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JOURNAL OF SOLID STATE CHEMISTRY · 2021 · IF 3.498

Effect of morphology and acidity control of Ni-SAPO-34 zeolite on catalytic performance of dimethyl ether to olefins

Shichao Zhang,Wenbin Chen,Ling Yang,Tong Xie,Weike Li,Daoke Yu,Yiwen Fang

SAPO-34 molecular sieve is one of the main catalysts for DMTO reaction and shows excellent catalytic performance. In this work, a series of Ni-SAPO-34 molecular sieve with different crystal morphologies , such as cubic, melting angle cube , spherical, polygon cube, were synthesized using Ni-DETA as a structure-directing agent. We explored the influence of Ni-DETA structure-directing agent on the formation of crystal morphology, and found that the different morphology is related to the amount of Ni-DETA introduced, and also had an impact on the acidity of the Ni-SAPO-34 molecular sieve. The properties of these samples were characterized by SEM, XRD , EDS, UV–Vis, FT-IR, NH 3 -TPD and N 2 physicalsorption. The synthesized polygonal cubic Ni-SAPO-34 molecular sieve has lower strong acidity due to the introduction of a small amount of nickel, which is beneficial to reduce the production of carbon deposits and improve the catalytic reaction activity. Moreover, the multi-edge morphology and hierarchical porous structure are also advantageous to the catalytic reaction. The polygon cube Ni-SAPO-34 catalysts display the highest DTO catalytic performance, and the total selectivity of ethylene and propylene can reach 83.76%.

研究领域: 化学工程 · 材料科学
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JOURNAL OF POROUS MATERIALS · 2022 ·Vol. 29 ·期 5 ·1387-1398 · IF 2.523

In situ synthesis of mesoporous Pt/SAPO–11 for the preparation of biological aviation kerosene

Ma Jingye,Liu Xiaolong,Yuan Hong

This work employed dodecyl trimethyl ammonium bromide, sodium dodecyl benzene sulfonate (SDBS) or dodecyl dimethyl betaine (BS–12) along with a PEO–PPO–PEO (P123) block copolymer to obtain a dual template system for catalyst synthesis. Using Pt(NH 3 ) 4 (NO 3 ) 2 as the platinum source, a series of mesoporous Pt/SAPO–11 catalysts with different Pt loadings were prepared via an in situ synthesis and characterized by X-ray diffraction, specific surface area analysis, temperature programmed desorption, X-ray photoelectron spectroscopy and transmission electron microscopy. These catalysts each had a complete AEL model structure with pore diameters in the range of 8.1–10.9 nm and specific surface areas between 103 and 168 m 2 /g. At a Pt loading of 1.0 wt%, the Pt/SAPO–11–S synthesized with SDBS–P123 as the dual template showed the least Pt loss, the largest specific surface area (159 m 2 /g) and the smallest Pt particle size (6.1 nm). This material also exhibited the highest ratio of Pt metal to oxide, indicating that it contained more active metal sites. This catalyst was applied to the decarboxylation of oleic acid under CO 2 to prepare C8–C17 alkanes, the main component of biological aviation kerosene. At a reaction temperature of 340 °C and catalyst-to-oil mass ratio of 1:10, the yield of C8–C17 alkanes reached 80.6% after 6 h. This same catalyst provided a 73.8% yield after six reuses, demonstrating good stability.

