燃料化学学报Pub Date : 2024-03-01DOI: 10.1016/S1872-5813(23)60395-0
Pengyu REN , Zhuo LIU , Yanhong QUAN , Junjun GUO , Hong MA , Jianbing WU , Yongzhao WANG
{"title":"Theoretical calculation study on the reaction mechanism of methanol/dimethyl ether carbonylation catalyzed by the B/Al/Ga-MOR zeolites","authors":"Pengyu REN , Zhuo LIU , Yanhong QUAN , Junjun GUO , Hong MA , Jianbing WU , Yongzhao WANG","doi":"10.1016/S1872-5813(23)60395-0","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60395-0","url":null,"abstract":"<div><p>The reaction mechanism of methanol/dimethyl ether (DME) carbonylation catalyzed by isomorphously substituted B-, Al-, and Ga-MOR zeolites (B/Al/Ga-MOR) was comparatively investigated by the density functional theory (DFT) calculations. The commonalities and differences between methanol and dimethyl ether as the reactant as well as among various MOR zeolites in the catalytic reaction pathways were disclosed, where one Si atom was substituted by B, Al or Ga at the 8-ring side pockets T3 sites or the 12-ring channels T4 sites of MOR. The results indicate that the insertion of CO into methoxy group to form acetyl groups follows the S<sub>N</sub>2 mechanism and is the rate-determining step in the carbonylation reactions. Under 473 K, either methanol or dimethyl ether is used as feedstock, the formed acetyl group prefers to interact with CH<sub>3</sub>O in methanol to form methyl acetate. The T3 sites show better carbonylation selectivity, whereas T4 sites display better trimethoxonium ions selectivity which favors the generation of aromatics and leads to the catalyst deactivation. Comparing with Al-MOR, the introduction of Ga and B at the T3 sites increases the free energy barriers of carbonylation, whereas the introduction of Ga and B in particular at the T4 sites can substantially increase the energy barriers of generating trimethyloxonium ions, which can effectively suppress the side reaction and improve the catalyst stability. This work contributes to the understanding of the catalytic roles of various acidic sites in different channels of the MOR zeolites and provides certain theoretical support for tailoring and designing efficient MOR zeolite catalysts for methanol/dimethyl ether carbonylation.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 3","pages":"Pages 323-334"},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140123094","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-03-01DOI: 10.1016/S1872-5813(23)60388-3
Yang LI, Bo XU, He YANG, Lijun JIN, Haoquan HU
{"title":"Promotion of Cu/Ce supported red mud for NO removal from low and medium temperature flue gas","authors":"Yang LI, Bo XU, He YANG, Lijun JIN, Haoquan HU","doi":"10.1016/S1872-5813(23)60388-3","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60388-3","url":null,"abstract":"<div><p>Red mud is a solid waste in aluminum industry and has been proven to be an efficient alternative to NO<sub><em>x</em></sub> selective catalytic reduction (SCR) catalysts. Acid washing treatment to red mud can improve its alkalinity and surface properties, and increase the conversion rate of NO<sub><em>x</em></sub>. In this paper, Cu, Ce, and Cu/Ce was supported on acid washed red mud and NO<sub><em>x</em></sub> catalytic conversion performance on metal modified red mud catalysts was studied. The research results indicate that Cu<sup>+</sup> and Cu<sup>2+</sup> in the Cu supported catalyst effectively promote NO conversion rate of red mud in low-temperature (200–300 °C) flue gas, reaching a maximum of 90.7%; Ce<sup>3+</sup> and Ce<sup>4+</sup> in Ce supported catalysts effectively promote the NO conversion rate of red mud in flue gas at 200–400 °C, reaching a maximum of 94.0%; Cu/Ce supporting exhibits better NO conversion rate than single metal supported catalysts at low-temperatures, the optimal Cu:Ce ratio for supporting is 1:1; and also exhibits better NO conversion rate than Cu supported catalysts at high-temperature (300–400 °C), reaching a maximum of 95.5%. The reason may be that under the synergistic effect of Cu/Ce, ACRM-Cu1Ce1 has stronger low-temperature redox ability, higher weak acidic peaks, higher average oxidation state of Fe ions, and higher Cu<sup>+</sup> content.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 3","pages":"Pages 362-371"},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140123095","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-03-01DOI: 10.1016/S1872-5813(23)60385-8
