CATALYSIS LETTERS
·
2021
·Vol. 152
·期 6
·1651-1659
·
IF 3.186
Tao Lei,Zhang Xueliang,Song Lizhu,Hu Huilin,Liu Lequan,Ye Jinhua,Wang Defa
As one of the most promising routes for production of low-carbon olefins (e.g., ethene and propene etc.), methanol-to-olefins (MTO) reaction is influenced largely by the temperature. Noble metal (e.g., Au, Ag, etc.) nanoparticles are known to exhibit the localized surface plasmon resonance (LSPR) effect, which has been applied in photothermal reactions. Owing to the increased light absorption ability in near-infrared region, titanium nitride (TiN) nanoparticles exhibit a superior LSPR effect over noble metals. Herein, we report on the MTO reaction via photothermal effect over a series of TiN(x)/SAPO-34 (x = 0.5, 0.75, 1, 2, 5, 10, 13 wt%) catalysts prepared by a simple mechanical grinding method. The MTO reaction over TiN(x)/SAPO-34 was carried out under a 300 W xenon lamp irradiation. The MTO reactivity of TiN(x)/SAPO-34 was influenced by both the photothermal temperature from the LSPR effect of TiN nanoparticles and the Brønsted acid sites on SAPO-34, both of which were dependent on the loading amount of TiN nanopartiles. The synergistic effect of high photothermal temperature, sufficient Brønsted acid sites and moderate BET surface area gave rise to the optimal catalytic performance of MTO reaction over TiN(10)/SAPO-34, which exhibited a methanol conversion of 73.1% and an ethene selectivity of 62.5%. Graphic Abstract
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Tingting Lu,Yufei Sun,Zhiwei Wang,Shuo Zhang,Yongsheng Yang,Hongdan Zhang,Peng Cheng,Zhen Zhao
A facile and effective post-treatment route has been systematically applied for the preparation of hierarchical zeolites SAPO-18 using oxalic acid or sodium citrate etching solution. The influence of acidic or alkaline post-treatment on the relative crystallinity, morphology, chemical composition, pore characteristics, and acidity of a series of zeolites SAPO-18 was investigated by X-ray diffraction, scanning and transmission electron microscopy, X-ray fluorescence spectroscopy, nitrogen adsorption–desorption, temperature-programmed desorption of ammonia, and solid-state magic angle spinning nuclear magnetic resonance spectroscopy experiments. Post-treatment led to an increase in mesoporosity by widening the micropores, but a decrease in the acid strength of zeolite SAPO-18 samples. The effects of mesoporosity and acidity on the catalytic cracking performance of zeolite SAPO-18 samples were studied. The hierarchical zeolite SAPO-18 sample post-treated by alkaline sodium citrate solution with suitable concentration exhibited better catalytic conversion and improved light olefin selectivity in cracking of 1-butene.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Xiaona Liu,Yi Cao,Nana Yan,Chao Ma,Lei Cao,Peng Guo,Peng Tian,Zhongmin Liu
The high-temperature (HT) and low-temperature (LT) hydrothermal stabilities of molecular-sieve-based catalysts are important for the selective catalytic reduction of NO x with ammonia (NH 3 -SCR). In this paper, we report a catalyst, Cu 2+ loading SAPO-17, synthesized using cyclohexylamine (CHA), which is commercially available and inexpensive and is utilized in NH 3 -SCR reduction for the first time. After systematic investigations on the optimization of Si and Cu 2+ contents, it was concluded that Cu-SAPO-17-8.0%-0.22 displays favorable catalytic performance, even after being heated at 353 K for 24 h and at 973 K for 16 h. Moreover, the locations of CHAs, host–guest interaction and the Brönsted acid sites were explored by Rietveld refinement against powder X-ray diffraction data of as-made SAPO-17-8.0%. The refinement results showed that two CHAs exist within one eri cage and that the protonated CHA forms a hydrogen bond with O4, which indicates that the proton bonding with O4 will form the Brönsted acid site after the calcination .
