ACS Sustainable Chemistry & Engineering
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2020
·
IF 7.632
Tao Gan,Yifei Liu,Qian He,Hao Zhang,Xiaohui He,Hongbing Ji
Catalytic conversion of biomass-derived 5-hydroxymethylfurfural (HMF) into high-quality biofuel 2,5-dimethylfuran (DMF) is significant for the utilization of biomass but remains a substantial challenge. Herein, we report a straightforward, eco-friendly, and scalable ball milling method for the synthesis of Co-alloyed Pt (Pt1/Co) single-atom alloy (SAA) catalysts at kilogram levels. The catalysts exhibit superior catalytic performance for the hydrodeoxygenation of HMF to DMF, obtaining 100% HMF conversion and 92.9% selectivity to DMF under 1.0 MPa H2 at 180 °C for 2 h. The reaction pathway is also investigated, which shows that the hydrogenolysis of the C═O bond in HMF to form 2,5-dihydroxymethylfuran is the main route during the hydrodeoxygenation and promoted by the synergistic effect of Pt and Co. Pt1/Co SAA catalysts display excellent stability without aggregation after five successive runs. More inspiringly, our method achieves the mass production of Pt1/Co at the kilogram scale, rendering its potential for practical applications. Moreover, by varying acetylacetonate precursors, we show the general synthesis of different Co-supported noble metal SAA catalysts (M1/Co, M = Pd, Ru, Ir, and Rh). Our findings not only offer a facile and readily scalable synthetic approach of SAA catalysts but also open new avenue to the exploitation of biomass.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Heng Ban,Youdi Zhang,Shuaibo Chen,Youwei Cheng,Teng Pan,Lijun Wang,Xi Li
In this contribution, readily available 5-methyl furfural (MF) derived from biomass was used as an excellent substitute of the chemically unstable 5-hydroxymethylfurfural (HMF) for preparing the commercial precursor 2,5-furandicarboxylic acid (FDCA). MF was catalytically oxidized by air into FDCA in acetic acid over homogeneous Co/Mn/Br catalysts at 130–170 °C. It was found that both the substitute reactivity and the ring chemical stability have a remarkable impact on the yield of aromatic dicarboxylic acids. The effects of reaction temperature, pressure, catalyst composition and concentration, water concentration in the solvent, and substrate/solvent mass ratio on both the main reaction and the side reaction were investigated systematically and thoroughly using HPLC and an online tail gas monitoring system. Under optimized conditions, the oxidation of MF gave 100% conversion of MF and 75.8% yield of FDCA with 99.6% purity. It was also proven that the addition of 200 ppm cerium could work well at low temperatures (130–140 °C) for enhancing FDCA selectivity via suppressing the side reactions.
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RSC Advances
·
2020
·Vol. 10
·期 37
·22126-22136
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IF 3.119
Hongchang Yu,Fuwei Li,Wen He,Caifeng Song,Yansong Zhang,Zhixia Li,Hongfei Lin
Micro–mesoporous ZSM-5 with different Si/Al ratios (MZ-X, X = 27, 80, 150) were synthesized by adding microcrystalline cellulose (MCC) as co-template into the hydrothermal synthesis process of zeolites. The resultant ZSM-5 were used for catalytic cracking of high density polyethylene (HPDE) and polypropylene. It was found that introduction of MCC significantly enhanced the formation of mesopores and strong acid sites. MZ-27 achieved the highest oil yield: 21.5% for HPDE and 32.1% for polypropylene, and the light aromatics (BTEX) selectivity therein were 87.6% and 79.7%, respectively. HZ-150 (MCC-free ZSM-5, Si/Al = 150) achieved the highest gas yield: 85.4% for HDPE and 76.7% for polypropylene, and the light olefins (C2–4) selectivity therein were 44% and 48.3%, respectively. The dense acidic sites and mesoporous structure of MZ-27 were responsible for its better activity for producing aromatic products. The moderate acidity and microporous structure of HZ-150 were helpful for producing light olefins from catalytic cracking of polyolefin plastics.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Xuemei Li,Junying Tian,Hailong Liu,Congkui Tang,Chungu Xia,Jing Chen,Zhiwei Huang