Youhua ZUO , Hui WU , Junfeng HUA , Junning ZHENG , Lixin XU , Mingfu YE , Chao WAN
{"title":"Preparation of layered porous carbon supported ruthenium catalyst and its performance for ammonia borane hydrolyzing to hydrogen","authors":"Youhua ZUO , Hui WU , Junfeng HUA , Junning ZHENG , Lixin XU , Mingfu YE , Chao WAN","doi":"10.1016/S1872-5813(23)60385-8","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60385-8","url":null,"abstract":"<div><p>In this paper, layered porous carbon sheet (LPCS) was obtained through high temperature calcination under argon atmosphere by using coal pitch as carbon material, sodium chloride as template agent and potassium carbonate as activator. Then, the active component Ru was loaded onto the LPCS support by impregnation to synthesize Ru/LPCS catalyst whose catalytic performance for hydrogen production by hydrolysis of ammonia borane was studied. The results showed that in the presence of light, the maximum value of the turnover frequency (TOF), 334.8 min<sup>–1</sup>, was obtained at a calcination temperature of 1123 K and a loading of 2% of Ru which is 1.38 times higher than that in the absence of light. The activation energy (<em>E</em><sub>a</sub>) of the catalyst decreased from 90.60 to 70.33 kJ/mol in the presence of light. The hydrogen production rate order with respect to ammonia borane concentration was 0.75, which is first-order relation to the amount of the catalyst.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 3","pages":"Pages 430-437"},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140123097","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Preparation of Ag+ modified NaY molecular sieve and its adsorption and denitrogenation properties","authors":"Tian FU, Xin HONG, Yu TIAN, Xiaodi SUN, Jucai WANG, Ke TANG, Xiuyang LUAN","doi":"10.1016/S1872-5813(23)60386-X","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60386-X","url":null,"abstract":"<div><p>An AgY molecular sieve modified by Ag<sup>+</sup> ion was characterized by XRD, FT-IR and N<sub>2</sub> adsorption and desorption and used to the adsorption denitrogenation from model fuels containing pyridine, aniline and quinoline basic nitrides. The adsorption capacity for N with the AgY molecular sieve was obviously better than that with the NaY molecular sieve. The effects of adsorption temperature and adsorption time on the adsorption capacity of three kinds of nitrides by AgY molecular sieve were investigated. The experimental results show that the adsorption capacity for N is aniline>quinoline>pyridine. To study the adsorption mechanism of AgY, the 12T cluster model of AgY molecular sieve was established by Materials Studio software and the adsorption of three kinds of nitride molecules on the AgY molecular sieve was simulated at 303, 323 and 343 K. The adsorption energy, the distance between the active center and pyridine, aniline and quinoline molecules, the frontier orbit, the isodensity distribution, the radial distribution function and other relevant parameters were calculated. The calculated results show that the adsorption of aniline by AgY molecular sieve is better than that of quinoline and pyridine, which is consistent with the experimental results. Moreover, the adsorption is mainly the chemical adsorption, and the S and W sites of AgY molecular sieve are the main adsorption sites. The results of isothermal adsorption show that the adsorption of pyridine on the AgY follows the Langmuir-Freundlich mixed adsorption model, and the adsorption of aniline and quinoline follows the Freundlich adsorption model. The results of adsorption kinetics and thermodynamics show that the adsorption of pyridine on the AgY molecular sieve conforms to the quasi-second-order kinetic model, while the adsorption of aniline and quinoline conforms to the quasi-first-order kinetic model, and all adsorption processes are spontaneous entropy increasing process.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 3","pages":"Pages 384-394"},"PeriodicalIF":0.0,"publicationDate":"2024-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140123096","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-02-01DOI: 10.1016/S1872-5813(23)60372-X
