ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Xusheng Guo,Haoxiang Zhu,Yuxi Si,Heng Ban,Xilei Lv,Youwei Cheng,Lijun Wang,Xi Li
Converting carbohydrates to 5-hydroxymethylfurfural (HMF) is an important goal for biorefinery. Although various deep eutectic solvents (DESs) have been reported for HMF production, the field lacks systematic research on the effect of cations and anions and an effective catalytic system for converting concentrated carbohydrates. Here, 12 kinds of DESs containing four cations and six anions were systematically evaluated and tetraethylammonium bromide (TEAB) was confirmed as the most effective DES, which provided HMF yields of 90 and 76% from fructose and glucose, respectively. The stable bromide-substituted intermediate may explain the positive effect of bromide based on the results of density functional theory calculation. A high concentration substrate has an adverse impact on the selectivity of HMF due to the HMF concentration caused by glucose, CrCl3·6H2O, and concentrated HMF. To inhibit the condensation, a biphasic system of TEAB/THF is developed to convert a highly concentrated glucose of 62.5 wt % (83.3 wt % with respect to TEAB), providing an excellent HMF yield of 72%. This study has revealed the impact of cations and anions of DESs on HMF production, which will serve as a base for designing task-specific DESs. Moreover, an efficient catalytic system to produce HMF from concentrated glucose was also provided.
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RENEWABLE ENERGY
·
2022
·
IF 8.634
Xiaocui Wei,Yanan Liu,Yang Cao,Jin Li,Xianghao Meng,Zhao Zhang,Zhongyi Jiang
The catalytic pyrolysis of biomass is a sustainable approach for biofuel production, contributing to replacing fossil resources with renewable resources . The ZSM-5 zeolite remains an attractive catalyst in the catalytic pyrolysis of biomass, and how to reduce the product diffusion resistance and regulate the surface acidity of ZSM-5 should be explored more deeply. Herein, a hierarchical gallium-modified ZSM-5@SBA-15 catalyst is fabricated through coating a mesoporous layered SBA-15 shell on a hollow ZSM-5 core with gallium modified on the surface, which is effective for increasing hydrocarbon production during the catalytic pyrolysis of biomass process. The synergistic effect of hollowness, mesoporosity, and activity in the hierarchical gallium-modified ZSM-5@SBA-15 catalysts is found to affect the yield and quality of bio-oil. Accordingly, the hierarchical gallium-modified ZSM-5@SBA-15 catalyst with 11 wt% Ga loading exhibits a superior deoxygenation ability, and the relative content of hydrocarbons in bio-oil reach to 49.76 area% which is much higher than that of ZSM-5 (35.30 area%). Furthermore, a possible catalytic pyrolysis mechanism of biomass was also proposed to clarify the potential application of hierarchical gallium-modified ZSM-5@SBA-15 catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Z.W. Zhu,Q.R. Zheng
Comparisons were made between the samples mechanochemically (MOF-5(M)) and solvothermally (MOF-5(S)) prepared for the development of efficient hydrogen storage medium. Synthesized samples were undergone structural characterization as well as adsorption equilibrium measurements of hydrogen at temperature-pressure range 77 K–87 K and 0.1–10 MPa. Grand Canonical Monte Carlo (GCMC) simulations were further conducted to study the behaviors of hydrogen molecules adsorbed on MOF-5. It shows that, besides the advantage of large scale synthesis and a lower cost, mechanochemical method respectively brings about 207% and 90.5% increments in the specific surface area and the maximum excess adsorption capacity of hydrogen at 77 K within pressure range 0–10 MPa. Results also reveal that the crystal within MOF-5(M) is regular and distributing uniformly with a mean size only one tenth of that of the MOF-5(S); at 77 K within pressure range 0–10 MPa, Toth equation can predict the adsorption equilibrium data of hydrogen on two MOF-5 samples with a mean relative error less than 1.5%. It suggests that MOF-5(M) is more promising for hydrogen storage by adsorption for practical applications.
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ACS Catalysis
·
2022
·
IF 13.7
Xuliang Pang,Hongye Bai,Huaiquan Zhao,Weiqiang Fan,Weidong Shi
Electrocatalytic conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to value-added 2,5-furandicarboxylic acid (FDCA) is of great significance for sustainable chemical production. The key challenge is to establish an electrocatalytic system with a wide potential window, which can selectively oxidize HMF to FDCA without causing water oxidation. In this study, Cu foam decorated with Cu(OH)2 (CF-Cu(OH)2) was successfully fabricated as an efficient catalyst, and CuOOH active species generated by electrochemistry were demonstrated as the main catalytic sites for HMF oxidation. As a result, the current density of CF-Cu(OH)2 reached up to 198.2 mA/cm2 (100 mM HMF, 1.0 M KOH, 0.8 V vs Ag/AgCl), and a high faradic efficiency close to 100% for FDCA production (yield: 98.7%) was realized. Moreover, we reveal the mechanism for the electro-oxidation of HMF to FDCA and further provide an insight into the oxidation pathway for HMF. A paired electrochemical system exhibits superior catalytic performance of synergetic reactions (HMF oxidation and 4-NP reduction). Therefore, this work proposes a strategy to simultaneously produce two types of value-added chemicals at both electrodes, which can be applied in other electrocatalytic systems for the green synthesis of organic compounds.
