Materials Today Nano
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2023
·
IF 10.3
R. Zhang,F. Gao,C. Yang,Y. Bian,G. Wang,K. Xue,J. Zhang,C. Wang,X. Gao
Coupling electrocatalytic 5-hydroxymethylfurfural (HMF) oxidation reaction (HMFOR) with hydrogen evolution reaction (HER) is capable of potentially enhancing energy efficiency for hydrogen production and converting biomass into high-valued products. Herein, a novel metallic heterostructure based on Ni 3 S 2 and Co 9 S 8 (Co 9 S 8 @Ni 3 S 2 /NF) was designed for H 2 production and selective oxidation of HMF into 2, 5-furandicarboxylic acid (FDCA). Benefiting from the merit of metal heterojunction, Co 9 S 8 @Ni 3 S 2 /NF not only possesses appropriate H∗ adsorption energy , but also promotes the adsorption and desorption process of organic, thus making reaction dynamics for both HER and HMFOR more exceptional. Furthermore, the anion exchange membrane (AEM) electrolyzer with Co 9 S 8 @Ni 3 S 2 /NF as anode and cathode electrodes toward HMFOR and HER only required a low potential of 1.61 V for continuous hydrogen and FDCA production at the initial current density of 50 mA/cm 2 . The generation rate of H 2 and FDCA are as high as 45.6 L/h/m 2 and 7.25 mg/h/cm 2 , corresponding to the Faraday efficiency of ∼100% and 93.0%, respectively. The in-situ Raman and theoretical calculations demonstrated that the electron transfer from Ni 3 S 2 to Co 9 S 8 at heterogeneous interface contributes to the formation of Ni/Co–OOH, which is the active species of HMFOR.
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FUEL
·
2022
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IF 8.035
Fuwei Li,Xiaofeng Wang,Hengshuo Gu,Hongbing Fu,Asad Ali,Hongfei Lin,Zhixia Li
Minimizing the catalyst cost is critical to achieving long-term economic feasibility for obtaining bio-chemicals directly from biomass. In the present study, low cost ZSM-5 was synthesized via hydrothermal crystallization of the activated aluminosilicate gel without adding any organic ammonium templates and additional seed crystals . The activation process promoted the depolymerization of the silica-alumina species and the formation of active pasty gel containing nucleation precursors, consequently accelerating the subsequent crystallization reaction. The addition of eucalyptus sawdust (ES) in the synthesis process increased the BET (Brunauer-Emmett-Teller) surface area and acidity of the resultant zeolites . The ES-mediated ZSM-5 (AGZ-10) achieved a higher benzene, toluene, ethylbenzene and xylene (BTEX) carbon yield (18.9 %) from co-cracking of ES and waste plastics (WP) (ES/WP mass ratio at 1:1) at 500 °C and exhibited better synergistic effect and anti-coking ability compared to the commercial ZSM-5. The results provide an efficient synthetic strategy to produce low-cost zeolites, and a promising technique to effectively utilize biomass and plastic wastes.