Huimin ZHOU , Nuannuan YANG , Haichao FU , Meijun WANG , Yanfeng SHEN , Dong LIU , Jiancheng WANG , Liping CHANG
{"title":"Effect of KOH addition on electrochemical properties of coal-based active carbon foams","authors":"Huimin ZHOU , Nuannuan YANG , Haichao FU , Meijun WANG , Yanfeng SHEN , Dong LIU , Jiancheng WANG , Liping CHANG","doi":"10.1016/S1872-5813(23)60372-X","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60372-X","url":null,"abstract":"<div><p>Using strong-caking coking coal as raw material, coal-based carbon foam (NCF) was prepared by constant pressing and self-foaming method and used as carbon base to produce coal-based active carbon foamed (HPCs) together with KOH activator, which was used as electrode material for double-layer capacitor. The effects of KOH added by mechanical mixing, aqueous solution impregnation and ethanol solution impregnation methods on microstructure and electrochemical properties of the prepared materials were studied. The results show that formation of pore structure, crystal structure, surface chemistry and electrochemical performance of HPCs are significantly affected by KOH dispersion and adhesion. The NCF itself has a three-dimensional connected bubble pore structure, which is conducive to the activator (KOH) penetrating into the bubble pore and providing a large number of attachment sites, thus increasing the contact area between the activator and the carbon matrix and resulting in efficient activation. The good fluidity of KOH solution can make K<sup>+</sup> more effectively interspersed in the bubble structure of NCF, act on the defect site during activation, and generate more micropores and mesoporous structures on the internal matrix of carbon matrix, effectively amplifying the activation effect. ACF-W obtained by KOH aqueous impregnation has the highest specific surface area (3098.35 m<sup>2</sup>/g), total pore volume (1.68 cm<sup>3</sup>/g), mesoporous volume ratio (59.13%). It shows excellent specific capacitance (310 F/g) and cycle stability when used as electrode material.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 2","pages":"Pages 249-264"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139714448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-02-01DOI: 10.1016/S1872-5813(23)60389-5
Guosheng LI , Kunhong LI , Xiaohan LI , Xinrui YIN , Jiaxin SHAO , Rong GUO , Shenyong REN , Qiaoxia GUO , Baojian SHEN
{"title":"Acidity regulation of Fe-based catalysts and its effect on the selectivity of HDS reaction pathways","authors":"Guosheng LI , Kunhong LI , Xiaohan LI , Xinrui YIN , Jiaxin SHAO , Rong GUO , Shenyong REN , Qiaoxia GUO , Baojian SHEN","doi":"10.1016/S1872-5813(23)60389-5","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60389-5","url":null,"abstract":"<div><p>An Fe-based hydrodesulfurization (HDS) catalyst modified by Y zeolite was developed using Fe as the main active metal and Zn as a promoter. The change of morphology, pore structure, dispersity, reducibility, electronic defect structure and acidity of the Fe-based catalysts before and after modification were investigated using low-temperature nitrogen physical adsorption, X-ray diffraction (XRD), H<sub>2</sub>-temperature programmed reduction (H<sub>2</sub>-TPR), NH<sub>3</sub>-temperature programmed desorption (NH<sub>3</sub>-TPD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and pyridine infrared spectroscopy (Py-IR). Meanwhile, the HDS performance of the Fe-based catalyst was evaluated using a fixed-bed reactor. The results showed that the introduction of Y zeolite provided the Brønsted (B) acid sites, which increased the sulfur removal rates of Fe based catalysts by 10.7%–34.1%. Meanwhile, the B acid sites improved the selectivity of the direct desulfurization (DDS) reaction pathway. In addition, the B acid sites not only promoted the increase of DDS selectivity but also inhibited further deep hydrogenation of tetrahydrodibenzothiophene (THDBT) and hexahydrodibenzothiophene (HHDBT) in the hydrogenation (HYD) reaction pathway, thereby ensuring an increase in desulfurization efficiency while reducing hydrogen consumption. The fundamental reason was that the introduction of Y zeolite enhanced the acidity of the modified catalyst, especially the interaction between B acid sites and active metal promoted electron transfer, which adjusted the electronic defect structure of Fe species, resulting in the improvement of HDS performance.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 2","pages":"Pages 234-247"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139714447","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-02-01DOI: 10.1016/S1872-5813(23)60384-1