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Meiqiu Hu,Hong Yuan,Wei Liu
Ordered mesoporous SAPO-11 molecular sieves (OMSMS) with a single mesoporous structure were prepared via a one-step hydrothermal method. Metal–acid bifunctional Pt/SAPO-11 (Pt/OMSMS-700) catalysts with Pt loadings of 1% and 2% were synthesized by a deposition–precipitation method using OMSMS-700 as a carrier. The OMSMS and Pt/OMSMS-700 were characterized using transmission electron microscopy (TEM), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (N2-BET) analysis, and X-ray powder diffraction (XRD). TEM and small-angle XRD results revealed that the degree of order in the OMSMS increased as the calcination temperature increased from 500 to 700 °C. The N2-BET analysis revealed that the OMSMS had a mesoporous structure with an average pore diameter of 6.4–7.8 nm and a BET surface area of 149–171 m2/g. The sizes of the Pt nanoparticles supported on OMSMS-700 were in the range of 3 to 6 nm and displayed good dispersibility. The catalytic performance of Pt/OMSMS-700 during the decarboxylation of oleic acid to form C8–C17 alkanes under a CO2 atmosphere was investigated. As the reaction temperature increased from 320 to 360 °C, the total yield of C8–C17 alkanes initially increased and then decreased. Increasing the Pt loading led to an increased yield of C8–C17 alkanes. The total yield of C8–C17 alkanes reached 78% when 2 wt % Pt/OMSMS-700 was used at 340 °C for 3 h.
研究领域:
催化化学
·
能源化学
·
多相催化
·
生物燃料
·
材料化学
✓ 已验证
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2019
·Vol. 128
·期 1
·523-538
·
IF 1.428
Liu Zhonghai,Sun Zhenzhu,Qin Dongling,Yang Gang
Sulfonic acid-functionalized hierarchical SAPO-34 (S 1 -SAPO-34-SO 3 H) was prepared by post-grafting 3-mercaptopropyltriethoxysilane, and the sulfonic acid group was then oxidized by H 2 O 2 . The obtained catalysts were characterized by XRD, SEM, FTIR, TG, nitrogen adsorption, XRF, and acid–base titration. The acidity of the modified SAPO-34 increased, which confirmed the success of grafting. The catalytic properties during the dehydration of fructose to 5-hydroxymethylfurfural (5-HMF) were investigated. The yield of 5-HMF was up to 72%, and a 34% increase was found compared with the case of SAPO-34. The findings were discussed and attributed to the synergistic effects caused by both the acid groups and the mesopores. More basic investigations with regard to the conditions, including the reaction time, temperature, solvent, load and regeneration, are needed.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Saisai Liu,Jing Liu,Guanyi Chen,Jingang Yao,Beibei Yan,Weiming Yi,Zhanjun Cheng,Chunyan Tian,Huijie Zao
Syngas is a key precursor for synthesizing gasoline (C 5 -C 11 ) hydrocarbons, offering an efficient route for utilizing non-petroleum carbon sources. However, the conventional Fischer-Tropsch synthesis (FTS) process faces a constraint with a maximum 45% selectivity for C 5 -C 11 , attributed to the Anderson-Schultz-Flory (ASF) distribution. Herein, bifunctional catalysts comprising ZnZrO x with different Zr/Zn ratios along with SAPO-11 zeolite sieves featuring varied morphologies like nanosheets (SA-A), petals (SA-B), and spheres (SA-C) have been effectively formulated and employed for the syngas-to-gasoline hydrocarbons (STG) reaction. Notably, the selectivity toward C 5 -C 11 far exceeded the ASF limits. Under identical reaction parameters, the Zn 1 Zr 4 O x /SA-A catalyst demonstrated notable enhancements of 6.6% and 26.2% in CO conversion, along with 4.6% and 7.6% increases in C 5 -C 11 selectivity, as compared to that of Zn 1 Zr 4 O x /SA-B and Zn 1 Zr 4 O x /SA-C catalysts, respectively. Furthermore, under the ideal conditions (380 °C, 4.5 MPa and gas hourly space velocity (GHSV) of 2400 mL min −1 g −1 ), Zn 1 Zr 4 O x /SA-A exhibited an exceptional C 5 -C 11 selectivity of 69.8% (CO 2 -free) alongside a single-pass CO conversion of 30.4%. Impressively, isoparaffin constituted 39.2% of the total composition , with the iso/n-paraffin ratio reaching 11.8. Even after 100 h, the catalyst maintained its remarkable catalytic activity , with the CO conversion and C 5 -C 11 selectivity maintaining levels of 27.5% and 66.85%, respectively.
