Catalysis Science & Technology
·
2025
·
IF 4.2
Dajian Li,Alfin Kurniawan,Tania Roy,Jin Wang,Cheng lan Liu,Ze Zhen Wang,Rong Zhen Mu,Chun Hui Zhou
The efficient production of allyl alcohol from glycerol is of great importance due to its significance as a valuable intermediate in chemical industries. While catalytic conversion of glycerol to allyl alcohol by solid acid catalysts, carbon deposition (coking) is prone to occur on the catalyst surface, leading to slow down the conversion process and fast deactivation of the catalyst. In this study, we obtained an efficient catalyst for the preparation of allyl alcohol from gas-phase glycerol by controlling the pore structure and surface acidity of the catalyst. The characterization results showed that hydrochloric acid and citric acid removed the silicon and aluminium elements from montmorillonite, and the acidity, pore volume, and surface area ratio of Na-MMT (SBET=34.5 m2 g-1, VT=0.19 cm3 g-1) of the porous montmorillonite(HA1MMT) catalyst were all improved (SBET=97.9 m2 g-1, VT=0.28 cm3 g-1); After adding MoOx and VOx, the selectivity of Mo/V-HA1MMT catalyst for allyl alcohol was improved. The XPS characterization results indicate that the synergistic effect of Mo and V can promote the transfer of electrons during the reaction process of glycerol conversion. Within 480 minutes of catalyzing glycerol dehydration reaction, Mo0.6V0.4(5)-HA1MMT was almost deactivated (Conv.= 19.5%, Sel.allyl alcohol=31.2%) due to carbon deposition. When the catalyst was doped with calcium and magnesium components, a new active phase CaMo4 was discovered on the catalyst, and the acidity of Ca0.5Mg0.5-Cat. (Cat. is Mo0.6V0.4(5)-HA1MMT) decreased to 214.0 μmol g-1. The coking resistance performance of Ca0.5Mg0.5-Cat. was improved, and after 660 minutes of reaction, the catalyst was deactivated (Conv.= 32.1%, Sel.allyl alcohol=30.1%) due to carbon deposition. During the 3rd catalyst regeneration test, Ca0.5Mg0.5-Cat. still maintained high activity (Conv.= 63.3%, Sel.allyl alcohol=35.2%, Sel.acrolein=31.2%). The results of this study indicate that suitable pore structure and acidity are crucial for designing a catalyst with coking resistance properties.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2020
·Vol. 11
·期 1
·48-56
·
IF 3.119
Yingjie Hu,Yuxin Mei,Baining Lin,Xuhong Du,Fan Xu,Huasheng Xie,Kang Wang,Yonghua Zhou
The one-pot synthesis of methyl isobutyl ketone (MIBK) and methyl isobutyl methanol (MIBC) from acetone and hydrogen is a typical cascade reaction comprised of aldol condensation-dehydration-hydrogenation. Pd loss and aggregation during long term operation are typical problems in industrial application. In this paper, an active and stable catalyst was achieved with defective UiO-66 as a support for Pd, which was synthesized with the ratio 15 : 1 of ZrOCl2·8H2O to ZrCl4 as Zr-precursors. The resultant Pd catalyst remained active for at least 1000 h with a MIBK + MIBC selectivity of 84.87–93.09% and acetone conversion of 45.26–53.22% in a continuous trickle-bed reactor. Besides the increased Brønsted acid amount generated by the defect sites was favorable for the activity, the cavity confinement in the UiO-66 (R = 15 : 1) structure also efficiently prevented Pd loss and aggregation during the long term run. The contrast of the characterization of the fresh and used Pd/UiO-66 (R = 15 : 1) indicated that the deactivation of the catalyst was attributed to carbonaceous accumulation on the catalyst surface, which could be easily regenerated by calcination. This work supplied a new alternative for the design and utilization of industrial catalysts for MIBK and MIBC synthesis.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Nano
·
2022
·
IF 13.364
H. Wang,Y. Liu,H. Wang,J. Song,D. Ma,Z. Dai
Efficient utilization of hydrocarbon fuels holds great significance for the current vehicle low-emission requirements and future carbon-neutral society. However, the scenario that limits the effective fuel use and combustion is the present undesirable hydrocarbon-cracking catalysts of low activity, serious coking, and easy degradation. To tackle these issues, we rationally designed and synthesized an active, anti-coking, and recyclable all-in-one zeolite@Ru–Al 2 O 3 catalyst on FeCrAl support by steam-assisted crystallization and atomic layer deposition . Ru nanoclusters dispersedly on ZSM-5 can boost the catalytic efficiency for hydrocarbon cracking and anti-coking, while the protective Al 2 O 3 thin layers further ensure the reusable economy. As for n-dodecane (C 12 H 26 ) cracking reaction, the ZSM-5@Ru–Al 2 O 3 showed a high unit activity up to 0.1253%·ml·mg −1 ·min −1 , low-carbon deposition rate, and the enhanced first-cycle carbon removal rate of 78.3% for recyclable use. Density functional theory (DFT) calculations have further confirmed that high catalytic efficiency and low-carbon deposition benefit from the timely adsorption of C 12 H 26 and timely transfer of reactant products at the composite interface. This work opens interesting possibilities for the rational design and fabrication of high-efficient, anti-coking, and recyclable hydrocarbon cracking catalysts through multifunctional structural regulations.
