Materials
·
2023
·Vol. 16
·期 2
·684
·
IF 3.4
Yunxin Yang,Cong Wang,Hua Zhang,Jiancai Qian,Song Yang,Huiyun Liao,Xuehui Sun,Yipeng Wang,Peijian Sun,Yunzhen Jia,Junwei Guo,Huaiyuan Zhu,Cong Nie
Removal of 1,3-butadiene from cigarette smoke plays an important role in human health and environmental protection. Herein, a series of UiO-66 X% containing different ratios of the -NH2group was synthesized via the solvothermal method by using terephthalic acid (H2BDC) and 2-aminoterephthalic acid (NH2-BDC) as ligands. Using GO as support, a series of UiO-66-NH2/GO Y% were prepared by controlling the ratio of UiO-66-NH2and GO. The effects of -NH2and GO contents on the structure and composition of MOFs were investigated. Finally, the different -NH2contents of UiO-66 X% and the different GO contents of UiO-66-NH2/GO Y% were applied in 1,3-butadiene removal from cigarette smoke. The results showed that UiO-66 X% with the higher contents of -NH2showed a higher rate of 1,3-butadiene removal, and UiO-66-NH2/GO Y% with the GO contents of 5% showed the highest removal rate of about 33.85%, which was 25.54% higher than that of activated carbon. In addition, the saturation capacity of the adsorbent materials for 1,3-butadiene was as high as 210.01–239.54 mg/g, showing great potential in reducing harmful components in cigarette smoke and environmental protection.Keywords:UiO-66;UiO-66-NH2/GO;1,3-butadiene removal;cigarette smoke
研究领域:
材料科学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xianquan Li,Jifeng Pang,Yujia Zhao,Lin Li,Wenguang Yu,Feifei Xu,Yang Su,Xiaofeng Yang,Wenhao Luo,Mingyuan Zheng
The catalytic synthesis of 1,3-butadiene (1,3-BD) from bio-based ethanol offers an alternative and sustainable process beyond petroleum. However, the intrinsic active sites and corresponding mechanism of 1,3-BD formation have not been fully elucidated yet. By correlating systematic characterization results with catalytic performance, the open Zr species, i.e., Zr(OH)(OSi) 3 moieties, were identified as the active site over the Zr/MFI-BM catalysts for the catalytic transformation of ethanol-acetaldehyde into 1,3-BD. In conjunction with controlled experiments and theory calculations, ethanol and acetaldehyde are proposed to synergistically co-adsorb on the Zr(OH)(OSi) 3 species in a bi-molecular mode, which assists the acetaldehyde condensation and accelerates the critical Meerwein-Ponndorf-Verley-Oppenauer reduction, and accordingly promotes 1,3-BD formation. These findings will stimulate the search towards new metal-zeolite combinations for efficient production of value-added 1,3-BD via biomass-derived ethanol and beyond.