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
FUEL PROCESSING TECHNOLOGY
·
2019
·
IF 4.507
Lingmei Yang,Shiyou Xing,Hongzhe Sun,Changlin Miao,Ming Li,Pengmei Lv,Zhongming Wang,Zhenhong Yuan
In this study, a series of Ni/SAPO-11 catalysts with different Ni loadings were prepared by citric acid-assisted impregnation for the hydroisomerization of oleic acid to iso-alkanes. Serving as a chelating ligand, citric acid first promoted the dispersion of Ni nanoparticles loaded on SAPO-11. Because of its acid properties, citric acid facilitated the removal of aluminium oxide species, contributing to the formation of a mesoporous SAPO-11 structure. A maximum of 67.3 mol% of iso-alkanes was formed using 7Ni/SAPO-11 as a catalyst under optimal conditions of 360 °C, 4 h, and 4.0 MPa H 2 . After reusing for five cycles, the catalyst still exhibited 21.5 mol% isomer selectivity. The reaction pathways and catalytic mechanisms concerning the oleic acid hydroisomerization process were proposed and discussed. The hydroisomerization of oleic acid mainly depended on the catalyst's Lewis acid sites, with the assistance of the metal centre and Brönsted acid sites. The mesoporous structure of SAPO-11 facilitated the availability of a significant number of catalytic Lewis acid sites, which, together with the highly dispersed Ni centres, contributed to the enhanced product isomerization.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Xin Su,Guosheng Li,Chao Fan,Tingting Zhou,Jing Liu,Beibei Yan,Yang Zhang,Guanyi Chen,Jingang Yao
Herein, the SAPO-31 produced phenol-rich bio-oil from Arundo donax (AD) via catalytic fast pyrolysis (CFP) in a fixed bed. Effective variables including type of catalyst, temperature, weight hourly space velocity (WHSV) and N 2 flow rate (Nfr) were evaluated to enhance the CFP. The results showed that SAPO-31 demonstrated selectivity of 80.28 % towards naphtha-range compounds and 33.57 % towards phenolic compounds (PCs) within the naphtha range at 500 °C, Nfr of 300 mL min −1 and WHSV of 1 h −1 , contrasting sharply with those of control groups (50.82 % and 14.40 %, respectively), HZSM-5 (67.66 % and 5.51 %, respectively) and Hβ (61.10 % and 25.50 %, respectively). Moreover, SAPO-31 gave the highest bio-oil yielded (26.97 wt%) compared to that of the control group (22.45 wt%), Hβ (22.21 wt%) and HZSM-5 (21.42 wt%). These results indicate that the SAPO-31 self-synthesized exhibits promising capabilities in producing phenol-rich naphtha-range compounds via the CFP of AD.
研究领域:
能源植物学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 15
·4519-4525
·
IF 7
Chaoran Wang,Xiao Li,Shiyue Liu,Tingting Wang,Puxu Liu,Xiaowei Song,Zhiqiang Liang
Silicoaluminophosphate (SAPO) zeolites with small pores (8-ring window), such as SAPO-34, SAPO-17, and SAPO-RHO, have attracted a lot of attention due to their unique structural features, and their applications in the field of small-molecule gas adsorption and separation. However, the fast, efficient and green synthesis of SAPO zeolites remains a great challenge. In this work, SAPO-17 zeolites were synthesized within 1 min for the first time by a seed-assisted microwave method, and the resulting samples possessed excellent performance in the application of CO2 adsorption and separation for flue gas and natural gas. The microwave-assisted route can shorten the crystallization time of traditional hydrothermal methods from a few hours to 30 min. Furthermore, the crystallization time could be drastically shortened to 1 min with the addition of seeds, which represents the shortest time for the preparation of a SAPO-17 zeolite up to now. SAPO-17 synthesized within 1 min (SAPO-17-S-1) possessed the smallest crystal size, and the largest micropore volume and specific surface area among all the samples, which enhanced mass transfer and exposed more active sites, and thus it possessed prominent performance for CO2 adsorption (3.47 mmol g−1 at 273 K and 1 bar) and gas separation. At 298 K and 100 kPa, SAPO-17-S-1 exhibited the highest gas selectivity for CO2/N2 (276) and CO2/CH4 (63) over the other samples, which were synthesized in a relatively long time. Transient binary breakthrough experiments on SAPO-17-S-1 further verified the highly-efficient gas separation performance. This work proposes a green and ultrafast strategy for the synthesis of SAPO-17 zeolites with highly selective CO2 adsorption over N2 and CH4.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2020
·Vol. 2020
·期 22
·2170-2176
·
IF 2.529
Xueshuai Chen,Rongli Jiang,Zihan Zhou,Xingwen Wang