Huanhuan XU , Yihu KE
{"title":"Synthesis of glycerol carbonate from glycerol and CO2 over Cu-Zr complex oxide","authors":"Huanhuan XU , Yihu KE","doi":"10.1016/S1872-5813(23)60384-1","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60384-1","url":null,"abstract":"<div><p>A series of Cu<sub>1–<em>x</em></sub>Zr<sub><em>x</em></sub>O<sub>2</sub> bimetallic oxides with different Cu-Zr molar ratios for glycerol carbonate synthesis from glycerol and CO<sub>2</sub> were prepared by hydrothermal method. The results found that the performance was significantly affected by the Zr doping amounts. Under the optimal reaction conditions, the Cu<sub>0.99</sub>Zr<sub>0.01</sub>O<sub>2</sub> catalyst had the best catalytic performance. The conversion of glycerol and the selectivity of glycerol carbonate reached 64.1% and 85.9%, respectively. Cu<sub>1–<em>x</em></sub>Zr<sub><em>x</em></sub>O<sub>2</sub> complex oxide exhibited better activity than pure CuO and pure ZrO<sub>2</sub>. The structures, morphologies and surface properties of the catalysts were characterized by X-ray powder diffraction (XRD), Scanning electron microscopy (SEM), Transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), N<sub>2</sub> adsorption and desorption, Temperature programmed reduction (H<sub>2</sub>-TPR), Temperature programmed desorption (TPD) and Fourier Transform Infrared Spectroscopy (FT-IR). It is speculated that the high activity is related to the degree of dispersion of Zr on the surface of CuO, the surface content of oxygen species and the number of acidic-basic sites. In addition, catalytic activity did not change significantly after six cycles, indicating the excellent stability of the catalyst.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 2","pages":"Pages 171-182"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139714443","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Catalytic performance of La-modified Cu/SiO2 in the hydrogenation of methyl acetate","authors":"Chuanming ZHANG, Weijie LI, Jincan KANG, Lina LIN, Changxin LI, Lincai LI, Haoyu ZOU, Hongping ZHU","doi":"10.1016/S1872-5813(23)60382-2","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60382-2","url":null,"abstract":"<div><p>A series of Cu/SiO<sub>2</sub> catalysts modified with lanthanum (La) (30Cu-<em>n</em>La/SiO<sub>2</sub>, <em>n</em>=0, 0.5, 1 and 2) were synthesized using the ethanol (EtOH)-assisted ammonia-evaporation method; their catalytic performance in the gas-phase hydrogenation of methyl acetate (MeOAc) to produce ethanol (EtOH) was investigated. The results indicate that the catalytic performance of Cu/SiO<sub>2</sub> can be greatly enhanced by La modification. In particular, the 30Cu-0.5La/SiO<sub>2</sub> catalyst exhibits excellent performance in the MeOAc hydrogenation; under 230 °C, 2 MPa H<sub>2</sub>, an LHSV of 2 h<sup>-1</sup> and an H<sub>2</sub>/MeOAc molar ratio of 20, the MeOAc conversion reaches 98.5%, with a total EtOH yield of 97.0%. The N<sub>2</sub>-sorption, XRD, ICP-OES, H<sub>2</sub>-TPR, FT-IR, TEM, XPS, and AES characterization results reveal that the introduced La metal has a strong interaction with Cu, which can promote the dispersion of the copper species on the SiO<sub>2</sub> support. Moreover, the content of Cu<sup>+</sup> is increased significantly, which can enhance the electronic interaction with MeOAc via the acyl and methoxide groups and thus promote the hydrogenation of MeOAc to EtOH.