研究领域: 催化化学 · 能源化学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2025 · IF 3.7

Enhanced activity and stability of SAPO-5 zeolite supported RuMn catalyst for aqueous-phase selective hydrodeoxygenation of guaiacol to cyclohexanol

Mengting Chen,Minjie Zhu,Tingyu Zhou,Qifeng Zhong,Meihua Zhang,Yingxin Liu,Zuojun Wei

SAPO-5 zeolite supported RuMn was a highly efficient catalyst for the aqueous-phase selective hydrodeoxygenation of guaiacol to cyclohexanol. The optimal catalyst achieved a high cyclohexanol yield of 93.7% at full guaiacol conversion under mild conditions, with a high TOF of 920 h -1 . Moreover, the catalyst displayed remarkable performance for the hydrogenation of phenol to cyclohexanol, where a 100% yield of cyclohexanol was obtained at a phenol-to-Ru molar ratio of about 17900. In particular, the catalyst exhibited excellent recyclability and could be recycled for 20 times without obvious activity loss. The as-prepared RuMn/SAPO-5 catalyst exhibited higher performance than most of the reported Ru-based catalysts.

研究领域: 催化化学 · 能源化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

One-pot in situ synthesis of Cu-SAPO-34/SiC catalytic membrane with enhanced binding strength and chemical resistance for combined removal of NO and dust

Jiahao Chen,Bin Wang,Kai Yuan,Yutang Kang,Shasha Feng,Feng Han,Hongmiao Wu,Rongfei Zhou,Zhaoxiang Zhong,Yiqun Fan,Weihong Xing

The SiC catalytic membrane combining dust removal and denitration can realize the efficacious treatment of atmospheric pollutants. Unfortunately, a large amount of SiO 2 , formed by the partial oxidation of SiC at a high temperature, results in the decreased chemical resistance of SiC catalytic membrane. In addition, the complicated preparation processes and susceptible to loss of catalytic components under harsh conditions restrict the industrial application of SiC catalytic membranes. Here, the Cu-SAPO-34(D)/SiC catalytic membranes were directly prepared via a facile one-pot hydrothermal synthesis method, which ingeniously utilized the generated SiO 2 as a Si source to participate in the growth of Cu-SAPO-34 zeolites. Excellent binding strength and chemical resistance were simultaneously realized for the SiC catalytic membranes. As a comparison, a Cu-SAPO-34(I)/SiC catalytic membrane was fabricated via the conventional two-step ion-exchange method. The 0.2 Cu-SAPO-34(D)/SiC (Cu molar ratio of 0.2) achieved the best NH 3 -SCR performance among the prepared catalytic membranes for its highly active copper and oxygen species, abundant Lewis acid sites and remarkable redox capacity. When implementing the simultaneous removal of NO and PM, the 0.2 Cu-SAPO-34(D)/SiC catalytic membrane achieved a high NO degradation performance of 98% from 200 to 280 °C, coupled with an excellent PM 0.3 (model dust with average size of 300 nm) filtration performance of 99.99%. These results were better than those of the Cu-SAPO-34(I)/SiC catalytic membrane (92% for NO degradation and 99.98% for PM 0.3 filtration). The one-pot in situ synthesis of Cu-SAPO-34(D)/SiC catalytic membrane with enhanced binding strength and chemical resistance provides a novel strategy for preparation of high-performance SiC catalytic membrane with double benefits.

研究领域: 环境科学 · 材料科学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2015 · IF 3.453

Hydrothermal preparation of hierarchical SAPO-34 constructed by nano-sheets using rapeseed pollen extract as water and its CO2 adsorption property

Jie Gong,Chongqing Wang,Changfeng Zeng,Lixiong Zhang

Herein we report a biosynthesis route to prepare hierarchical SAPO-34 constructed by numerous nano-sheets. Rapeseed pollen extract was used as water to prepare the synthesis solution, which underwent hydrothermal synthesis to obtain the hierarchical SAPO-34. The product is characterized by XRD , FT-IR, SEM, N 2 adsorption–desorption and TG analysis . The hierarchical SAPO-34 shows a distinctive morphology with curly nano-sheets and gaps between nano-sheets, forming a blooming flower-like structure. Its specific surface area is 683 m 2  g −1 . The effect of the content of rapeseed pollen suspension was examined. Increasing in the content leads to the formation of the hierarchical SAPO-34 constructed with curlier and much more numbers of nano-sheets. The formation process of SAPO-34 was investigated and a possible formation mechanism was proposed. Such hierarchical SAPO-34 exhibits a high CO 2 adsorption capacity of 2.77 mmol/g at 100 kPa and the CO 2 /CH 4 ideal separation factor of 8.2. It takes 6.1 min for CO 2 to reach the adsorption equilibrium, which is faster than that of conventional SAPO-34, possibly due to such nano-sheet-constructed fine structure.

