APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Jieyi Liu,Junde Wei,Xiao Feng,Mingxia Song,Song Shi,Sibao Liu,Guozhu Liu
Hydrodeoxygenation (HDO) is one of the effective methods for upcycling polycarbonate (PC) plastic waste, but the development of low-cost, high-performance HDO catalysts still faces great challenges. In this work, we report that a bifunctional Ni/HZSM-5 catalyst can directly upgrade PC plastic wastes into sustainable aviation fuel ranged cycloalkanes in high yields (99.3 %) with 81.2 % yield of C 15 dicycloalkane under mild reaction conditions (190 °C, 4 MPa H 2 ). Controlled reactions of PC and probe molecules demonstrated the conversion of PC into C 15 dicycloalkanes involves PC depolymerization by direct cleavage of C-O bonds adjacent to benzene ring and ester group, forming C 15 aromatics and C 15 monophenols at the metal sites, followed by hydrogenation of C 15 aromatics rings on metallic Ni sites and HDO of C 15 monophenols on metal-acid dual sites parallel to generate C 15 dicycloalkane. The C-C cracking mainly occurred on the tertiary carbon adjacent to the benzene ring on acidic sites of HZSM-5, thus forming C 6 ∼C 9 monocyclic alkanes. The realization of this process can be attributed to the cooperation between metal sites and acid centers on Ni/HZSM-5. Besides, the metal-acid balance (MAB) in Ni/HZSM-5 significantly affected the HDO activity and product distribution. 20Ni/HZSM-5(200) with suitable MAB showed good HDO activity and excellent selectivity to C 15 dicycloalkane. In addition, the obtained catalyst was also capable of converting common real PC plastics wastes (CD disk, DVD disk and PC sheet) into cycloalkanes with the yield up to 98 % and exhibited excellent stability. This approach to construct inexpensive bifunctional catalysts highlights an efficient and reliable route for HDO of PC to sustainable aviation fuel, providing a new avenue towards a circular economy.
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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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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Xiaohong Zhou,Wenfeng Zhou,Wei Zhuang,Chenjie Zhu,Hanjie Ying,Hongman Zhang
Cytidine 5′-monophosphate (5′-CMP) is an essential nucleotide for additives. In this study, enhanced production of 5′-CMP was realized by the transformation of cytidine using co-immobilized di-enzymes, uridine-cytidine kinase (UCK) and acetate kinase (AcK). The immobilization yield of the enzyme had a clear correlation with the surface charges as zeta potential ( ξ ). Among them, ε -polylysine-functionalized sepharose (SA-EPL, ξ = 9.31 mV) showed high immobilization yield (78.8%), which was 4.9-fold than that of nitrilotriacetic acid functionalized sepharose (SA-NTA, ξ = −12.6 mV). The residual activity of affinity co-immobilized enzyme (EPL-Ni/ [email protected] ) was higher than 70.6% after recycled 10 times. Thus, this study provides an effective approach for the production of 5′-CMP with the advantages of low adenosine 5′-triphosphate (ATP) consumption, reduced side reactions, and improved reusability by co-immobilized UCK and AcK on the functionalized Sepharose.
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Catalysts
·
2022
·Vol. 12
·期 10
·1216
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IF 4.501
Xiaoling Zhao,Jinlong He,Jinjin Li
A method of phase-transfer water/toluene synthesis was developed to fabricate mesocrystals of Zeolite Socony Mobil-5 (ZSM-5) that contain both meso-/micropores and nanometer crystallites. The construction of a hierarchical architecture from nanozeolites via oriented attachment growth was achieved by a simple phase-transfer water/toluene synthesis by minimizing classical atom-by-atom crystallization. This opens the way to the cheap, highly efficient engineering of zeolitic morphologies. The physicochemical properties of the crystal were revealed by powder X-ray diffraction (XRD), N2physical adsorption, inductively coupled plasma atomic emission spectroscopy (ICP-AES), scanning electron microscopy (SEM), transmission electron microscopy (TEM), ammonia temperature-programmed desorption (NH3-TPD) and pyridine infrared spectroscopy (Py-IR), indicating that the material has a high specific surface area, mesopore volume and Lewis acid content. The hierarchical ZSM-5 exhibits a prolonged catalytic lifetime in dimethyl ether–methyl ether (DTO) conversion and enhanced selectivity for propylene owing to the enhanced structural properties. The method can be extended to the synthesis of other graded zeolites controlled by the crystallization process and produce crystals comprising traversing mesoporosity and ultrasmall crystallites that are crucial for mass transfer enhancement.Keywords:phase-transfer water/toluene synthesis;ZSM-5;hierarchical architecture;dimethyl ether–methyl ether
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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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CHEMICAL ENGINEERING JOURNAL
·
2022
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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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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yaoyu Zhang,Yuxiong Wang,Yue Liu,Huimin Xu,Zhongbiao Wu
Aiming at the coexistence of pollutants in the actual industrial process, the catalytic oxidation of acetonitrile and ethyl acetate mixture on the Cu–Ce/ZSM–5 catalyst was studied. The mutual inhibition effect during catalytic removal of acetonitrile and ethyl acetate mixture was observed. Acetonitrile showed a more obvious inhibitory effect on the conversion of ethyl acetate, and the introduction of ethyl acetate reduced the N 2 selectivity of acetonitrile oxidation. The simulation results demonstrated acetonitrile could be preferentially adsorbed on Cu center of the catalyst surface, leading to significant inhibition of the initial conversion of ethyl acetate. In addition, the coexistence of ethyl acetate would weaken the hydrolysis of acetonitrile to generate carboxylic acid and –NH x species. As such, no enough adsorbed NH x species could be used to reduce the NO x produced by excessive oxidation of acetonitrile, resulting in a decreased in N 2 selectivity. This study could provide reference on the application of catalysts for cyanide–containing waste gas degradation.
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FUEL
·
2022
·
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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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
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 35
·16990-16997
·
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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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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