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Nature Catalysis
·
2022
·Vol. 5
·期 1
·45-54
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IF 40.706
Qi Guodong,Davies Thomas E.,Nasrallah Ali,Sainna Mala A.,Howe Alexander G. R.,Lewis Richard J.,Quesne Matthew,Catlow C. Richard A.,Willock David J.,He Qian,Bethell Donald,Howard Mark J.,Murrer Barry A.,Harrison Brian,Kiely Christopher J.,Zhao Xingling,Deng Feng,Xu Jun,Hutchings Graham J.
The oxidation of methane, the main component of natural gas, to selectively form oxygenated chemical feedstocks using molecular oxygen has been a long-standing grand challenge in catalysis. Here, using gold nanoparticles supported on the zeolite ZSM-5, we introduce a method to oxidize methane to methanol and acetic acid in water at temperatures between 120 and 240 °C using molecular oxygen in the absence of any added coreductant. Electron microscopy reveals that the catalyst does not contain gold atoms or clusters, but rather gold nanoparticles are the active component, while a mechanism involving surface adsorbed species is proposed in which methanol and acetic acid are formed via parallel pathways.
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AICHE JOURNAL
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2022
·Vol. 68
·期 7
·e17677
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IF 4.167
Shen Hu,Jiaxuan Chen,Qunfeng Zhang,Junru Liu,Jinlin Meng,Guanghua Ye,Xinggui Zhou,Weikang Yuan
Surface barriers persist in the molecular transport across external crystal surface of zeolites, which brings strong influences on zeolite catalysis. This study probes the role of crystal-size–dependent surface barriers in zeolite catalysis, with n -pentane isomerization catalyzed by Pt/ZSM-5 as a model reaction system. Chemical liquid deposition of SiO 2 is performed to reduce surface barriers on ZSM-5 crystals with different sizes. After SiO 2 deposition, surface barriers on both small (266 nm) and large (1304 nm) crystals are significantly reduced, while the improvement in catalytic activity for the large crystals (76.1%–129.1%) is much higher than that for the small ones (−17.4% to 16.7%). For the large ZSM-5 crystals, diffusion limitation is stronger, and thus the effect of surface barriers on catalytic activity is more important. This study reveals the unique role of crystal-size–dependent surface barriers in zeolite catalysis, and understanding this is important for the optimal design of zeolite catalysts.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2022
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IF 5.895
Xiaoqi Wang,Dongli Li,Yong Cao,Chi-Tang Ho,Qingrong Huang
5-Demethylated polymethoxyflavones (5-OH PMFs) are the most unique monodemethylated PMFs with relatively low polarities and are proved to possess better anticancer and anti-inflammatory effects than their respective permethoxylated ones. However, their detailed in vivo metabolic fates have not been fully studied. 5-Demethylsinensetin (5-OH Sin), being one of the 5-demethylated citrus PMFs, was used in the present research to investigate its biotransformation in pharmacokinetics and excretion in rats. The results showed that 5-OH Sin was mostly accumulated in the large intestine, indicating its poor absorption in the small intestine. In addition, 5,3′-didemethylsinensetin and 5,4′-didemethylsinensetin were identified as two dominated metabolites of 5-OH Sin, and the C-3′ position of 5-OH Sin was more facile to be demethylated in systemic circulation. Moreover, other than demethylation reactions, the methylation transformation of 5-OH Sin and its metabolites were also observed and quantified, suggesting that the bidirectional biotransformation between 5-OH Sin and its parent compound, Sin, occurred under in vivo conditions.
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PubMed
高影响因子
Nano Today
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2022
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IF 18.962
Shuwen Guo,Qiaoxian Huang,Jianwen Wei,Shengpeng Wang,Yitao Wang,Leyong Wang,Ruibing Wang
Due to membrane impermeability of proteins, intracellular delivery of protein is of significant challenge. Although numerous protein carriers have been reported, it remains difficult to efficiently deliver proteins with different isoelectric points into cells. Herein, guanidinium perfunctionalized pillar[5]arene (GP5) was employed for efficient delivery of proteins with different isoelectric points into different cell lines, and the bioactivities of the proteins were well maintained after intracellular delivery. After comparison with linear cell-penetrating peptides, unsymmetrical guanidinium-macrocycles, primary and quaternary ammonium functionalized pillar[5]arene derivatives, and the monomer of GP5, the high protein delivery potency of GP5 was mainly attributed to the densely pre-organized guanidinium groups on both sides of the pillar[5]arene skeleton, which could not only facilitate GP5 to bind with proteins to form protein nano-aggregates, but also promote cellular uptake of proteins via interactions with cellular surface. This study offers important new insights to the design and development of cell-penetrating peptide mimetic molecules for protein transductions.