研究领域:
催化化学
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材料科学
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Minerals Metallurgy and Materials
·
2018
·Vol. 25
·期 2
·226-235
·
IF 1.261
Chen Zhi-yuan,Bian Liu-zhen,Yu Zi-you,Wang Li-jun,Li Fu-shen,Chou Kuo-Chih
Carbon deposition on nickel powders in methane involves three stages in different reaction temperature ranges. Temperature programing oxidation test and Raman spectrum results indicated the formation of complex and ordered carbon structures at high deposition temperatures. The values of I (D)/ I (G) of the deposited carbon reached 1.86, 1.30, and 1.22 in the first, second, and third stages, respectively. The structure of carbon in the second stage was similar to that in the third stage. Carbon deposited in the first stage rarely contained homogeneous pyrolytic deposit layers. A kinetic model was developed to analyze the carbon deposition behavior in the first stage. The rate-determining step of the first stage is supposed to be interfacial reaction. Based on the investigation of carbon deposition kinetics on nickel powders from different resources, carbon deposition rate is suggested to have a linear relation with the square of specific surface area of nickel particles.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF FLUORINE CHEMISTRY
·
2024
·
IF 1.7
Xiaoli Wei,Yiwei Sun,Jianhai Jiang,Zhen Wang,Wei Zhang,Bing Liu,Shucheng Wang,Xiaodan Yang,Wanjin Yu,Jianjun Zhang,Wenfeng Han
Al 2 O 3 exhibits high activity for the resource utilization of potent greenhouse gases, hydrofluorocarbons via dehydrofluorination or F/Cl exchange. However, it experiences completely fluorination under corrosive HF environment, leading to thorough fluorination of F-Al-O active site into F-Al-F, accompanied with serious carbon deposition. In this work, we successfully confined Al 2 O 3 in SiC (Al 2 O 3 @SiC) via treating Al 2 O 3 /SiC under high temperatures (>800 °C). The results showed that different with simple loaded Al 2 O 3 (Al 2 O 3 /SiC), during high temperature treatment, reaction between Al 2 O 3 and SiC occurred, leading to the confinement effect. Then, contributed by the interaction, desired F-Al-O species could be stabilized on the surface of SiC. While for Al 2 O 3 /SiC, it thoroughly turned into AlF 3 under identical reactive conditions, leading to inferior stability during CH 3 CHF 2 dehydrofluorination. Furthermore, the reaction rate of 5 %Al 2 O 3 @SiC is nearly up to 4 folds higher than that of traditional AlF 3 . Facilitated by the suitable Lewis acid intensity, less carbon deposition formed on Al 2 O 3 @SiC. Thus, constructing strong interaction between F-Al-O and stable SiC provides a potential strategy to stabilize unstable active centers.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Jiming Wang,Min Ji,Jiaqi Lv,Min Wang
Photo-thermo-chemical dry reforming of methane (PTC-DRM) produces syngas has been a promising strategy to utilize abundant solar energy and alleviate greenhouse effect. Herein, we report an efficient PTC-DRM process on Ni-based catalyst with Zn doping and investigate the effect of Zn on the catalytic performance of catalysts. Zn promoted the generation of active sites on the surface of Ni-Al 2 O 3 , suppressed the accumulation of coke during the reaction process and enhanced the photocatalytic activity of the catalyst. Ni-ZnO-Al 2 O 3 catalyst exhibited highest thermal catalytic performance and the conversion of CH 4 and CO 2 are 50.2% and 58.1% at 650 ℃, respectively. All catalysts exhibited higher reaction rates of CH 4 and CO 2 and higher hydrogen selectivity under light conditions. Light also significantly enhanced the carbon deposition resistance and stability of the catalyst. And possible reaction mechanism of the Ni-ZnO-Al 2 O 3 was proposed during PTC-DRM process.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Su Li,Jinkai Qiu,Zijun Bian,Bin Shao,Zhicheng Liu,Cheng Lian,Honglai Liu,Jun Hu
