CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
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IF 3.171
Xiao Zhao,Xuan Shi,Zhongshun Chen,Long Xu,Chengyi Dai,Yazhou Zhang,Xinwen Guo,Dongyuan Yang,Xiaoxun Ma
A series of ZnO-ZrO 2 solid solutions with different Zn contents were synthesized by the urea co-precipitation method, which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts. As a new benzene alkylation reagent, syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene. A suitable ratio of ZnO-ZrO 2 led to the significant improvement in the catalytic performance, and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C 9 + aromatics. The highest benzene conversion of 89.2% and toluene/xylene selectivity of 88.7% were achieved over 10% ZnO-ZrO 2 &H-ZSM-5 (Si/Al = 23) at a pressure of 3 MPa and a temperature of 450 °C. In addition, the effect of the zeolite framework structure on product distribution was examined. Similar to the molecular dynamics of aromatic hydrocarbons , H-ZSM-5 zeolites comprise 10-membered-ring pores, which are beneficial to the activation of benzene; hence, the conversion of benzene is higher. H-ZSM-35 and H-MOR zeolites exhibited small eight-membered-ring channels, which were not conducive to the passage of benzene; hence, the by-product ethylbenzene exhibits a higher selectivity. The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance, and the powder mixing method was more conducive to the conversion of syngas and benzene.
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ACS Sustainable Chemistry & Engineering
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2021
·
IF 8.198
Wen Li,Kuncan Wang,Guowu Zhan,Jiale Huang,Qingbiao Li
Transformation of CO2 with the help of green hydrogen (prepared from renewable energy) into valuable light olefins (C2=–C4=) is a promising route for utilizing the carbon resource in CO2. Currently, most of the reported bifunctional catalysts for CO2 hydrogenation to light olefins follow a methanol-mediated route that adopts SAPO-34 as the zeolite component. Although ZSM-5 has been widely used in the methanol to propylene process using fixed bed reactors due to high shape-selective property and long lifetime, ZSM-5-based bifunctional catalysts have seldomly been used for CO2 hydrogenation to light olefins. Herein, we proposed a novel synthetic strategy for bio-ZSM-5 with mild acid strength and relatively low acid density using the natural rice husk as a template. The bio-ZSM-5 was integrated with ZnZrOx solid solution nanoparticles, and the derived ZnZrOx&bio-ZSM-5 catalysts exhibited a high C2=–C4= selectivity of 64.4% and total C2–C4 selectivity of 94.5%, but relatively low CH4 selectivity (5.5%) and aromatic selectivity (<1%). The post-modified ZnZrOx&bio-ZSM-5 catalysts further enhanced the catalytic stability with less coke deposition and regulated the ethylene to propylene ratio in light olefin distribution. Furthermore, *CHxO was found to be the key intermediate formed on the ZnZrOx surface and was transferred to the Brønsted acid sites in the bio-ZSM-5 for the subsequent conversion to light olefins, as confirmed by in situ DRIFTS and chemical trapping mass spectrometry.
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ENERGY & FUELS
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2020
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IF 3.421
Yang Qu,Yuan Zhao,Shanshan Xiong,Chenguang Wang,Shurong Wang,Lingjun Zhu,Longlong Ma
5-Hydroxymethylfurfural (HMF) and levulinic acid (LA) are two important platform compounds that can be produced by the dehydration of hexoses from hydrolysis of cellulose. In this study, glucose dehydration was catalyzed by the SO42–/ZrO2 catalyst in the NaCl–THF/H2O biphasic solvent system. Complete conversion of glucose was achieved at 160 °C. The highest HMF yield and LA yield were 61.84% and 29.68%, respectively. The results showed that the conversion and product distribution were influenced by catalyst acidity, solvent composition, temperature, and time. The SO42– load greatly changed the acidity of the catalyst, thus affecting the product distribution. By changing the composition of the catalyst and the biphasic solvent system, different yields of HMF and LA could be obtained, so as to realize directional synthesis of the target products.