A highly efficient and green process was developed for the synthesis of useful 5-amino-1-pentanol (5-AP) from biomass-derived dihydropyran by coupling the in situ generation of 5-hydroxypentanal (5-HP, via the ring-opening tautomerization of 2-hydroxytetrahydropyran (2-HTHP)) and its reductive amination over supported Ni catalysts. The catalytic performances of the supported Ni catalysts on different oxides including SiO 2 , TiO 2 , ZrO 2 , γ-Al 2 O 3 , and MgO as well as several commercial hydrogenation catalysts were investigated. The Ni/ZrO 2 catalyst presented the highest 5-AP yield. The characterization results of the oxide-supported Ni catalysts showed that the Ni/ZrO 2 catalyst possessed high reducibility and a high surface acid density, which lead to the enhanced activity and selectivity of the catalyst. The effect of reaction parameters on the catalytic performance of the Ni/ZrO 2 catalyst was studied, and a high 5-AP yield of 90.8% was achieved in the reductive amination of 2-HTHP aqueous solution under mild conditions of 80 °C and 2 MPa H 2 . The stability of the Ni/ZrO 2 catalyst was studied using a continuous flow reactor, and only a slight decrease in the 5-AP yield was observed after a 90-h time-on-stream. Additionally, the reaction pathways for the reductive amination of 2-HTHP to synthesize 5-AP were proposed.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2020
·
IF 2.627
Xianfeng Liu,Fu Yang,Shuying Gao,Bo Shao,Shijian Zhou,Yan Kong
Design and synthesis of low cost and efficacious industrial catalyst for the oxidation of styrene has been an important research project. Herein, ZSM-5 zeolite containing tetrahedral vanadium (V) and Brønsted acid sites (V-H-ZSM-5) was prepared, and identified by characterizations such as XRD, SEM, UV–vis, NH 3 -TPD, H 2 -TPR N 2 -adsorption/desorption and FTIR. V-H-ZSM-5 performed extremely enhanced catalytic activity for the oxidation of styrene with 30% H 2 O 2 at 40 °C. Moreover, in-situ FTIR spectrum was used to investigate the catalytic mechanism. The results demonstrate that Brønsted acid site could not only increase the adsorption concentration of styrene in the micropores of V-H-ZSM-5 via the π complex interaction between double bond of styrene and Brønsted acid sites, but also increase the oxidation potential of H 2 O 2 . The synergetic action of tetrahedral vanadium (V) and Brønsted acid enhanced the catalytic activity for the oxidation of styrene with 30% H 2 O 2 . Impressively, V-H-ZSM-5 performed high reusability within five runs at a low reaction temperature (40 °C) for the first time.
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APPLIED CATALYSIS A-GENERAL
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2021
·
IF 5.706
Xiaochao Xian,Mengjun He,Yakai Gao,Yi Bi,Yirong Chu,Jun Chen,Lichun Dong,Jin Wang,Shuo Zhao
Reducing the acid density and strength of HZSM-5 zeolite are typical strategies to inhibit coke deposition during catalytic cracking reactions. Herein, direct titration of HZSM-5/H 2 O suspension using dilute NaOH aqueous solution at room temperature was introduced to neutralize excessive Brønsted acid sites of HZSM-5 zeolite (Si/Al = 25). SEM, XRD, N 2 adsorption and n -propylamine temperature-programmed decomposition confirmed that simultaneous acid strength weakening and acid density reducing were achieved without obvious influence on crystalline or textural property. The evolution of the surface charge during the titration process tracked by Zeta-potential measurement reveals that the mechanism of such neutralization is: liquid phase neutralization between H + and OH − & solid phase ion exchange between Na + and H + . Supercritical catalytic cracking of n -dodecane over a series of partial neutralized HZSM-5 catalysts showed that moderate neutralization can enhance the conversion of n -dodecane by alleviating both the coke amount and harmfulness per unit mass of coke.