Graphical SAPO-34 zeolite was successfully synthesized from laponite as the single Si source. Laponite itself contains Li and Mg atoms, which were subsequently introduced into the structure of SAPO-34 via depolymerization-reorganization of laponite. Metal incorporation can reduce the amount of stronger acid sites and enhance the catalytic performance in the MTO reaction. In this work, SAPO-34 zeolite with high catalytic activity was successfully synthesized by hydrothermal method from laponite as the single Si source. Compared with the traditional method of synthesizing zeolites from clay, the laponite after swelling can be directly used in the synthesis process of zeolite. The crystallization behavior of SAPO-34 synthesized from laponite was investigated by XRD, FTIR, N 2 adsorption–desorption, SEM-EDX, ICP-MS, and DR-UV/Vis. The process can be summarized as follows: the Si and Mg elements were produced by the depolymerization of laponite, then the primary building units of SAPO-34 zeolite were formed under hydrothermal conditions; finally, the crystal nucleus began to form, and crystallization was triggered. Compared with the conventional SAPO-34 synthesized from TEOS, the SAPO-34 synthesized from laponite exhibited higher selectivity to light olefins and longer lifetime, which can be attributed to the suitable strength of acidity. This work points to a straightforward route to the synthesis of SAPO-34 from laponite.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nanomaterials
·
2025
·Vol. 15
·期 5
·321
·
IF 4.3
Boyang Xu,Jie Chen,Kai Wang,Pengfei Li,Le Kang,Huiling Du,Qianqian Liu,Xiaoqing Lian
The accumulation of organic pollutants and solid waste is one of the major environmental challenges faced globally. Establishing an efficient recycling system for solid waste and designing cost-effective, high-performance photocatalysts are urgent tasks for the removal of organic pollutants from water. This study utilizes coal gangue as the precursor to synthesize a coal gangue-based phosphorus–silicon–aluminum molecular sieve (SAPO-5) via hydrothermal synthesis. The resulting material was then composited with bismuth oxybromide (BiOBr) to form a novel BiOBr/coal gangue-based SAPO-5 nanocomposite. When the mass ratio of BiOBr to coal gangue-based SAPO-5 molecular sieve is 0.3, the synthesized nanocomposite exhibits excellent adsorption and photocatalytic performance for the removal of methylene blue, achieving a removal rate of 97.8% and the mineralization rate of 57.4% within 30 min. The superior performance can be attributed to the optimal pore size, rapid charge transfer rate, and high photogenerated charge density of the BiOBr/coal gangue-based SAPO-5 nanocomposite. The novel BiOBr/coal gangue-based SAPO-5 molecular sieve nanocomposite catalyst presents a new approach for the harmless treatment of organic dye wastewater and the high-value utilization of coal gangue.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemCatChem
·
2018
·Vol. 10
·期 11
·2481-2487
·
IF 4.674
Yani Zhang,Yue Peng,Chizhong Wang,Kezhi Li,Shuai Liu,Xiansheng Li,Jianjun Chen,Junhua Li
Graphical Change for copper : Copper ion exchanged SAPO-47 zeolite catalysts are synthesized and used for the selective catalytic reduction (SCR) of NO x with ammonia, for which they exert high activity. The structure–activity relationship is explored. Copper-exchanged H-SAPO-47 zeolites were synthesized by an aqueous solution ion exchange method and applied in the selective catalytic reduction of NO with NH 3 (SCR). The microporous chabazite (CHA) structure of the catalysts was characterized and confirmed using synchrotron X-ray diffraction and nitrogen adsorption–desorption experiments. The synthesized Cu x -SAPO-47 catalysts exhibited excellent SCR activity and nearly 100 % N 2 selectivity in a wide temperature range. The Cu 0.1 -SAPO-47 sample exhibited higher activity than the other samples below 250 °C. The weak Lewis acid sites originating from the introduction of Cu 2+ were more active than the Brønsted acid sites of the zeolites framework at low temperature. Two types of isolated Cu 2+ species with different coordination surroundings were found, namely, Cu 2+ cations bonded with the six-membered rings and those bonded in the CHA cages. The former species exhibited good stability and activity at high temperature, whereas the latter ones were more active at low temperature. The Cu 0.1 -SAPO-47 catalyst provided a considerable amount of isolated Cu 2+ bonded in the CHA cages. These results indicated that active Lewis acid sites and isolated Cu 2+ species are responsible for their excellent SCR activity.
研究领域:
化学工程
·
催化材料科学
✓ 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）