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JOURNAL OF CHEMICAL RESEARCH
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2022
·
IF 1.097
Ying Wang,Fei Du,Chunyan Wang,Jiaqiang Zhao,Haizhu Sun,Chuanyin Sun
High-performance hierarchical cheese-like C-ZSM-5 nanocrystals are successfully prepared by acid–base treatment and are evaluated for oxidative desulfurization of dibenzothiophene. The acid–base treatment can generate a large number of Si-OH bonds and an open-mesoporous structure, which is conducive for the dispersion of TiO2 and also for the transport of dibenzothiophene and its oxidation products simultaneously. The catalytic results indicate that the hierarchical cheese-like C-ZSM-5 nanocrystals are highly active catalysts for the oxidative desulfurization of dibenzothiophene due to open mesoporosity. Complete conversion was obtained within 80 min at 338 K. The excellent performance is due to the large number of active framework sites and open mesopores generated by post-processing.
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CATALYSIS LETTERS
·
2022
·Vol. 152
·期 12
·3716-3724
·
IF 2.936
Chen Hong,Li Yingying,Yu Linhao,Wang Sen,Ma Xueli,Wang Can,Li Yongdan
A series of hydroxyapatite (HAP) supports with different Ca/P ratios were synthesized to prepare the MnO x /HAP catalysts. A MnO x /HAP catalyst showed highly efficient conversion of 5-hydroxymethylfurfural (HMF) into 2, 5-diformylfuran (DFF) in toluene solvent under no-alkali condition. 86.4% conversion of HMF with 90.9% selectivity of DFF at 120 °C for 12 h under 1.0 MPa O 2 over the MnO x /HAP-10.0-400 were obtained. The redox of Mn 4+ /Mn 3+ improved the oxidation of 5-HMF to DFF by the lattice oxygen, and the lattice oxygen was replenished by adsorbing O 2 molecules. The reusability tests were found the catalyst could be reused up to four cycles without notable loss of catalytic activity. The MnO x /HAP-10.0-400 was a stable and reusable material for further industrial exploration of DFF in an environmentally friendly way. Graphical Abstract
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BIOMASS & BIOENERGY
·
2022
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IF 5.774
Gang Liu,Yujiao Xie,Chunjie Wei,Chang Liu,Feng Song,Xiuyu Sun,Yuan Zhang,Hongyou Cui
The one-pot approach was developed by using molten salt hydrate consisting of ZnCl 2 ·4H 2 O and LiCl·3H 2 O to produce 5-hydroxymethylfurfural (5-HMF) from cellulose . Cellulose was dissolved and regenerated to study the interaction of cellulose and molten salt hydrate. The effects of ZnCl 2 ·4H 2 O concentration, reaction time, and temperature on the conversion of cellulose to 5-HMF were investigated. 5-HMF yield increased when ZnCl 2 ·4H 2 O was mixed with LiCl·3H 2 O, and the maximum value (44.1%) was reached at 160 °C and 90 min when ZnCl 2 ·4H 2 O concentration was 64.9 mol%. The species of ZnCl 2 ·4H 2 O–LiCl·3H 2 O were analyzed, and the function of species concentration was correlated with the 5-HMF yield from the conversion of glucose and fructose. It was found that the synergistic catalysis of ZnCl 3 − , Zn 2+ , Zn(OH) + , H + as well as Li + promoted the efficiently cellulose conversion to 5-HMF.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 4
·1083-1088
·
IF 2.726
Xiao Peiwen,Li Hui,Wang Pingmei,Liu Bolun,Jing Wendan,He Lipeng,Wang Runwei,Han Xue,Zhang Zongtao,Qiu Shilun,Luo Jianhui
Herein, we propose a novel approach to reduce the viscosity of heavy oil by functional hierarchical CTMS-ZSM-5-PTMS zeolites. CTMS-ZSM-5-PTMS zeolites synthesized by asymmetric modification and selective alkali etching can reduce the viscosity of heavy oil through adsorbing asphaltenes. This method can reduce the viscosity of heavy oil from hundreds of thousands mPa·s to about ten thousand mPa·s. The work provides an economical and environmentally friendly candidate for heavy oil viscosity reduction under low-temperature conditions.
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危险品化学品经营许可证（带存储）