研究领域:
化学工程
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催化科学
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材料科学
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DOI
高影响因子
AICHE JOURNAL
·
2020
·Vol. 67
·期 4
·e17114
·
IF 3.519
Ihtisham Ul Haq,Tao Wang,Ao-Shuai Zhang,Heng Mao,Rehan Khan,Li-Hao Xu,Zhi-Ping Zhao
1,3-Butadiene (BD) is a petrochemical-based volatile organic compound, extensively used for the manufacture of synthetic rubber. There is no method reported for its recovery from nitrogen mixture. Herein, for the first time, BD is efficiently recovered by gas separation through facile and novel mixed-metal ZIF-8 based mixed matrix membranes (MMMs). Addition of Ni-ZIF-8 nanoparticles in PDMS matrix, significantly improved the penetrant-membrane interactions and the solution-diffusion properties of BD. Positron annihilation lifetime spectroscopy analysis showed that the well dispersion of Ni-ZIF-8 in PDMS enhanced the free volume of membrane and created efficient continuous paths for BD diffusion. Then, 15 wt% Ni-ZIF-8 MMM exhibited the BD permeance of 323 GPU and the BD/N 2 ideal selectivity of 19.5, which were 60 and 81% higher than pure PDMS membrane, respectively. The simultaneous enhancement of BD permeance and BD/N 2 ideal selectivity indicated that Ni-ZIF-8 was an effective filler applied in MMMs for efficient BD recovery.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 12
·7140-7149
·
IF 3.108
Yuchao Xu,Zongzhang Liu,Zheng Han,Minhua Zhang
ZnO promoted ZrO2–SiO2 catalysts synthesized by a sol–gel method were investigated in the two-step ethanol transforming to 1,3-butadiene process. The influence of promoters and the preparation method of the catalysts on the catalytic performance were studied in detail and the reaction conditions were optimized. The as-prepared catalysts were characterized by BET, X-ray diffraction (XRD), Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), Fourier Transform Infrared Resonance (FT-IR), X-ray photoelectron spectroscopy (XPS), FT-IR spectroscopy of adsorbed pyridine (Py-IR) and temperature-programmed desorption of NH3 (NH3-TPD). ZnO added ZrO2–SiO2 catalysts show the best catalytic activity and the catalysts prepared by the hybrid sol–gel method were superior to those prepared by the sol–gel coupled with impregnation method. The addition of promoters in the ZrO2–SiO2 system decreased the total acidity and lowered the selectivity to dehydration products. The best performance with ethanol/acetaldehyde conversion of 40.7% and 1,3-butadiene selectivity of 83.3% was reached at 310 °C, ethanol/acetaldehyde mole ratio of 3.5 and WHSV of 1.4 h−1 using a 0.5 wt% ZnO doped ZrO2–SiO2 catalyst.
研究领域:
催化化学
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材料科学
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能源化工
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ihtisham Ul Haq,Shen Hui Li,Hong-Gang Zhen,Rehan Khan,Ao-Shuai Zhang,Zhi-Ping Zhao
For separating 1, 3-butadiene (BD) from BD/N 2 mixture, among numerous studied metal–organic frameworks-based adsorbents, Ni-ZIF-8 was comparatively selected here based on intelligent gravimetric analysis, simulation studies, facile synthesis, and very good IAST selectivity. Experimental results showed good butadiene uptake capacity of Ni-ZIF-8 of 7.41 mol/kg, which is 42% higher than pure ZIF-8. Additionally, Ni-ZIF-8 exhibits IAST selectivities of 2826 and 3302 at 0.1 bar, at 25 and 45 °C respectively, for 20% BD/N 2 adsorption. The molecular simulation results showed that Ni-ZIF-8 has binding energies of 65.25, 9.54 kJ/mol, while ZIF-8 has 56.07, 15.03 kJ/mol for butadiene, and nitrogen, respectively. This strongly supported the experimental results. To the best of our knowledge, Ni-ZIF-8 showed the best working capacity of 5.91 mol/kg for butadiene among all the reported adsorbents. Moreover, dynamic adsorption experiments revealed that butadiene could be recovered from BD/N 2 mixtures at room temperature, suggesting great potential for industrial BD/N 2 separation.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS SURVEYS FROM ASIA
·
2023
·Vol. 27
·期 3
·207-216