The dry reforming of carbonate with methane (CaDRM) can be one of the breakthrough technologies to address the challenge of mitigating inevitable CO 2 emissions into value-added chemicals but remains great challenges for efficient catalysts design. In this study, we break the trade-off between the catalytic activity and the carbon deposit by tailoring the d-band center of Ni through Fe doping, which matches the energy level of CH 4 * dehydrogenation but is far away from that of the over cleavage of CH* . In this light, the porous spherical Fe x Ni/Al 2 O 3 catalysts with Ni 3 Fe alloy nanoaggregates are obtained through a one-step spray drying method. The optimized Fe 0.6 Ni/Al 2 O 3 catalyst shows an excellent catalytic activity with a superior CO selectivity of 91.75 % at a complete CaCO 3 conversion at 700°C, and successfully prevents the carbon deposit to maintain its excellent stability. Moreover, the extremely low activation energy of 45.2 kJ/mol and the good porosity of Fe x Ni/Al 2 O 3 ensure its fast dynamics. Therefore, this tailoring d-band center approach through the formation of alloy catalysts supplied a novel strategy for effectively cracking hydrogen species while avoiding over cleavage of CH x * in the thermal catalysis, which promoted the CaDRM technology to be a promising solution for carbon neutrality in industrial sectors in near future.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 1.9
Sarmad Soomro,Zhenkun Sun,Dennis Y. Lu,Zhihao Zhou,Lin Li,Lunbo Duan
Catalyst deactivation due to carbon deposition and sintering poses a significant challenge to the efficient dry reforming of CH 4 and CO 2 into syngas, particularly at high Ni loadings. To tackle this difficulty, ordered mesoporous silicas with varied pore symmetries were employed as supports in this study to synthesize the Ni-based catalysts using hydrothermal treatment. The 10% Ni/MCM-41 catalyst exhibited the highest conversion rates for CO 2 (81%) and CH 4 (77%), with favourable H 2 /CO (0.92) ratios indicating efficient syngas production Higher Ni concentrations increase active sites and catalytic performance, they also increase carbon deposition, reducing catalyst durability. At lower Ni loadings (4% Ni), catalysts with a 3D pore structure showed improved activity and stability, effectively reducing carbon deposition. This study demonstrates that optimized mesopore symmetries and Ni loadings can enhance catalyst efficiency and durability for syngas production.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2019
·
IF 4.914
Jingqing Tian,Haocheng Li,Xin Zeng,Zichun Wang,Jun Huang,Chen Zhao
ABSTRACT Development of dry reforming of methane and carbon dioxide is an effective route to convert in-dustrial waste gases such as coke-oven gas and coal-to-oil gas into platform syngas. However, this process encounters severe problems of metal particle sintering and coke formation at high tem-peratures. In this work, we developed a new synthetic method for preparing confined Ni/MCM-41 catalysts, which impede the sintering of metal nanoparticles (NPs) and coke deposition at high temperatures, enabling them to be successfully applied to methane dry reforming . The method results in high activity and stability of the catalyst at 700 °C for 200 h. The Ni precursor is immersed in ethanol and impregnated into MCM-41 by the peculiar capillary action of hexagonal straight mesopores . By this method, 10 wt% Ni NPs (d = 2 nm) is equably confined to the mesoporous channels with strong metal-support interactions, as confirmed by HRTEM, TEM mapping, H2-TPR, and XRD measurements. Such a confined structure has a significant effect on the inhibition of metal NP agglomeration and carbon deposition during methane dry reforming, as evidenced by TEM, Raman, TGA, and TPO measurements of used Ni/MCM-41 catalysts. In contrast, unconfined Ni/MCM-41 catalysts, with Ni NPs located on the pore exteriors, are rapidly deactivated after 12 h due to the blocked contact between the active metal centers and the gas feedstock. Additionally, a fast increase in the Ni NP size and the formation of substantial carbon nanotubes on the unconfined catalyst surface are seen. This work offers a facile approach for the synthesis of anti-sintering, car-bon-resistant confined Ni catalysts that can operate at high temperatures
