JOURNAL OF CATALYSIS
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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
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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
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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
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Weiping Liao,Haoyi Lin,Jiaxing Zhang,Jiaqi Wang,Kaixuan Yang,Ting Su,Hongying Lü,Zhiguo Zhu
2,5-Furandicarboxylic acid (FDCA) is a potential substitute of petroleum-based terephthalic acid to manufacture polymer. The selective aerobic oxidation of renewable 5-hydroxymethylfurfural (HMF) to FDCA is a promising and appealing route for establishing sustainable and environmentally friendly chemical process. Au catalysts have exhibited exceptional catalytic performances for this highly anticipated chemical transformation, where the used support intensively impacts the catalytic productivity from the standpoint of metal-support and guest organic-support interactions. Herein, Sn-Beta zeolite was straightforward and rapidly synthesized via structural reconstruction without the auxiliary of any solvents, which was adopted as support for Au catalyst to construct bifunctional catalysts. As for Au/Sn-Beta sample, Lewis acid sites were related to Sn 4+ ions in the zeolite framework, while electronic properties and particle size of Au species were capable of being modulated by Au dosages. In addition, charge transfer from Au species to framework Sn 4+ ions resulted in the formation of Au δ+ species. Au/Sn-Beta catalyst with metal-Lewis acid cooperative active sites showed unique catalytic productivity of FDCA product in the aerobic oxidation of HMF to FDCA, whose catalytic performance was correlated with Lewis acid amounts as well as geometric and electronic effect of Au particle. Reaction mechanism analysis revealed the pathway and concrete step that Lewis acid site functioned. The aim is to provide some guidance for constructing a task-specific multifunctional supported catalyst from the view of support-enhanced effect for the catalytic conversion of biomass resource with multi-functional-groups.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Tuo Xin,Rongkun Zhou,Qiuju Xu,Xiangcheng Yuan,Zilong Zheng,Yiqing Li,Qi Zhang,Jinzhang Liu
Aqueous rechargeable Zn-ion batteries (ZIBs) have been regarded as a complement to LIBs due to their merits in terms of high safety, low cost, environmentally benignity, and long cycle life. However, the Zn metal anode suffers from corrosion and parasitic reactions in the aqueous electrolyte, which lead to growth of byproduct flakes and hydrogen gas evolution in the Zn platting/stripping process. Here, an organic additive, 15-crown-5 ether (15-CE-5), is added into the aqueous ZnSO 4 electrolyte to improve the Zn anode performance by altering the Zn 2+ solvation sheath. Other CE molecules such as 12-CE-4 and 18-CE-6 are also tested, while their efficacies are inferior compared to that of 15-CE-5. The optimal concentration of 15-CE-5 in the ZnSO 4 electrolyte is found to be 2 wt%, which enables the best performance of Zn anode in either Zn||Zn symmetric cells or MnO 2 ||Zn full cells. Using this modified electrolyte, the Zn||Zn symmetric cell exhibits a cycle life of 770 h when tested at 2 mA cm −2 and a set capacity of 2 mAh cm −2 , and the MnO 2 ||Zn full cell shows enhanced and stable capacity over 1000 cycles. The experimental results are elucidated by theoretical studies including molecule dynamics simulations and density functional theory calculations.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Huijie Xie,Wei Xu,Saiai Ran,Xiaolong Li,Bin Li,Yanyan Li,Lei Wang
Green synthesis of zeolite has been made much progress due to solvent-free grinding methods. Although solid-state synthesis is a simple green process with a high yield, its kinetics of the solid-phase crystallization process is still slow and the precursor materials are not uniformly heated throughout the reactor resulting into the poor uniformity of the particles. Herein, we report a high-efficiency organotemplate-free synthesis of ZSM-5 combining solid state grinding and steam-assisted crystallization. Solid state grinding (SSG) of aluminosilicate precursor avoids usage of solvent and steam-assisted conversion (SAC) in an organic-template-free condition grants a fast crystallization rate of ZSM-5. More importantly, the vapor fulfilled in the reactor ensures uniform heating of solid feedstock for crystallization of ZSM-5, leading the high crystallinity and the uniform particle size distribution . This combination can guarantee 100% relative crystallinity of ZSM-5 in 12 h, compared to that of 80% crystallinity from sole solid state at the same crystallization temperature (180 °C). Furthermore, this combination can achieve 83% relative crystallinity of ZSM-5 at 160 °C, compared to that of 37% crystallinity from the solid state alone. Highly dispersed ZSM-5 zeolite with adjustable SiO 2 /Al 2 O 3 ratio is prepared by steam-assisted crystallization of grinding solid raw materials. The catalytic activity of ZSM-5 catalyst from this combination strategy for the acetalization of cyclohexanone is superior to that of the solid-state method alone. This sustainable and green synthesis method provides a potential way for the preparation of zeolites in an industrial scale.