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 2","pages":"Pages 131-139"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139714449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Effect of Ce modification on the performance of CuLDH catalyst for CO2 hydrogenation to methanol","authors":"Haoran LIU , Zhiqing YU , Wenbin HUANG , Qiang WEI , Peng JIANG , Yasong ZHOU","doi":"10.1016/S1872-5813(23)60392-5","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60392-5","url":null,"abstract":"<div><p>A series of Ce modified CuLDH-Ce<sub><em>x</em></sub> catalysts were synthesized by adding different amounts of Ce to CuMgAl hydrotalcite (CuLDH) catalysts. The physicochemical properties of the catalysts were characterized by X-ray diffraction (XRD), N<sub>2</sub> adsorption-desorption (BET), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), etc. The results showed that the addition of Ce changed the hydrotalcite structure of CuLDH catalyst, and an appropriate amount of Ce increased the surface area of the catalyst and improved the dispersion of Cu particles. At the same time, an appropriate amount of Ce was beneficial for increasing the density of strong alkaline sites and the number of oxygen vacancies on the catalyst surface, promoting the adsorption and conversion of CO<sub>2</sub>. Ce was beneficial for adjusting the Cu<sup>+</sup>/Cu<sup>0</sup> ratio on the catalyst surface, and a higher Cu<sup>+</sup>/Cu<sup>0</sup> ratio was conducive to the formation of methanol. When the Ce/Cu ratio was 0.3, the catalyst exhibited higher activity with 7.5% CO<sub>2</sub> conversion, 78.4% methanol selectivity and 362.8 g/(kg·h) spatiotemporal yield at 240 °C under 2.5 MPa with a GHSV=9000 mL/(g·h). It was proved by <em>in-situ</em> DRIFTS that CuLDH-Ce0.3 catalyst followed HCOO* reaction path during CO<sub>2</sub> hydrogenation for methanol.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 2","pages":"Pages 159-170"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139714442","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-02-01DOI: 10.1016/S1872-5813(23)60383-4
Rui FENG , Zhou FANG , Peng ZHOU , Tianbo LI , Xiaoyan HU , Xinlong YAN , Zhongdong ZHANG
{"title":"Regulation of the Lewis acidity on matrix and their performance in the catalytic cracking of light hydrocarbons","authors":"Rui FENG , Zhou FANG , Peng ZHOU , Tianbo LI , Xiaoyan HU , Xinlong YAN , Zhongdong ZHANG","doi":"10.1016/S1872-5813(23)60383-4","DOIUrl":"https://doi.org/10.1016/S1872-5813(23)60383-4","url":null,"abstract":"<div><p>The reasonable matching of zeolite and matrix is one of the most effective strategies to increase the yield of light olefins in naphtha catalytic cracking. However, the influence of the surface Lewis acidity within the matrix on the cracking reactions has remained ambiguous. Therefore, in present study, boron and zinc co-modified γ-Al<sub>2</sub>O<sub>3</sub> and tin modified mesoporous silica KIT-6 with tuned surface Lewis acidity were applied to evaluate the cracking reactivity of <em>n</em>-heptane and 1-hexene to light olefins, in which the matrix was used alone and coupled with ZSM-5 zeolite in different packed modes. The effects of the modifiers on the textural properties and surface acidity of γ-Al<sub>2</sub>O<sub>3</sub> and KIT-6 were investigated by XRD, TEM, N<sub>2</sub> physical absorption-desorption, and NH<sub>3</sub>-TPD. The results showed that B doping reduced the Lewis acidity (both in the amount and acid strength) of γ-Al<sub>2</sub>O<sub>3</sub>, while the incorporation of Zn doping led to increased Lewis acidity. In addition, the Lewis acidity of ordered mesoporous KIT-6 increased as Sn doping rose. While for pure matrix, the ascend in conversions of <em>n</em>-heptane and 1-hexene was consistent with the increased Lewis acidity of the B and Zn co-modified γ-Al<sub>2</sub>O<sub>3</sub> and <em>x</em>Sn/KIT-6 rose, along with decreased activation energy. In contrast, when coupled with ZSM-5 zeolite, the highest conversion was achieved in the dual-bed manner of matrix and zeolite, and the conversion increased concomitantly with the increase in the Lewis acidity of the matrix. However, excessive Lewis acidity can accelerate the hydrogen transfer rate while diminishing the selectivity of light olefins.</p></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 2","pages":"Pages 218-231"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139714444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}