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IF 3
Li Shuying,Huang Bin,Jin Changzi,Wang Rui,Jiang Heng,Yang Guang-Sheng,Huang Shengjun
The conversion of ethanol and acetaldehyde to 1,3-butadiene has been an emerging process to produce key chemicals. The preparation of highly efficient catalysts and the understanding of reaction mechanism are current research priority. Herein, mesoporous silica framework confining zirconia (Zr-HMS) was prepared and act as catalyst for 1,3-butadiene production from ethanol and acetaldehyde. The prepared catalysts were characterized by Low-angle X-ray powder diffraction, transmission electron microscopy, N 2 physical adsorption-desorption, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and UV–vis spectra. It has been shown that the Zr-HMS exhibits similar textural properties to supported catalyst (ZrO 2 /HMS). However, regardless of their comparable activities, higher 1,3-butadiene selectivity is obtained over Zr–HMS, which can be due to the different active zirconia species in two catalysts. Mesoporous framework confining character of Zr-HMS can achieve uniformly dispersed zirconia species. Further investigation toward the reaction process has presented new viewpoints for formation and consumption of some typical intermediates and byproducts, which will help to understand the reaction mechanism and construct efficient catalysts for conversion of ethanol and acetaldehyde to 1,3-butadiene.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 150
·期 5
·1462-1470
·
IF 2.372
Zhang Minhua,Qin Yu’nan,Tan Xuechao,Wang Lingtao,Yu Yingzhe,Jiang Haoxi
Abstract In this paper, the MgO–SiO 2 catalyst was prepared with the deposition–precipitation method, which was used to catalyse the conversion of ethanol to 1,3-butadiene through a two-step process. The carbon deposition deactivation of the catalyst was mainly caused by that the carbon species occupied the acid-basic active sites on the catalyst surface. The carbon deposition mainly includes chain alkanes and aromatic compounds from outer to inner layers, and its site was mainly MgSiO 3 , followed by MgO, while SiO 2 showed weak carbon deposition ability. Graphic Abstract
研究领域:
催化化学
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材料科学
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DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 126
·103982-103988
·
IF 3.84
Zheng Han,Xiang Li,Minhua Zhang,Zongzhang Liu,Meixiang Gao
A series of ZrO2–SiO2 catalysts synthesized by sol–gel method were investigated for the 1,3-butadiene formation from bioethanol and acetaldehyde. The influence of ZrO2 content and reaction conditions on catalytic performance were studied. The catalysts were characterized by N2 adsorption–desorption analysis, temperature-programmed desorption of NH3 (NH3-TPD), IR spectroscopy of adsorbed pyridine (Py-IR), Fourier Transform Infrared Resonance (FTIR), X-ray diffraction (XRD) and Transmission Electron Microscope (TEM). These characterization results indicated that suitable intensity of acid sites, especially Lewis acid, are very crucial to obtain an active catalyst. The catalysts showed significantly higher selectivity for C4 chemicals, and 2 wt% ZrO2 content reached the highest selectivity to BD (69.7%), at space velocity (WHSV) of 1.8 h−1.
研究领域:
催化化学
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可再生资源转化
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材料科学
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DOI
高影响因子
RUBBER CHEMISTRY AND TECHNOLOGY
·
2016
·Vol. 89
·期 4
·700-711
·
IF 0.878
Hong Kan,Ni Xufeng,Shen Zhiquan
Organic supporter poly(styrene-co-divinylbenzene) (PS-DVB) was synthesized, and gas-phase polymerization of 1,3-butadiene was performed with PS-DVB–supported Nd(vers) 3 /Al 2 Et 3 Cl 3 /Al(i-Bu) 3 catalysts. Millimeter-sized granules of high cis -1,4 content (>98%) polybutadiene with an M n of 5.3–5.5 × 10 5 were obtained. Dispersants used in gas-phase polymerization of 1,3-butadiene have a significant influence on apparent activities of catalysts and appearance of products. The morphology of polybutadiene granules was also investigated by scanning electron microscopy.