研究领域: 材料科学 · 环境科学
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Journal of Physical Chemistry C · 2024 · IF 3.3

Insights into Migration and Transformation of Cu Species during SO2 Poisoning and Hydrothermal Aging of Cu/SAPO-34 NH3–SCR Catalysts

Fumei Wang,Qi Cai,Xinhua He,Boxiong Shen,Leila Negahdar,Shuo Feng,Andrew M. Beale

Cu/SAPO-34 catalysts have been widely used for the reduction of NOx from diesel exhaust by ammonia-selective catalytic reduction (SCR). Sulfur poisoning remains a challenge for Cu/SAPO-34 catalysts in NH3–SCR, restricting its application. In this study, Cu/SAPO-34 samples containing a mixture of Cu species comprising isolated Cu2+ located in the 6MR, Cu(OH)+ in 8MR, CuO clusters/nanoparticles, and Cu+ species were prepared. The Cu speciation during SO2 and hydrothermal aging of Cu/SAPO-34 SCR catalysts was subsequently studied. While hydrothermal aging had little effect on catalytic activity, the sulfur-aged sample exhibited deterioration in NH3–SCR activity over the temperature range of 100–575 °C. The breakage and collapse of the zeotype framework and chemical deactivation of the Cu/SAPO-34 catalyst after exposure to SO2 and H2O took place. A combination of X-ray photoelectron spectroscopy (XPS) and TGA-DT-DSC revealed the presence of ammonium bisulfate, copper bisulfate/sulfate, aluminum sulfate, and sulfuric acid after SO2 and H2O copoisoning under SCR conditions. Furthermore, Cu(OH)+ tended to migrate to form isolated Cu2+ and Cu+, as well as agglomerate to form CuO particles. Density functional theory (DFT) calculations revealed that SO2 and O2 could readily be absorbed by CuO particles to form stable copper bisulfate/sulfate species with the following order of preference: CuO > Cu+ > Cu2+ > Cu(OH)+. In contrast, Cu(OH)+ was less prone to be poisoned by easily releasing SO3 than other Cu species sites.

研究领域: 环境科学 · 催化化学
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY · 2019 · IF 3.261

Enhanced photo-Fenton degradation performance over multi-metal co-supported SAPO-18 zeolites by promoted active species yield

Xi Li,Zhengang Tian,Kun Liang,Yuhua Wang

Fe, Mn co-supported SAPO-18 zeolite was synthesized via ion-exchange method and exhibited high performance in catalytic degradation of methyl orange (MO). The bimetallic Fe-Mn/SAPO-18 catalyst showed almost 100% MO (50 mg/L) removal within 20 min, which was superior to the MO degradation efficiency over monometallic Fe or Mn catalysts. The hydroxyl group (OH ) generated in the photo-Fenton catalysis was determined by fluorescence probe and the corresponding reaction mechanism was explored. We proposed that the light and synergistic effect of bimetal promote the conversion of metal ion valence, thereby enhancing the generation of the active species and the degradation efficiency of MO. Furthermore, the influences of some essential factors on MO degradation rate were investigated. The results indicated that the pH of the solution plays an important role in Fenton degradation of MO. 100% MO degradation is achieved within 10 min when the initial pH is set at 2–3 under UV for Fe-Mn/SAPO-18. Moreover, it also shows good performance under neutral conditions, thus exhibits considerable activity at expanded pH range. And the concentrations of H 2 O 2 and MO solution and the dosage of catalysts can influence the degradation rate of dyes. This work not only made significant progress on the development of high-performance catalysts for the degradation of MO, but also provided a direction for the study of organic contaminant degradation.