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CHEMOSPHERE
·
2021
·
IF 7.086
Wanyi Huang,Yixing Yuan,Dan Zhong,Wencheng Ma,Yuan Yuan,Peng Zhang
In this study, we investigated the use of pipe growth rings from water distribution networks as a catalyst in heterogeneous Fenton-like oxidation processes. The major constituents of real pipe growth rings (α- and γ-FeOOH) were prepared and considered as a simulated growth ring (SGR). Its performance in removing 5-bromosalicylic acid (5-BSA), a novel phenolic halogenated disinfection byproduct , was examined. SGR exhibited strong catalytic ability and a certain degree of adsorption capacity. Under acidic conditions, the adsorption and oxidation efficiencies were 32.65% and 87.67%, respectively. Furthermore, 72.19% of 5-BSA could be oxidized even at pH 0 of 7. Kinetic characterizations at various temperatures revealed that both the adsorption and catalytic oxidation processes followed pseudo-second-order kinetic models and were surface-controlled with high activation energies (31.26 and 23.58 kJ mol −1 , respectively). Ecotoxicity analyses of the transformation products (TPs) showed that the SGR/H 2 O 2 system could effectively reduce the toxicity of 5-BSA. Moreover, the number of iron ions leaching from SGR was below 0.1 mg L −1 in all experiments. The results of this study support further investigation of using real pipe growth rings in off-line water treatment , as well water network contamination remediation.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2021
·
IF 2.694
Yang Cong,Cunbin Du,Meng Wang,Zhouyu Jiang,Mingliang Wang
In this work, the phase equilibrium solubility of 5-fluorocytosine (5-FC) in dimethyl sulfoxide (DMSO), N,N-dimethylformamide (DMF), 1-butanol, acetonitrile, 1-propanol, 1,4-dioxane, acetone, ethyl acetate, 2-propanol, 2-butanone, and mixture systems (DMSO + 2-propanol and DMF + 2-propanol) at a series of temperatures (283.15–323.15 K) is determined, and model correlation, solvent effect, and preferential solvation analysis are researched. The solubility of 5-FC is related to temperature, which decreases with decreasing temperature. For monosolvent systems, the mole solubility order is DMSO > DMF > 1-butanol > 1-propanol > 2-propanol > acetone > 2-butanone > 1,4-dioxane > acetonitrile > ethyl acetate. The solvent effect has been studied in monosolvents, hydrogen-bonding acceptor (HBA) interactions and nonspecific dipolarity/polarizability interactions favor dissolution, and solvent self-cohesiveness is not beneficial to dissolution. For two mixture systems, the mole solubility of 5-FC in DMSO + 2-propanol solvent systems is higher than that in DMF + 2-propanol solvent systems. A dimensionless parameter (δ) is defined to observe the deviation from ideality of mixed solvents whose values are all greater than zero. The equilibrium constant of the solvent exchange process (Kps) can be used to evaluate the preferential solvation of 5-FC. DMSO or DMF dissolves 5-FC in the local region around 5-FC preferentially. The equilibrium solubility data is correlated by four correlation models (modified Apelblat, λh, CNIBS/R-K, and Jouyban–Acree models). The greatest relative average deviation (RAD) and root-mean-square deviation (RMSD) values are 2.01% and 11.87 × 10–5 in pure solvent systems and 2.20% and 5.99 × 10–5 in mixture systems, respectively. These four models show excellent correlation with the experimental solubility data.
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NEUROPHARMACOLOGY
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2021
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IF 5.251
Mengwen Shi,Jiaxin Tang,Chengmei Yang,Guanlong Guo,Huaxing Ou,Weihai Chen
Prepulse inhibition (PPI) is disrupted in many neuropsychiatric diseases. Although the inverse agonist of the 5-hydroxytryptamine 2A (5-HT 2A ) receptors, pimavanserin , alleviates PPI deficits in rodents, the precise mechanisms and critical brain areas in the reversal effect of 5-HT 2A receptor inverse agonists remain unclear. The present study aimed to investigate the critical brain areas responsible for the reversal effect of the 5-HT 2A receptor inverse agonist on PPI deficits in male mice. The results showed that intraperitoneal administration of pimavanserin was found to improve normal PPI behavior and reverse PPI deficits elicited by the dopamine D 1 /D 2 receptor nonselective agonist, pergolide . Further, local infusion of pimavanserin into the nucleus accumbens and ventral hippocampus reversed PPI deficits, whereas the same manipulation in the medial prefrontal cortex or ventral tegmental area did not reverse PPI deficits. Overall, the nucleus accumbens and ventral hippocampus are the critical brain areas responsible for the reversal effect of 5-HT 2A inverse agonists on PPI deficits. Such findings contribute to the extensive exploration of the accurate molecular and neural mechanisms underlying the antipsychotic effects of 5-HT 2A receptor inverse agonists, especially the neural circuits modulated by 5-HT 2A receptor activity.