研究领域:
高分子化学
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催化化学
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DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 7
·期 1
·168-180
·
IF 5.287
Xiaoxiong Huang,Yong Men,Jinguo Wang,Wei An,Yuanqiang Wang
A series of magnesia–silica binary composite catalysts with different molar ratios were prepared using various preparation methods and evaluated for the one-step production of 1,3-butadiene (BD) from bio-ethanol. The MgO–SiO2 catalyst prepared by wet-kneading is distinguished from the samples prepared by other methods by its superior activity. An exceptionally high productivity of butadiene with the high ethanol conversion of 95% and BD selectivity of 77% was obtained over wet-kneaded hierarchical flower-like MgO nanostructures with the catalytic material made up of SiO2 spheres (with a MgO : SiO2 molar ratio of 65 : 35 at 450 °C and an WHSV of 4.1 h−1), which translates into an unprecedented BD yield of 0.025 mol gcat−1 h−1. The as-prepared catalysts were characterized by XRD, FESEM, BET, FT-IR, UV/vis, CO2-TPD and NH3-TPD. The Mg precursor used and the preparation method are found to influence the extent of MgO and SiO2 interactions during preparation, as estimated by various techniques, which, in turn, was found to correlate with the catalytic performance. A subtle balance of surface acidity/basicity was found to be necessary to achieve a high butadiene yield which can be obtained by variation of MgO : SiO2 ratios in wet-kneaded samples. In view of the difference in catalytic activity and the physicochemical properties of the MgO–SiO2 composite catalysts, the Si–O–Mg chemical bond formed by the strong MgO and SiO2 interaction is suggested to be essential for the balanced surface acid/base sites in relation to the strong interaction between MgO and SiO2 and the consequent high catalytic performance.
研究领域:
催化化学
·
材料科学
·
能源化学
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产品关联
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 59
·34069-34077
·
IF 2.936
Minhua Zhang,Xuechao Tan,Tong Zhang,Zheng Han,Haoxi Jiang
A deactivation study on the ethanol/acetaldehyde conversion to 1,3-butadiene over a ZnO promoted ZrO2–SiO2 catalyst prepared by a sol–gel method was performed. The samples were characterized by N2 adsorption–desorption isotherms, scanning electron microscopy (SEM), NH3 temperature programmed desorption (NH3-TPD), X-ray powder diffraction characterization (XRD), thermogravimetric analyses (TGA), Fourier transform infrared resonance (FT-IR), 13C magic-angle spinning nuclear magnetic resonance (13C NMR) and X-ray photoelectron spectroscopy (XPS). The pore structure characteristics and surface acidity of Zn0.5–Zr–Si catalysts were largely decreased with time-on-stream and no crystal structure was formed in the used catalyst, indicating that the deactivation was caused by carbon deposition. Two main types of carbon deposition were formed, namely low-temperature carbon deposition with the oxidation temperature of around 400 °C and high-temperature carbon deposition with the oxidation temperature of 526 °C. The carbon species were mainly composed of graphitized carbon, amorphous carbon, carbon in C–O bonds and carbonyls. The deactivated catalyst could be regenerated by a simple oxidation process in air. Adding a certain amount of water into the feed had a positive effect on reducing the carbon deposition.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 98
·期 7
·1620-1630
·
IF 3.4
Minhua Zhang,Yan Zhang,Yuxin Tan,Guochao Yang,Haoxi Jiang,Lingtao Wang
BACKGROUND With the improvements in bioethanol production, the process of converting ethanol to 1,3-butadiene (ETB) has received substantial scholarly attention, whose industrialization has been constrained by the stability of the catalysts. RESULTS In this work, the deactivation behavior of Zr- β zeolite in the process of ethanol/acetaldehyde conversion to 1,3-butadiene was investigated. In addition, the deactivation kinetics of ETB was studied using an isothermal differential microreactor. A kinetic model was developed and parametrized with the Langmuir–Hinshelwood mechanism, and the intrinsic kinetic equation was derived. The deactivation kinetic model of the ETB reaction was established from the active site content of the catalyst as a function of time on stream. The validity of the kinetic model was tested, and the results were found to be accurate. CONCLUSIONS Catalyst deactivation was mainly caused by coke species, which are mainly long-chain unsaturated oxygenated organic compounds and aromatic compounds, covering Lewis acid sites in the microporous channels of the catalyst; nevertheless the zeotype topology and morphology were not destroyed. The kinetic data suggested that the reaction was of first order and the activation energy of the deactivation process was 75.59 kJ mol −1 . © 2023 Society of Chemical Industry (SCI).
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）