin (5-HT), and melatonin (MEL). Electrochemical studies showed that the GEFAD had high selectivity and sensitivity in the determination of DA, 5-HT, and MEL with their significant separation peaks. The linear ranges of DA, 5-HT, and MEL were respectively found to be 0.1–70 μM, 0.1–100 μM, and 0.1–150 μM, with the corresponding detection limits of 0.054 μM, 0.071 μM, and 0.087 μM (S/N = 3). In addition, the GEFAD presented a good anti-interference ability and satisfactory reproducibility, and can be used in real calf serum sample analysis. The introduced in-flow electrochemical detection device showed excellent repeatability, less sample consumption, and simple operation, which increases the possibility to implement POCT. This study also proposed a promising application prospect for the development of portable biomolecules detection devices.
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PubMed
高影响因子
CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Lirong Yang,Xuan Luo,Lin Yan,Yawen Zhou,Shaoqing Yu,Hui Ju,Yan Wang,Lin Zhang
In the present study, a novel eco-friendly foam (CS-AMP) was successfully prepared by grafting adenosine 5′-monophosphate (AMP) with high biocompatibility onto environment-friendly monomer chitosan (CS). The CS-AMP foam was used to absorb uranium and exhibited an efficient selective adsorption of uranium from aqueous solution and natural seawater . Due to the phosphate group of AMP, the CS-AMP foam shows an excellent adsorption capacity of 311 mg/g (pH 5.0 and 308 K) for uranium, which is much higher than that of CS-PTA foam without modification by AMP. The adsorption process is fitted well with Sips isothermal and pseudo-second-order kinetic models . As a highly selective uranium adsorbent, it is expected to be applied to extract uranium from wastewater and seawater.
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PubMed
高影响因子
Solar RRL
·
2021
·Vol. 6
·期 4
·2100995
·
IF 8.582
Chunyan Wang,Jihuai Wu,Shibo Wang,Zhongliang Yan,Xuping Liu,Guodong Li,Liqiang Chen,Sijia Zhu,Weihai Sun,Zhang Lan
Interface engineering has been proven to be an effective method to improve the performance and stability of perovskite solar cells (PSCs). Herein, 5-chloroindole (Cl-indole) is introduced into the interface of a SnO 2 electron transport layer and perovskite light-absorbing layer to improve the photovoltage performance of the device. The results show that Cl−indole can not only form hydrogen bonds with iodine in the perovskite to optimize the interface contact but also coordinate and passivate the Pb 2+ and Sn 4+ interface defects to alleviate carrier nonradiative recombination. Compared with the pristine SnO 2 -based planar PSCs with a power conversion efficiency (PCE) of 20.58%, the Cl−indole-modified SnO 2 -based device achieves a PCE of 22.47%. Meanwhile, the stability of the modified device is effectively improved and the hysteresis effect is reduced. This work demonstrates a promising strategy for high-efficient and stable PSCs by optimizing interface contact and passivating interface defects.
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Catalysts
·
2023
·Vol. 13
·期 6
·969
·
IF 3.9
Srinivasan Vinju Vasudevan,Jin Cai,Junming Xu,Hongjian Lin,Hongliang Wang,Quan Bu
In this work, the microwave-assisted reaction of 5-hydroxymethylfurfural (5-HMF) into valuable ether and acylated production formation was investigated with the help of molybdophosphoric acid encapsulated dendritic fibrous silica (KCC-1) as a catalyst. XRD, N2adsorption-desorption, SEM, FT-IR, NH3-TPD, and TEM were used to analyze the physicochemical and structural properties of the synthesized catalysts. The microwave etherification of 5-HMF with ethanol was tested using synthesized catalysts. The effects of the reaction temperature, reaction time, catalytic amount, and microwave power were investigated. The resulting MPA-KCC-1 and IMPA-KCC-1 catalysts demonstrated excellent activity for the etherification of 5-HMF with ethanol, producing 5-(hydroxymethyl) furfural diethyl acetal (HMFDEA) and 5-(ethoxymethyl)furfural diethyl acetal (EMFDEA) products selectively. The significant advantages of the work are the selective production of EMFDEA at 82%, the catalyst can be easily removed via filtration, and the catalyst activity remains nearly intact even after five reaction cycles.Keywords:biomass;acetylation;5-HMF;etherification;heteropolyacid;fibrous silica
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高影响因子
Nanoscale
·
2021
·Vol. 14
·期 2
·250-262
·
IF 7.79
Jian Tian,Lixue Qi,Quan Zhang,Guowu Zhan,Daohua Sun,Qingbiao Li