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Processes
·
2022
·Vol. 10
·期 10
·1970
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IF 3.352
Xuan Zhou,Hongling Pan,Shuixiang Xie,Guotao Li,Zhicai Du,Xiang Wang,Yan Luo
The aim of this research is to design and synthesize an efficient catalyst to enhance high value-added products, such as aromatic hydrocarbons and phenols, from the catalytic fast pyrolysis (CFP) of different types of forestry and agricultural residues. All three biomasses (rape straw, wheat straw, and bamboo powder) had no aromatic production via thermal pyrolysis alone; however, the aromatic selectivity and monocyclic aromatic selectivity were largely enhanced using ZSM-5, with suitable silica-alumina ratios and Ni loadings. Specifically, for rape straw, the optimum catalyst was 15 wt.% Ni/ZSM-5 (silica-aluminum ratios = 85), and the selectivity of aromatic hydrocarbons was achieved at 39%, of which 71% were monocyclic aromatic hydrocarbons. For wheat straw, the optimum catalyst was 10 wt.% Ni/ZSM-5 (silica-aluminum ratios = 18), and the selectivity of aromatic hydrocarbons was 67%, of which 55% were monocyclic aromatic hydrocarbons. For bamboo powder, the optimum catalyst was 10 wt.% Ni/ZSM-5 (silica-aluminum ratios = 18), and the selectivity of aromatic hydrocarbons was achieved at 21%, of which 80% were monocyclic aromatic hydrocarbons. Meanwhile, biomass types have significant effects on the pyrolyzed product distribution due to their different components. Cellulose and hemicellulose promoted the production of aromatic hydrocarbons, while lignin enhanced the production of phenols. The promotion of phenol by Ni was better and more efficient than that by the molecular sieve.Keywords:catalytic fast pyrolysis;forestry and agricultural residues;Ni/ZSM-5;aromatic hydrocarbons;phenols;Py-GC/MS
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 8
·2504-2516
·
IF 2.936
Chen Jiaxuan,Hu Shen,Chen Zhuo,Sun Xincheng,Chen Minhao,Chen Tianjiao,Ye Guanghua,Zhou Xinggui
The effects of molecular size on SiO 2 deposition regulated surface barriers and zeolite catalysis are probed, taking n -pentane isomerization and benzene alkylation with ethylene as model reactions. Chemical liquid deposition of SiO 2 on the parent ZSM-5 sample only modifies its external surface slightly and passivates a small proportion of Brønsted acid sites. The apparent diffusivities increase significantly at 363–393K after SiO 2 deposition, indicating SiO 2 on ZSM-5 crystals reduces surface barriers at low temperatures. The conversion for n -pentane isomerization increases by up to 26% after SiO 2 deposition, while the conversion for benzene alkylation decreases by up to 19%. Obviously, the positive effect of SiO 2 deposition can be balanced out by the pore confinement effect at high temperatures, which is stronger for a larger molecule. This work provides a unique understanding of molecular size effects on surface barriers, which should serve to guide the design of zeolite catalysts. Graphical Abstract
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JOURNAL OF POLYMER RESEARCH
·
2022
·Vol. 29
·期 10
·1-9
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IF 3.061
Huangfu Fei,Li Wanrong,Yang Zhongqiang,You Jiang,Yang Po
This work aims to explore the bulk ring-opening metathesis copolymerization of dicyclopentadiene and 5-ethylidene-2-norbornene by modifying the comonomer feed ratios. Thorough studies showed that their performance can be enhanced by polymerization at elevated temperature and there was a little deviation of properties from mixing rules. That is, the copolymers properties depend on monomer composition and can be roughly predicted by empirical mixing rules. We believe this can help researchers design and prepare ROMP derived polydicyclopentadiene copolymers and apply them in more applications.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Yingshu Liu,Haiyang Tao,Xiong Yang,Xiaoyong Wu,Jinjuan Li,Chuanzhao Zhang,Ralph T. Yang,Ziyi Li
Adsorption is a promising technology for capturing nitrogen oxides (NO x ) from humid flue gases , for which as the preferred NO x adsorbent, zeolite with an appropriate silica to alumina (Si/Al) ratio provides the key step for success in practical applications. In this work, the effects of Si/Al ratio, temperature, relative humidity (RH), and feed gas (NO x -H 2 O(g)–CO 2 –O 2 -N 2 ) compositions on NO x sorption behavior on HZSM-5 zeolites were systematically investigated, based on a series of characterizations, fixed-bed adsorption and temperature programmed desorption (TPD) tests. The low-silica HZSM-5(25) showed the best performance (326.6 μmol/g and 39.2 μmol/g at dry and 90%RH) as compared to others with higher Si/Al ratios at each RH, in which the roll-up effect was positively correlated with the Si/Al ratios and humidity. O 2 enhanced NO x adsorption and reached an optimal adsorption capacity at the concentration of 14%, while CO 2 had little effect on NO x adsorption. The decrease in temperature increased NO x adsorption capacity on HZSM-5(25), benefitting from NO 2 physisorption as well as satisfactory NO oxidation within the active adsorbent structure. The facile thermal desorption of NO x and significant NO–NO 2 conversion on HZSM-5(25) was exhibited by bimodal TPD peaks at 343–353K and 533–543K respective for NO and NO 2 , in contrast to those on Silicalite-1. A potential “water-resistant” strategy via the enhancement of NO x adsorption competitiveness was revealed, providing a theoretical guideline for NO x adsorbent screening in industrial applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Yixuan Feng,Haixin Guo,Richard L. Smith,Xinhua Qi
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) was examined as an alternative to thermocatalytic methods in which two-dimensional (2D) cobalt-metal–organic framework (Co-MOF, ZIF-L-Co) nanoplate arrays were prepared on nickel foam (NF) and then transformed into hierarchical porous Co 3 O 4 nanostructures by chemical etching and low temperature annealing to form electrode materials . Hierarchical porous nanoarrays formed during synthesis enlarged the surface area of the as-prepared catalysts introduced a large number of defects and exposed active sites leading to reduced charge diffusion , improved mass transfer and efficient HMF oxidation . Co 3 O 4 /NF electrode materials were able to achieve a current density of 10 mA·cm −2 at an overpotential of 105 mV in 1 M KOH with 10 mM HMF, which was reduced by 175 mV compared with water oxidation. Electrocatalytic oxidation experiments afforded 100 % HMF conversion and 96.7 % FDCA yields with a minimum 96.5 % faradaic efficiency at 1.43 V vs RHE. The proposed MOF-structured synthesis method fundamentally reduces charge diffusion , improves mass transfer of electrodes and is generally applicable to fabrication of hierarchical porous nanostructured materials.