研究领域: 环境科学 · 催化材料 · 污染控制
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CATALYSIS TODAY · 2022 · IF 6.562

PtCo nanoparticles supported on hierarchical SAPO-34 for hydrolysis of ammonia borane and tandem reduction of 4-nitrophenol

Wenwen Cong,Changyou Xu,Yahang Mu,Qiang Li,Liancheng Bing,Fang Wang,Dezhi Han,Guangjian Wang

In this work, hierarchical SAPO-34 supported PtCo bimetallic catalysts with different Pt/Co ratios were prepared by impregnation method. The obtained PtCo/SAPO-34 catalysts displayed high catalytic activities and durability for the dehydrogenation of ammonia borane (AB). Among them, Pt 1 Co 5 /SAPO-34 catalyst delivered the highest hydrogen generation activity with a turnover frequency (TOF) of 262 mol H 2 ( mol Pt ∙ min ) − 1 molH2(molPt∙min)−1 at 303 K as well as excellent catalytic activity in catalytic hydrogenation of 4-nitrophenol (4-NP) by coupling with hydrolytic dehydrogenation of AB, due to the electron interaction of Pt and Co in PtCo alloy and the high metal dispersion and exposure of Brønsted acidic sites on SAPO-34 support. Moreover, it is noteworthy that the prepared Pt 1 Co 5 /SAPO-34 catalyst also exhibited superior recycle stability, with 81% of the initial TOF value after five runs of hydrolysis reaction.

CAS / MDL: 100-02-7
研究领域: 材料科学 · 催化化学
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Catalysts · 2021 ·Vol. 11 ·期 3 ·314 · IF 4.146

MnOx Supported on Hierarchical SAPO-34 for the Low-Temperature Selective Catalytic Reduction of NO with NH3: Catalytic Activity and SO2 Resistance

Lusha Zhou,Jinkun Guan,Chenglong Yu,Bichun Huang

The ethanol dispersion method was employed to synthesize a series of MnOx/SAPO-34 catalysts using SAPO-34 with the hierarchical pore structure as the zeolite carrier, which were prepared by facile acid treatment with citric acid. Physicochemical properties of catalysts were characterized by XRD, XPS, BET, TEM, NH3-TPD, SEM, FT-IR, Py-IR, H2-TRP and TG/DTG. NH3-SCR performances of the hierarchical MnOx/SAPO-34 catalysts were evaluated at low temperatures. Results show that citric acid etching solution at a concentration of 0.1 mol/L yielded a hierarchical MnOx/SAPO-34-0.1 catalyst withca.15 wt.% Mn loading, exhibiting optimal catalytic activity and SO2tolerance at low temperatures. Almost 100% NO conversion and over 90% N2selectivity at 120 °C under a gas hourly space velocity (GHSV) of 40,000 h−1could be obtained over this sample. Furthermore, the NO conversion was still higher than 65% when 100 ppm SO2was introduced to the reaction gas for 4 h. These could be primarily attributed to the large specific surface area, high surface acidity concentration and abundant chemisorbed oxygen species provided by the hierarchical pore structure, which could also increase the mass transfer of the reaction gas. This finding suggests that the NH3-SCR activity and SO2poisoning tolerance of hierarchical MnOx/SAPO-34 catalysts at low temperatures can be improved by controlling the morphology of the catalysts, which might supply a rational strategy for the design and synthesis of Mn-based SCR catalysts.