Inspired by the alveolar configuration, an alveoli-like ZSM-5 and the corresponding platinum encapsulated nanocomposite (Pt@PZ5) were fabricated via a dual-template method and a controlled selective desilication–recrystallization strategy. The dimensions of the central cavity, interconnected zeolitic vesicles, and mesoporous shell could be tuned by adjusting the synthesis parameters, as verified by scanning electron microscopy, transmission electron microscopy, nitrogen physisorption investigations, X-ray photoelectron spectroscopy, and X-ray diffraction techniques. Thanks to these properties and merits, the alveoli-like Pt@PZ5 showed the highest catalytic performance with excellent stability, obtaining 100% benzene conversion at 180 °C. Adsorption experiments combined with a finite-element simulation study uncovered that the alveolar architecture could expedite the accumulation of reactants and boost mass transfer; the conversion of intermediates in the voids could be further facilitated, giving optimal catalytic performance. Additionally, the alveolar architecture is resistant to metal sintering (5–20 nm) and leaching, even after calcination at 850 °C for 360 min. This work provides an alveolar concept into the rational design of efficient catalysts for fundamental catalytic action.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Weizhen Xie,Huai Liu,Xing Tang,Xianhai Zeng,Yong Sun,Xixian Ke,Tianyuan Li,Huayu Fang,Lu Lin
The catalytic conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), a renewably sourced substitution for petroleum-derived terephthalic acid, at a high concentration is highly demanding but challenging. Herein, the efficient conversion of HMF (10–25 wt%) in 1,4-dioxane/H 2 O was achieved, and a desirable FDCA yield of 98% was obtained from HMF (10 wt%) over commercial Ru/C (2 Equiv. NaHCO 3 , 4 MPa O 2 , 3 h, and 140 ℃). In addition, a two-step cascade reaction was developed for FDCA production, in which FDCA was employed as the acid catalyst to promote the dehydration of fructose (10 wt%) to HMF, followed by oxidation in 1,4-dioxane/H 2 O to FDCA over Ru/C. As compared to pure water or 1,4-dioxane, the better stability of HMF in 1,4-dioxane/H 2 O with a weak alkaline environment and the enhancement of superoxide radicals (·O 2 - ) in 1,4-dioxane/H 2 O could ensure high FDCA yield at high HMF concentration.
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高影响因子
FUEL
·
2021
·
IF 6.609
Nai-Yu Yao,Jing-Pei Cao,Jing-Ping Zhao,Zi-Meng He,Xiao-Bo Feng,Tian-Long Liu,Ze-Ying Wang,Xiao-Yan Zhao
A series of Zn-containing HZSM-5 (HZ5) with hierarchical pores (xZn(DS)) were obtained by adding different amounts of Zn(NO 3 ) 2 solution in a hydrothermal synthesis process. The performances of xZn(DS) in catalytic reforming of cellulose pyrolysis volatiles were investigated at 500 °C. The results showed that the addition of Zn during synthesis increased in the total pore volume of xZn(DS) and reduced the content of strong acid sites, and introduced new weak acid sites. The Zn species were highly dispersed inside the zeolite, and enhanced the accessibility of acid sites, so that the yields of light aromatic hydrocarbons and monocyclic aromatic hydrocarbons (MAHs) over 0.7Zn(DS) (The molar ratio of ZnO/Al 2 O 3 in the synthesis process of xZn(DS) was 0.7) were higher than those over S-HZ5 (Zn was not added in the synthesis process) and commercial HZ5. Compared with S-HZ5, the yield of MAHs over 0.7Zn(DS) increased from 92.8 to 114.1 mg/g and the coke yield decreased by 2.9%. The selectivity of MAHs over 0.7Zn(DS) was 87.7%, which was 5.3% higher than that over S-HZ5. Simultaneously, the increase in mesopores of xZn(DS) accelerated the mass transfer process, shortened the diffusion path and improved the anti-coking performance of the catalysts. In addition, this study also proposed a possible mechanism for the catalyst to adjust the distribution of aromatic products and provided a new idea for promoting the selective production of MAHs for the pyrolysis of cellulose.
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高影响因子
FUEL
·
2021
·
IF 6.609
Guo Qiu,Biaohua Chen,Ning Liu,Chongpin Huang
5-Hydroxymethylfurfural (5-HMF), an important and value-added platform chemical, has inspired increasing attention. In this study, hafnium-tin composite oxides (Sn-HfO 2 ) were prepared by one-pot coprecipitation process and used as effective synergistic catalysts for 5-HMF synthesis from the conversion of glucose. Pyridine-FTIR results reveal that Sn-HfO 2 catalysts have strong Lewis and weak Brønsted acid sites. With 0.5Sn-HfO 2 as the catalyst, the highest yield of 5-HMF obtained from glucose was 75.5% with 99.5% conversion at 170 °C for 2 h in a methyl isobutyl ketone (MIBK)/water biphasic system. Furthermore, the catalytic system also possesses excellent performance in converting other carbohydrates. The catalysis mechanism for the isomerization of glucose to fructose was explored by the density functional theory (DFT) method, indicating that Lewis acidic Hf active sites and proton mediator Sn-O species synergistically catalyzed the isomerization process, effectively lowering the reaction energy barrier. The cooperative action of terminal Hf-OH and Sn-OH also facilitated the formation of 5-HMF in fructose dehydration. 0.5Sn-HfO 2 could be reused for four runs without significant loss of catalytic activity. This approach provides the feasibility of composite oxides as synergistic catalysts for carbohydrate conversion to 5-HMF.
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