MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Tao Wang,Chao Xiao,Qiao Yu,Zhilin Chen,Shuming Peng
Development of a stable catalyst resistant to steam-induced sintering (10 vol%−15 vol% H 2 O, 450–550 °C) is challenging for catalytic combustion/oxidation of methane. We use the silicalite-1's internal defects to trap PdO clusters to construct a stable catalyst (PdO/silicalite-1). Silicalite-1 with sufficient amounts of silanol defects and ion exchange at alkaline condition are critical for this defect-trapping strategy. PdO/silicalite-1 shows long-term super-stability with respect to the temperatures and steam concentrations. The conversion remained stable over 200 h at 500 °C (10 vol% H 2 O) and declined slightly during 380 h at 550 °C (10 vol% H 2 O). PdO/silicalite-1's catalytic activity deteriorated slightly after hydrothermal aging at 750 °C or thermal aging at 850 °C. Electron microscopy reveals two growth modes for PdO clusters within silicalite-1 (PdO in ) and on the external surface (PdO surf ). PdO surf clusters agglomerate into PdO particles of 5–15 nm directly, but PdO in clusters first fuse into strip-shaped PdO in clusters, then migrate outwards and further agglomerate into PdO nanoparticles .
研究领域:
催化化学
·
材料科学
·
环境化学
·
纳米材料
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Yanxin Zhang,Xuesi Hong,Yuzhu Shi,Duo Xu,Yueqin Song,Xiaolong Zhou,Jin An Wang
The present study investigated a novel bimetallic Pt-Mo catalyst encapsulated within Silicalite-1 zeolite for propane dehydrogenation (PDH). The catalyst was synthesized via in situ hydrothermal crystallization, followed by direct high-temperature H 2 reduction without conventional calcination, leading to uniform encapsulation of Pt nanoparticles within the zeolite framework and simultaneous removal of the template and organic ligands. PDH performance was evaluated in a continuous-flow fixed-bed microreactor. Comprehensive characterizations (XPS, CO-DRIFTS, NH 3 -TPD, Raman, etc.) reveal that Mo incorporation in 0.4Pt@S-1 catalyst significantly enhances propane conversion while maintaining high propylene selectivity. Moreover, the bimetallic 0.4PtXMo@S-1 catalyst with 0.1 % Mo doping achieved an outstanding performance at 550 °C and a WHSV of 5.49 h −1 (propane conversion: 43 %, propylene selectivity: 97 %, propylene formation rate: 16.27 mol C3H6 ·g Pt -1 ·h −1 ). The prepared catalyst possessed favorable stability and regeneration performance, showing a deactivation rate of only 0.001454 h −1 after four reaction-regeneration cycles. This enhancement is attributed to synergistic effects arising from Mo incorporation, which promotes Pt nanoparticle dispersion, modulates Brønsted /Lewis acidity, and facilitates interfacial electron transfer between Pt and Mo species. These findings highlight the role of Pt-Mo interactions within zeolite frameworks, providing new insights for designing efficient and stable PDH catalysts.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2013
·
IF 2.206
Jiangfeng Yang,Junmin Li,Wei Wang,Libo Li,Jinping Li
Three hydrophobic microporous high-silica zeolites, DDR (with an 8-membered ring), silicalite-1 (a 10-membered ring), and beta (a 12-membered ring) were synthesized. The Si/Al ratios were 230, 1350, and 35, respectively. The samples were characterized by X-ray diffraction, scanning electron microscopy, thermal gravimetric analysis, water vapor adsorption, and volumetric nitrogen adsorption. They were tested for their CO2, CH4, and N2 adsorption properties at pressures of up to 10 bar at 288–313 K after activation, and the results were correlated with the Langmuir model. The heat of adsorption was calculated using the Clausius–Clapeyron equation based on the adsorption isotherms. These data were used to estimate the separation selectivities for CO2/CH4 and CH4/N2 binary mixtures at 298 K, using the ideal adsorbed solution theory (IAST) model. Experimental results showed that DDR and beta have good selectivities for CO2/CH4, because they have narrow pores (DDR) or more balance metal ions (relatively low Si/Al ratios beta) effect separately. The synthesized silicalite-1 has the lowest SCO2/CH4 but has the most suitable orifices for methane adsorption and the highest SCH4/N2. In addition, the breakthrough data for CH4/N2 mixtures further indicates that silicalite-1 is more suitable for the CH4 enrichment than the commercially used sorbents zeolite-5A and 13X. From the reproducibility of CH4 and N2 adsorption isotherms on silicalite-1, we can infer that which has the potential to be a commercial sorbent by the stable adsorption properties.