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高影响因子
FUEL
·
2022
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IF 8.035
Dengle Duan,Yongchuan Zhang,Juncheng Li,Liyin Huang,Zhimin Xu,Yayun Zhang,Weimin Sun,Qin Wang,Roger Ruan
The catalytic pyrolysis of low-density polyethylene over hierarchical HZSM-5 zeolite was studied to improve liquid oil quality in a facile reactor for the first time. The HZZ was successfully synthesized by using green and inexpensive nanocrystalline cellulose as a mesoporous template. Nanocrystalline cellulose played a disturbing role in the crystallization process of hierarchical HZSM-5 zeolite, which facilitated the formation of ordered surface morphology and excellent porous structure. Compared with conventional HZSM-5, hierarchical HZSM-5 zeolite can significantly improve the bio-oil yield. The relative content of cycloalkanes increased while the relative content of aromatics decreased. The 94.4 area.% of jet fuel range hydrocarbons with 51.8 area.% cycloalkanes and 25.0 area.% of aromatics can be obtained. Hierarchical HZSM-5 zeolite with a low Si/Al ratio had high acidity favors high liquid yield and aromatic hydrocarbon selectivity . The current work contributes to the green synthesis of Hierarchical HZSM-5 zeolite while providing a novel catalyst for value-added fuels production from waste plastics pyrolysis.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 35
·16990-16997
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IF 3.925
Guohao Xu,Xin Gao,Tao Luo,Yajie Duan,Huan Qian,Jisheng Yu,Xuedong Zhu
A novel core–shell ZSM-5@ZnO was successfully fabricated through a hydrothermal coating strategy, and the catalytic performance of ZSM-5@ZnO in the methane co-aromatization with propane (MCP) reaction was investigated using a physically-blended ZSM-5/ZnO catalyst as a comparison. Multi-techniques including XRD, ICP-AES, TEM, EDS, XPS, N2 adsorption, 27Al NMR, IR and IG were employed to investigate the deactivation of the carbon deposition and the physicochemical properties of ZSM-5@ZnO. The results revealed that the introduction of methane into propane aromatization can promote the formation of Zn methyl species, further promoting the conversion of reactants and the formation of products. The MCP reaction at 550 °C revealed that ZSM-5@ZnO showed a higher methane and propane conversion and greater aromatic selectivity than those of the physically-blended ZSM-5/ZnO catalyst. The special reaction pathway of the shell (ZnO, metallic sites)–core (ZSM-5, acidic sites) and the relatively close proximity between ZnO and ZSM-5 were responsible for the excellent properties in MCP. Additionally, the formation of the micro–mesoporous property accelerated the mass-transfer rate and inhibited the formation of carbonaceous deposition, significantly enhancing the lifetime of the catalyst. Thanks to the novel core–shell structure of the ZSM-5@ZnO catalyst, it showed excellent properties in the MCP reaction.
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高影响因子
RSC Advances
·
2022
·Vol. 12
·期 36
·23118-23128
·
IF 4.036
Luxin Zhang,Xu Xing,Ruijun Sun,Meng Hu
Selective catalytic conversion of carbohydrates to 5-ethoxymethylfurfural (EMF) is a critical approach to the biorefinery. In this work, solid acid catalysts of γ-AlOOH and CeO2@B2O3 were used to convert carbohydrates to EMF in a one-pot process, performed in an ethanol/DMSO solvent system. The synergistic effect of γ-AlOOH and CeO2@B2O3 was studied. Furthermore, the morpho-structural properties of the catalysts were characterized, and the effects of reaction time, reaction temperature, catalyst load, and the amount of cosolvent on the conversion of glucose to EMF were examined and optimized. Under the reaction conditions of 170 °C for 20 h, glucose, sucrose, cellobiose, inulin and starch were used as raw materials, and the EMF yield range was 9.2–27.7%. The results showed that the synergistic effect of γ-AlOOH and CeO2@B2O3 further causes the combination of multiple acid sites with different types and strength distributions. Particularly, the collaboration between weak, medium-strong, and strong acid, as well as between Lewis and Brønsted acidity, is of great significance for EMF generation. The reusability experiments showed that the combined catalytic system was easily separated and maintained catalytic activity for five successive reactions without further intermediate regeneration steps. This work provides a promising route for the catalytic conversion of biomass-derived carbohydrates into EMF.
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PubMed
高影响因子
Gels
·
2022
·Vol. 8
·期 8
·475
·
IF 4.432
Chengdi Huang,Hanwei Zhang,Ziqing Hu,Youping Zhang,Xiaofan Ji
Polymer gels have been widely used in the field for tissue engineering, sensing, and drug delivery due to their excellent biocompatibility, hydrophilicity, and degradability. However, common polymer gels are easily deformed on account of their relatively weak mechanical properties, thereby hindering their application fields, as well as shortening their service life. The incorporation of reversible non-covalent bonds is capable of improving the mechanical properties of polymer gels. Thus, here, a poly(methyl methacrylate) polymer network was prepared by introducing host–guest interactions between pillar[5]arene and pyridine cation. Owing to the incorporated host–guest interactions, the modified polymer gels exhibited extraordinary mechanical properties according to the results of the tensile tests. In addition, the influence of the host–guest interaction on the mechanical properties of the gels was also proved by rheological experiments and swelling experiments.Keywords:polymer gels;host–guest interactions;mechanical performance;pillar[5]arene
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PubMed
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Linhao Yu,Hong Chen,Yingying Li,Zhe Wen,Yongdan Li
The metallic cobalt supported on nitrogen dopped carbon material was employed as an efficient catalyst in the oxidative esterification of 5-hydroxymethylfurfural (HMF) to furan-2,5-dimethylcarboxylate (FDMC). The carbonization temperature has a significant effect on the morphology and structure of Co/N-C samples. The Co/N-C calcined at 900 °C exhibits the best catalytic performance and a 73.8% FDMC yield at 91.7% HMF conversion is measured at 130 °C for 20 h with K 2 CO 3 under 1 MPa O 2 . The catalytic activity of Co/N-C was benefited by the synergistic effect between the metallic cobalt and nitrogen-doped carbon material. The reaction mechanism of FDMC formation was proposed.
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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
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