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ACS Applied Materials & Interfaces
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2020
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IF 8.758
Peng Jiang,Yang He,Yiping Zhao,Li Chen
Patients with end-stage renal disease are prone to developing a complication of hyperhomocysteinemia, manifesting as an elevation of the homocysteine (Hcy) concentration in human plasma. However, Hcy as a protein-bound toxin is barely removed by conventional hemodialysis membranes. Here, we report a novel hemodialysis membrane by preparing a bioactive coating of pyridoxal 5′-phosphate (PLP) and adding biocompatible hyperbranched polyglycerol (HPG) brushes to achieve Hcy removal. The dip-applied PLP coating, a coenzyme with a role in Hcy metabolism, dramatically promoted a decrease in the Hcy concentration in human plasma. Moreover, the aldehyde group of PLP had an intrinsic chemical reactivity toward the terminal amino group to immobilize the HPG brushes on the hemodialysis membrane surface. The hierarchical PLP–HPG layer-functionalized membranes had a high efficacy for eliminating Hcy, with a concentration from the initial stage of 150 μmol/L reduced to a nearly normal level of 20 μmol/L in simulated dialysis. By analyzing the impact of HPG brushes with various chain lengths, we found that HPG brushes with a medium length enabled the PLP coating with the bioactive function of Hcy conversion to additionally protect Hcy-attacked target cells by providing excellent hydrophilicity and a dense enough chain volume overlap of the hyperbranched architecture. Simultaneously, the densely packed HPG brushes generated a maximal steric and hydration barrier that significantly improved biofouling resistance against blood proteins. The optimally functionalized membranes showed a clearance of 83.1% urea and 49.6% lysozyme and a rejection of 96.0% bovine serum albumin. The diversely functionalized PLP–HPG layers demonstrate a potential route for a more integrated hemodialysis membrane that can cope with the urgent issue of hyperhomocysteinemia in clinical hemodialysis therapy.
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PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2020
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IF 6.785
Dexin Du,Jiangnan Shu,Mingquan Guo,Mohammad A. Haghighatbin,Di Yang,Zhiping Bian,Hua Cui
Recently, nanoluminophores with the potential-resolved multicolor electrochemiluminescence (PRMCECL) property have emerged and shown promising applications in sensitive, selective, and accurate bioassays, bioimaging, and multicolor emitting devices. However, only limited PRMCECL nanoluminophores and their applications in ratiometric biosensors eliminating proportional errors have been reported. Herein, a novel PRMCECL nanoluminophore was synthesized by encapsulating CdS quantum dots (CdSQDs) into MOF-5 (CdSQDs@MOF-5). Using K2S2O8 as a coreactant, two electrochemiluminescence (ECL) peaks, ECL-1 centered at 685 nm and ECL-2 centered at 475 nm, were observed at −1.4 and −1.8 V, respectively. Related ECL mechanisms have been proposed. Based on the potential-resolved ECL signals, a label-free differential ECL immunosensor for the determination of cardiac troponin I (cTnI) was established by assembly of poly(diallyldimethylammonium chloride), CdSQDs@MOF-5, and cTnI antibody-functionalized silver nanoparticles on the surface of the fluorine-doped tin oxide electrode subsequently. In the presence of cTnI, cTnI was captured by the sensing interface, leading to an increase in ECL-1 and ECL-2 intensity. cTnI could be determined in the range of 0.01–1000 pg/mL with a detection limit of 5.01 fg/mL using the intensity difference between ECL-1 and ECL-2. This work provides a new family member of PRMCECL nanoluminophores. The proposed label-free differential ECL immunosensor provides a new strategy based on potential-resolved ECL signals, which could effectively eliminate the additive error and show better sensitivity, selectivity, and accuracy for the detection of cTnI than the single-signal strategy and ratiometric strategy.