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2021
·
IF 6.766
Shan Liu,Zhiquan Yu,Yao Wang,Zhichao Sun,Yingya Liu,Chuan Shi,Anjie Wang
Catalytic dehydration of glycerol over solid catalysts provides a sustainable and economic route to producing acrolein. Unsupported MoP catalyst was prepared by temperature-programmed-reduction method and used for the gas-phase glycerol dehydration. The catalyst was characterized by means of XRD, SEM, TEM, NH 3 -TPD, Py-IR, XPS, TG-DSC, and N 2 adsorption-desorption. It is indicated that the acidic P OH and M oOH groups, which are usually associated with the weak or moderate strength of Brønsted acid sites, were presented on the surface of MoP. The effects of reaction temperature and carrier gas flow rate on glycerol conversion and acrolein selectivity were investigated over MoP. The selectivity to acrolein was up to 89.0 % and kept constant in a 50-h run at 240 °C. The gradual decrease of glycerol conversion might be related to the insoluble carbonaceous materials deposited on the catalyst surface.
研究领域:
催化化学
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材料科学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 6
·062504
·
IF 4.386
Fangzhao Pang,Peng Li,Zhuqing Zhao,Lei Guo,Kaifa Du,Bowen Deng,Dihua Wang,Huayi Yin
Electrolysis of solid oxides in molten CaCl2 has been proven a straightforward process to extract various metals thanks to the wide electrochemical window of CaCl2 and CaO which is soluble in molten CaCl2. However, the CaO produced during the cathodic reduction of oxides not only shuttles O2−, but also captures CO2 to generate CO32− that can be reduced to carbon at the cathode, resulting in decreasing current efficiency and contaminating the cathodic products by carbon. To solve this problem, we employed CaSiO3 to replace CaO to suppress/avoid the formation of CO32− and thereafter prevent the carbon deposition. The suppression of CO32− formation is because SiO32− is thermodynamically more stable than CO32−, i.e., the CO2 generated on the graphite anode can not be captured by SiO32−. In molten CaCl2−8.0 wt% CaSiO3, Cr2O3 and SiO2 are reduced to Cr and Si with much less carbon deposition than in molten CaCl2. As a result, the current efficiency increases from 21.4% to 51.9% for the reduction of Cr2O3 and 37.1% to 72.2% for the reduction of SiO2. Although introducing SiO32− will slightly decrease the electrochemical window of CaCl2, it will be a promising method to avoid carbon contamination and increase current efficiency especially for Si production.
研究领域:
材料科学
·
冶金工程
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2017
·Vol. 9
·期 19
·3646-3654
·
IF 4.803
Bin Zhang,Qifan Wu,Chao Zhang,Xinluona Su,Ruhui Shi,Weiwei Lin,Yan Li,Fengyu Zhao
Graphical Stability from the support : The excellent stability of a Ru/ZSM-5 catalyst for levulinic acid hydrogenation in water relies on the higher tetrahedral-coordinated Al content and preferable pore connectivity in well-crystallized ZSM-5 zeolite, which suppress Ru aggregation and leaching and the formation of carbonaceous residues in the acidic environment. A long-life topic in the field of heterogeneous catalysis has been to develop supported catalysts that are stable against the aggregation of active metal and carbon deposition. Herein, we report a highly stable Ru/ZSM-5 catalyst for the hydrogenation of levulinic acid in water, which can be recycled at least 10 times without apparent loss of activity (conv. >95 %, yield >85 %). The influences of types of Al species, structure of support, Ru sizes, Ru leaching, and carbon deposition, etc. on activity and stability were discussed in detail. It was confirmed that the tetrahedral-coordinated framework Al in ZSM-5 contributed to the favorable metal–support interaction, and thus suppressed the aggregation and leaching of ruthenium during recycling. Besides, the suitable pore volume and channel network connectivity successfully prevent from deposition of carbonaceous residues.
研究领域:
催化化学
·
材料科学
✓ 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）