研究领域: 催化化学 · 环境科学
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JOURNAL OF POROUS MATERIALS · 2024 · IF 2.5

Synthesizing hierarchically porous SAPO-11 with polyvinyl alcohol phosphates as mesopore template: effects of phosphorus content and concentration of templates

Wang Chuangye,Liu Huili,Xue Jintang,Sun Ruixue,Song Xinrong,Zhang Xinyi,Zhang Longli

Introducing the second mesopores into SAPO-11 molecular sieve will be much helpful to improve the catalytic performance of its metal-supported catalysts in hydroisomerization of normal alkanes. In current paper, polyvinyl alcohol phosphates with different phosphorus contents were prepared and employed as mesopore template to prepare hierarchical SAPO-11. The effects of phosphorus content and concentration on the properties including mesopore structure, acidity and morphology of the prepared SAPO-11s have been investigated. The results showed that with appropriate phosphorus content and template concentration, PPVAs efficiently directed the generation of regular mesopore structure, extended the surface area and improved the acidity of the SAPO-11 molecular sieves. Pt/SAPO-11 bi-functional catalysts were prepared and their catalytic performances in hydroisomerization of n-hexane were evaluated. The highest conversion read 59.3%, while the optimal selectivity of branched hexanes was 86.5%.

研究领域: 催化材料 · 化学工程
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ACS Omega · 2019 · IF 2.584

Effect of Metal Precursors on the Performance of Pt/SAPO-11 Catalysts for n-Dodecane Hydroisomerization

Lili Geng,Jianjun Gong,Guilong Qiao,Songshou Ye,Jinbao Zheng,Nuowei Zhang,Binghui Chen

Pt(NH3)4(NO3)2, Pt(NH3)4(Ac)2, (NH4)2PtCl4, and H2PtCl6 were used to prepare Pt/SAPO-11 catalysts to investigate the effect of Pt precursors on the hydroisomerization of n-dodecane. The catalyst derived from Pt(NH3)4(NO3)2 displays the best hydroisomerization activity and selectivity among these precursors. The hydroisomerization conversion of n-dodecane is affected by the platinum particle size, platinum dispersion, the location of platinum, and the valence state of platinum. The selectivity of n-dodecane is determined by the number of Brønsted acid sites and Pt crystal planes. These conclusions are verified by combining transmission electron microscopy, high-resolution transmission electron microscopy, hydrogen temperature programmed reduction, NH3-temperature programmed desorption, and Py-IR studies. The catalyst prepared with Pt(NH3)4(NO3)2 as the precursor exhibits the smallest platinum particle size and the highest platinum dispersion. Most of the platinum particles are supported on the external surface of SAPO-11 with the Pt(111) crystal face. Such a catalyst also possesses a suitable number of Brønsted acid sites and then displays the best catalytic performance. Obviously, the use of various precursors for the Pt-based catalyst can significantly affect the performance of Pt/SAPO-11 for the hydroisomerization of n-dodecane.

研究领域: 催化化学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 38 ·18070-18081 · IF 3.591

Synthesis of mesoporous Pt@SAPO-11 via in situ encapsulation for the decarboxylation of oleic acid to prepare C8–C17 alkanes

Xiaolong Liu,Jingye Ma,Hong Yuan

A series of mesoporous Pt@SAPO-11 catalysts with different Pt loadings were prepared using an in situ encapsulation process. These materials exhibited good topological structures and high Brunauer–Emmett–Teller (BET) surface areas (132–166 m2 g−1). Transmission electron microscopy images showed that the Pt nanoparticles in this material were in the 5–8 nm size range and were highly dispersed on the inner surfaces of the SAPO-11 support. N2-BET analyses demonstrated that the samples had mesoporous structures with average pore sizes of 7.3–8.5 nm. Characterization of the 1.0 wt% Pt@SAPO-11 catalyst by X-ray photoelectron spectroscopy and H2-temperature programmed reduction indicated strong interactions between the Pt nanoparticles and the carrier. This material was used to promote oleic acid decarboxylation under CO2 and gave a C8–C17 alkane yield of 80.8% after 4 h at 340 °C. After five repeated uses, the catalyst still gave a yield of 77.6%.

研究领域: 催化化学 · 材料科学
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