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JOURNAL OF THE CHINESE CHEMICAL SOCIETY
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2020
·Vol. 68
·期 4
·582-591
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IF 1.554
Changzhou Chen,Peng Liu,Haihong Xia,Minghao Zhou,Jianchun Jiang
There is an urgent need to develop a selective hydrogenolysis of C aryl -O bonds in lignin to produce valued-added chemicals and fuels. Recently, hydrogen has been used in the hydrogenation reaction, which hides inevitable danger and is not economical. Therefore, isopropanol, as a hydrogen-donor solvent, is employed for aryl ether hydrogenolysis in lignin models over nickel supported on a carbon nanotube (CNT). Except for aromatic ether (4-O-5), the Ni/CNT catalyst is also found to be suitable for alkyl-aryl ether (α-O-4 and β-O-4) cleavage in control experiments. The physicochemical characterizations were carried out by means of H 2 -temperature-programmed reduction, X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy analyses. The catalyst can be magnetically recovered and efficiently reused for five consecutive recycling tests in the transfer hydrogenation of aromatic ethers. A mechanism study indicated that the hydrogenolysis cleavage of the ether bond is the first step in the reaction process, and hydrogenation of aromatic rings is only a successive step in which phenol and benzene are intermediate states and are then further hydrogenated. Furthermore, it has been demonstrated that aryl groups play an important role in the hydrogenation of phenol in the competitive catalytic hydrogenation reaction of phenol.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Dandan Jia,Ruoyan Tong,Liangmin Ning,Zewen Yang,Yuting Zhang,Wen Gu,Xin Liu
Graphite anode (specific capacity is only 372 mA h g −1 ) for lithium-ion batteries (LIBs) is not enough for high energy and high power density demands. In this work, MOF-5 was used as a precursor to prepare a porous carbon material embedded with BN (Boron Nitride), while B and N elements will enhance the electron transport speed thus improving the conductivity simultaneously. A large specific surface area of 1790.19 m 2 g −1 was provided with this material because of embedding of lamellar BN, therefore it caused excellent cycling stability and high capacity characteristics in LIBs. The capacity retention is 1290 mA h g −1 at 200 mA g −1 and 683 mA h g −1 at 2000 mA g −1 . This material provides a solution for improving the performance of LIBs, and it can also be a reference for the development in other fields.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Wen Li,Kuncan Wang,Guowu Zhan,Jiale Huang,Qingbiao Li
The chemical transformation of CO2 to value-added chemicals and fuels remains a daunting research challenge, requiring the development of more efficient catalysts. The present work offers highly active integrated nanocatalysts for CO2 hydrogenation to dimethyl ether (DME) through tandem catalysis, that is, Pd/ZnO converts CO2 to methanol, and bio-ZSM-5 further catalyzes methanol dehydration to DME. Notably, the hierarchically porous bio-ZSM-5 with high pore connectivity was prepared by using low-cost rice husk and luffa sponge as biotemplates. The formation of bio-ZSM-5 involved three consecutive steps, including (i) diffusion of precursor species, (ii) confined crystal growth, and (iii) calcination treatment to remove the residual biomass. Interestingly, the obtained bio-ZSM-5 possesses abundant hierarchical porosity, including the intrinsic micropores from ZSM-5 frameworks, the mesopores from intracrystalline void space or pinholes in the intergrown zeolite layers, and the macroscopic channels from the original biomass architecture. It was found that the tetrapropylammonium hydroxide amount and Si/Al ratio were two critical factors affecting the crystallinity and porosity of the bio-ZSM-5. The silicon content in biomass (8.3 wt % in rice husk and 0.016 wt % in luffa sponge) also played a crucial role in the synthesis of bio-ZSM-5. Different spatial configurations of Pd/ZnO and bio-ZSM-5 significantly affected the DME yield, wherein spatial distances between the bio-ZSM-5 and Pd/ZnO components were adjusted by controlling the size of Pd/ZnO or the integration manners. The current results indicated that the closest proximity of the bifunctional catalyst was unfavorable for DME production (selectivity < 3%), because of which low-valent Zn cations from Pd/ZnO could displace the Brønsted acid sites on bio-ZSM-5 by ion exchange, and the powder mixing in the mortar was the best combination configuration of Pd/ZnO and bio-ZSM-5, promoting the CO2 conversion (10.8%) with a DME selectivity of 31% under the reaction of 300 °C and 30 bar. Furthermore, as compared to the traditional ZSM-5 based catalyst, the obtained Pd/ZnO/bio-ZSM-5 bifunctional catalysts showed excellent long-term stability in 60 h on stream with a less amount of coke formed in the spent catalysts.
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INDUSTRIAL CROPS AND PRODUCTS
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2020
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IF 4.244
Yu Yin,Chunhui Ma,Wei Li,Sha Luo,Yushan Liu,Xueyun Wu,Zhenwei Wu,Shouxin Liu
The efficient conversion of glucose to 5-hydroxymethylfurfural (5-HMF) in ionic liquids with MoCl 3 as catalyst under microwave irradiation was demonstrated. Based on 5-HMF yield, the ionic liquid 1-butyl-3-methylimidazolium chloride ([BMIM]Cl) was the best solvent. The results showed that compared to conventional oil-bath heating, microwave irradiation not only reduced the required reaction time from hours to minutes, but also improved the 5-HMF yield. Using 10 mol% of the catalyst, the 5-HMF yield reached 20.61 % at 120 °C after 2.5 h with the oil-bath. However, a 5-HMF yield of 27.66 % could be achieved within 5 min when employing 300 W microwave irradiation. Analyses by nuclear magnetic resonance spectroscopy (NMR) and high-performance liquid chromatography–mass spectrometry (HPLC-MS) demonstrated that the coordinate bond interaction between MoCl 3 /[BMIM]Cl complex and glucose promoted the isomerism of glucose and the dehydration of fructose. Microwave irradiation was also shown to accelerate the bond breaking processes in the reaction.