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DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 9
·2813-2823
·
IF 2.936
Yang Jian,Li Xuemei,Zhang Jia,Tian Junying,Yao Xiaolan,Liu Hailong,Xia Chungu,Huang Zhiwei
Valuable 5-amino-1-pentanol (5-AP) was efficiently synthesized from biomass-derived dihydropyran over hydroxylapatite nanorod supported Ni catalysts (Ni-HAP), by coupling the in situ generation of 5-hydroxypentanal (5-HP, via the ring-opening tautomerization of 2-hydroxytetrahydropyran (2-HTHP)) and its subsequent reductive amination. The Ni-HAP catalyst with 10 wt% Ni loading exhibited the highest 5-AP yield than the other Ni-HAP catalysts with different Ni loadings and several commercial hydrogenation catalysts, including Ru/C, Pt/C and Pd/C, as well as Raney Ni. High Ni particles dispersion, high reducibility and acidic intensity were found to account for the superior catalytic performance of 10Ni-HAP. The effect of reaction parameters on the catalytic performance was investigated, and an excellent 5-AP yield of 92% was achieved under mild reaction conditions of 80 °C and 2 MPa H 2 . The stability of the Ni-HAP catalyst was studied using a continuous flow reactor, and the sintering of Ni nanoparticles was considered as the major reason for the decline in hydrogenation activity. Graphical Abstract The Ni-HAP catalyst exhibited high catalytic performance to synthesis 5-AP due to the high Ni particles dispersion, reducibility and acidic intensity.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Bo Jiang,Jinzhe Li,Xinyi Chen,Lu Huang,Shan Luo,Ying Xing,Jing Deng,Shuang Song,Feilong Dong
Exploring an environmentally friendly and highly activation catalysts in the advanced oxidation processes (AOPs) basing on sulfate radicals (SO 4 − •) has shown great importance for the remediation of refractory contaminants. Herein, Fe 3 O 4 -wrapped ZSM-5 (Fe 3 O 4 @ZSM-5) was constructed as heterogeneous catalyst to remove ciprofloxacin (CIP) via peroxymonosulfate (PMS) activation, in which performance, kinetics and mechanism insight were investigated in depth. The removal efficiency of CIP reached 90 % by Fe 3 O 4 @ZSM-5 catalysts within 100 min reaction when the initial pH was 3.0. During the reaction, SO 4 − • and HO• were proved to be coexisted in reaction system and SO 4 − • played a critical role in CIP degradation according to the radical quenching experiments and electron paramagnetic resonance (EPR) measurements. Based on the catalyst characterization and Langmuir-Hinshelwood adsorption kinetics analysis, the synthesis of Fe 3 O 4 nanoparticles (NPs) and ZSM-5 accelerated the dispersion process and enhanced adsorption ability of Fe 3 O 4 NPs, which further promoted the local concentration of CIP and PMS on the surface. In addition, the cycling experiments and metal leaching tests demonstrated that Fe 3 O 4 @ZSM-5 catalysts were stable and could be conveniently reused by magnetic separation. In addition, the impacts of coexisting irons (Cl − , SO 4 2− , NO 3 − , HCO 3 − ) confirmed that Fe 3 O 4 @ZSM-5 was still effective in real water. This study demonstrated the promising prospect of Fe 3 O 4 @ZSM-5/PMS system in the application of degradation refractory organic pollutants .