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ENERGY & FUELS
·
2021
·
IF 3.605
Xiangbo Song,Yuhe Liao,Yuting Zhu,Pengyao Sun,Lungang Chen,Longlong Ma,Hongwei Yang,Chenguang Wang
Highly effective production of 5-hydroxymethylfurfural (HMF) from biobased sugar is one of the vital steps for the synthesis of a fuel precursor. In this work, a slow-release effect of proton from a heterogeneous catalyst induced by 1-butyl-3-methylimidazole chloride ([Bmim]Cl) ionic liquids was found and employed to effectively convert biobased fructose to HMF. Under mild conditions of 100 °C and 60 min, a promising HMF yield of 94.6% with a fructose conversion of 99.1% could be achieved in a tetrahydrofuran solvent over the synergy of Amberlyst-15 with [Bmim]Cl, owing to the slow-release effect. Based on extensive control experiments and characterizations, a mechanism of slow release of proton induced by [Bmim]Cl was proposed to better understand the catalytic performance, mainly involving that proton in the −SO3H group of Amberlyst-15 was gradually replaced by the [Bmim]+ of the [Bmim]Cl additive. Additionally, the effect of various parameters (e.g., different ionic liquids and solvents, the loading of the ionic liquid and catalyst, and reaction temperature and time) was systematically investigated. Meanwhile, the stability of Amberlyst-15 and [Bmim]Cl was tested; both could be reused four times. This work provides a novel and highly effective strategy for conversion of biomass-based feedstock toward fuel precursors.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 24
·7034-7044
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IF 5.726
Liwei Zhang,Huaike Zhang,Zhiqiang Chen,Qiang Ning,Suyao Liu,Jie Ren,Xiaodong Wen,Yong-Wang Li
To correlate the relationship between the Al distribution and the catalytic performance of long-chain olefin aromatization, several ZSM-5 zeolites with different Al locations and proximities were prepared via adjusting the hydrothermal synthesis conditions. Characterization by XRD, SEM and N2-adsorption indicated that all the as-prepared ZSM-5 zeolites exhibited high crystallinities, uniform morphologies and open channels. However, a great difference in the framework Al (AlF) positions was observed by 27Al MAS NMR and UV-vis-DRS of Co(II) ions, thus leading to the distinct acidity of various zeolites as determined by NH3-TPD and Py-IR. In 1-octene aromatization reaction, ZSM-5 catalysts exhibited significantly different catalytic performances and reaction pathways, which were closely related to the types and locations of the AlF atoms. The ZSM-5 zeolite catalyst with the most abundant single Al sites exhibited the lowest aromatics selectivity, while Al pairs in the framework were more favorable to the formation of aromatics. Moreover, the product distribution revealed that the Al pairs in the channel intersections of the ZSM-5 zeolite were responsible for the improved selectivity to heavy aromatics due to the fewer space restrictions; however, the Al pairs in the sinusoidal and straight channels with severe size restrictions suppressed the generation of bigger aromatics on the Al sites. This result provided a new potential method for precisely tailoring the catalytic selectivity in olefin conversion and upgrading the Fischer–Tropsch oil.
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Journal of Central South University
·
2020
·Vol. 26
·期 11
·2974-2986
·
IF 1.249
Xu Si-quan,Pan Dong-hui,Xiao Guo-min
With the aim of achieving a high 5-hydroxymethylfurfural (HMF) yield from glucose with H-ZSM-5 catalyst at low cost, three inexpensive biphasic reaction systems, H 2 O—tetrahydrofuran (THF), H 2 O—2-methyltetrahydrofuran (MeTHF) and H 2 O’2-butanol, were discovered and proved to be particularly effective in promoting the formation of HMF from glucose over H-ZSM-5 zeolite. In order to determine the optimal process conditions, the effects of various experimental variables, such as reaction temperature, reaction time, catalyst dosage, volume of organic solvent, as well as inorganic salt type on glucose conversion to HMF in three systems were investigated in detail. It was found that under optimal reaction conditions, H 2 O—THF, H 2 O—2-butanol and H 2 O—MeTHF allowed the glucose dehydration process to achieve HMF yields of up to 61%, 59%, and 50%, respectively. Moreover, in the three biphasic systems, the H-ZSM-5 catalyst was also demonstrated to maintain excellent stability. Thus, the catalytic approach proposed in this paper can be believed to have potential prospects for industrially efficient and low-cost production of HMF.
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危险品化学品经营许可证（带存储）