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ACS Omega
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2020
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IF 2.87
Li Wang,Shengxian Liu,Wenjing Du,Tongyi Dou,Changhai Liang
5-Cyanovaleramide (5-CVAM) is an important intermediate of a herbicide and chemical raw material. Herein, we found a novel nitrile hydratase from the strain Rhodococcus erythropolis CCM2595, exhibiting high regioselectivity with higher substrate specificity toward dinitriles than mononitriles. In the past, the strain was shown to degrade only phenol, hydroxybenzoate, p-chlorophenol, aniline, and other aromatic compounds. In our study, 20 mM adiponitrile was completely consumed within 10 min with 95% selectivity to 5-CVAM and 5% selectivity to adipamide. In addition to its high regioselectivity, our recombinant Escherichia coli showed a higher substrate tolerance of up to 200 mM adiponitrile even after 3 h when compared with two reported strains with their cyano-tolerance concentrations of up to 100 mM, which is considered to be the highest cyano-tolerance. Such a robust biocatalyst is a desirable attribute of a biocatalyst intended for use in commercial applications of 5-CVAM.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yunpu Wang,Linyao Ke,Yujie Peng,Qi Yang,Yuhuan Liu,Qiuhao Wu,Yujie Tang,Haibin Zhu,Leilei Dai,Zihong Zeng,Lin Jiang,Roger Ruan
In view of the poor selectivity of aromatic hydrocarbons in bio-oil from biomass pyrolysis and the high pressure drop and rapid coking and deactivation of catalyst in industrial scale, a microwave-driven HZSM-5@SiC ceramic foam has been constructed, and applied to the ex-situ catalytic fast pyrolysis of soapstock to improve the content of aromatic hydrocarbons in bio-oil. The effects of different catalysts and heating modes and mass ratios of HZSM-5@SiC ceramic foam to soapstock on the distribution of pyrolysis products have been investigated. In addition, combined with the comparison of microwave and electric heating, the deactivation characteristics of HZSM-5@SiC ceramic foam have been studied. Finally, the process of preparing aromatic oil by microwave-driven catalytic pyrolysis of soapstock was discussed. Experimental results indicate that compared with HZSM-5, HZSM-5@SiC ceramic foam has a higher yield of bio-oil and higher aromatization activity. Under microwave heating, the relative content of aromatic hydrocarbons increases from 25.18% to 100% when the mass ratio of HZSM-5@SiC ceramic foam to soapstock increases from 0:1 to 1:1. Compared with electric heating catalysis, HZSM-5@SiC ceramic foam has the lowest yield of coke under microwave heating. After five consecutive uses, it still maintains more than 90% catalytic activity and has higher stability, which provides a scientific basis for the pilot scale experiments of soapstock catalytic pyrolysis.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Ying-Bo Zhu,Jia Guo,Yu-Long Ma,Yuan-Yuan Li
The production of high-value-added chemicals from the degradation of real lignin still has been an unresolved issue. In this study, a two-step strategy was proposed to obtain n-hexanol from alkali lignin, and high conversion of alkali lignin and selectivity of n-hexanol were achieved. The deoxygenation performance of the synthesized Ni-HZSM-5 catalyst, modified by Ca, was efficiently improved. At first, through the deoxygenation of alkali lignin via Ni/CaO-HZSM-5, the C–O bonds of the material were broken effectively and 44% degree of deoxygenation (DOD) was obtained. Second, n-hexanol was selectively produced over the Ni/HZSM-5 catalyst from the liquid product obtained by the first step. The efficiency of deoxygenation (DOD) was attained at 71%, and the heat value increased to 51.6 MJ/kg from 19.9 MJ/kg after the two-step strategy. This strategy showed a high catalytic effect to produce n-hexanol from alkali lignin using Ni/CaO-HZSM-5 and Ni/HZSM-5 catalysts and revealed a superior advantage in the hydrodeoxygenation of real lignin to form high additional value chemicals.
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