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Xinyi Xing,Xian Shi,Rui Hu,Ying Guan,Hui Gao,Siquan Xu
In this work, a series of (x)Hf-β zeolite catalysts were prepared by a simple wet impregnation method and used as bifunctional catalysts with Lewis and Brønsted acid sites for synthesizing 5-hydroxymethylfurfural (5-HMF) from cellulose in H 2 O (NaCl) -THF biphasic system. Characterization analysis of (x)Hf-β zeolite catalysts with ICP-OES, N 2 adsorption-desorption isotherm, XRD, FTIR , SEM, NH 3 -TPD and Py-FTIR indicated that the catalysts possessed favorable pore structure, appropriate acid strength and acidity. A superior 86.3 % cellulose conversion and 53.4 % 5-HMF yield could be obtained at 200 °C for 4 h by using (5 %)Hf-β zeolite as the catalyst. In addition, the catalytic system provided a favorable 5-HMF yield from other carbohydrates, including glucose (85.1 %), sucrose (80.6 %), starch (65.1 %), maltose (65.0 %), dextran (59.9 %), and Moso bamboo (21.9 %). Nevertheless, the recyclability of (5 %)Hf-β zeolite catalyst was unsatisfactory and the 5-HMF yield showed a downtrend from 53.4 % to 24.4 % after 5 cycles. The catalyst has promising potential for converting biomass materials into high-value platform compounds.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Ge Yang,Xi Yan,Yan Chen,Xiao-Jing Guo,Wan-Zhong Lang,Ya-Jun Guo
In recent years, Ga-based catalysts attract much attention in propane dehydrogenation (PDH) reaction due to environmental friendliness and low cost. Nevertheless, it is still challenging to obtain high selectivity of propylene under harsh reaction conditions. In this work, the supported catalysts (Ga- x Mg/ZSM-5) were prepared with the sequential impregnation method and applied in the PDH reaction. The results show that MgO as an additive reduces the acidity of the catalysts, promotes the dispersion of Ga 2 O 3 and improves the selectivity of propylene. As a result, the average particle size of the Ga/ZSM-5 catalyst is larger (4.5 nm), and the initial propylene selectivity is only 71.0 %. In contrast, the optimal Ga-0.7Mg/ZSM-5 catalyst shows the smallest particle size (2.4 nm) and the highest propylene selectivity of 90.8 %. In comparison with the previous GaO x catalysts in literatures, the Ga-0.7Mg/ZSM-5 catalyst exhibits a superior production rate of propylene ( r C 3 H 6 ) based on either catalyst weight or Ga 2 O 3 weight.
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FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Xiangbo Song,Yuhe Liao,Tingsen Liu,Dedu Yin,Haiyong Wang,Lungang Chen,Longlong Ma,Hongwei Yang,Leonid G. Voskressensky,Chenguang Wang
Synthesis of 5-hydroxymethylfurfural (HMF) from carbohydrate is one of vital step for bio-refinery development. In this work, a novel strategy was developed for catalytic conversion of fructose to HMF in 2-butanol. The inexpensive ionic liquids were used to adjust the acidity of biobased acid catalyst for enhancing the dehydration of fructose to HMF. The combination of 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) with oxalic acid afforded an excellent HMF yield of 97.1% at 98.7% fructose conversion under mild conditions of 100 °C and 60 min, owing to the enhanced dissociation ability of oxalic acid by [Bmim]Cl. A possible dissociation mechanism of oxalic acid induced by [Bmim]Cl was proposed based on control experiments and detailed analyses with NMR and FT-IR techniques. It involved that the [Bmim]Cl interacted with oxalic acid through hydrogen bond , which decreased the electron density of oxygen atom on hydroxyl group and weakened the O-H bond, thus making the hydrogen in the O-H group to easily dissociate in the form of H + . Moreover, the reusability of oxalic acid and [Bmim]Cl was demonstrated, and both could be reused up to six times without significant loss in activity
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