研究领域:
材料科学
·
化学工程
·
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
Baozhen Li,Jun Zuo,Tiantian Liu,Mengjia Zhu,Kun Jiang,Zhuangzhuang Ren,Hua Yang,Yu Tang,Li Tan,Lizhi Wu
The mildly selective oxidation of methane to oxygenates in the aqueous phase is of great significance for methane upgrade, while it suffers low conversion and multiple oxidation products. Fe-based zeolite, especially Fe/ZSM-5 with heteroatom Al is the most widely investigated catalyst for this reaction, while the Fe supported pure Si-based zeolite without Al is rarely reported. Herein, a series of Fe-S-1 catalysts without introducing heteroatom Al is synthesized via facial dissolution-crystallization method and applied for methane selective oxidation to formic acid. The optimized 0.5Fe-S-1 shows a superior performance with the formic acid space time yield of 49751 µmol·g cat −1 ·h −1 and a liquid-phase formic acid selectivity of 93 % at 70 °C with H 2 O 2 as the oxidant, and present an excellent stability without obvious deactivation after five cycles, which outperforms all previously reported Al-free Fe/Silicalite-1 catalysts, and is comparable with conventional Fe/ZSM-5. Combined with multifarious characterizations including TEM, UV-Vis, Raman, NH 3 -TPD, Py-IR and XAS etc., two kinds of Fe species including the mononuclear tetrahedrally coordinated framework Fe 3+ species and mononuclear octahedral coordinated extra-framework Fe 3+ species are highly dispersed over Fe-S-1 even with a high Fe loading of 1.5 wt%, in which the framework Fe 3+ species content is positively correlated with the catalyst acidity and could provide acid sites to adsorb reactants and then extra-framework Fe 3+ species could activate methane/H 2 O 2 effectively. And the further EPR, in-situ FT-IR characterizations and control experiments demonstrates that the methane selective oxidation to formic acid follows a radical mechanism, in which ·CH 3 combines with ·OH or ·OOH to form CH 3 OH, and then further oxidized to HCOOH and finally over-oxidized to CO 2 .
研究领域:
催化化学
·
环境化学
·
材料科学
·
绿色化学
·
无机化学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
·
2025
·
IF 5.6
Wenjing Li,Juan Shao,Chuxin Zhang,Guodong Cao,Yitao Yan,Qiongyi Han,Huimei Yu,Yingying Wei,Wenbo Zhang,Jie Zheng,Zhongyuan Guo
Colorectal cancer has emerged as a leading cause of global cancer-related morbidity and mortality, necessitating innovative therapeutic strategies. We developed a desilication-recrystallization method to synthesize Silicalite-1-X (X = 2, 8, 16, 32), a hierarchical porous silica molecular sieve with cost-effectiveness, facile synthesis, and tunable porosity. Its programmable mesoporous structure is achieved by precisely controlling the desilication-recrystallization kinetics. Tunable mesopores with precise diameters of 4–6 nm and 20–30 nm were fabricated by controlling cavity expansion through temporal modulation (2–32 h) of a time-dependent synthesis process. Detailed analysis of drug loading and release profiles revealed that although pore structure modification did not significantly alter drug loading efficiency (DLE), it induced a slight but consistent improvement in drug release rate as pore size increased. Systematic biocompatibility evaluation was conducted through an in vitro human colonic epithelial tissue model complemented by the KM mice in vivo studies. Histopathological analysis confirmed Silicalite-1-X caused minimal cytotoxicity and oxidative stress in healthy colon tissue, preserved mucus secretion, and showed no systemic toxicity. Furthermore, Doxorubicin (DOX) loaded Silicalite-1-X platform (Silicalite-1-DOX-X) exhibited dose-dependent cytotoxic efficacy against colorectal carcinoma in vitro models, confirming its anti-tumor therapeutic potential. Our findings provide a framework for engineering molecular sieves with tunable porosity and a platform for expanding their multifunctional applications in advanced materials.
研究领域:
材料科学
·
纳米技术
·
药学
·
生物医学工程
·
肿瘤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Ming Zhang,Guoli Fan,Liyuan Yuan,Feng Li
Bioethanol upgrading to higher alcohols (C4–10–OH) involves several sequential reaction steps occurring at multiple different active sites. Therefore, precisely engineering heterogeneous catalysts with appropriate local chemical structures of active sites and spatial environments is highly desired for efficient ethanol tandem conversion. Herein, we constructed a novel Cu-based catalyst featuring atomically dispersed Cu sites confined in a hierarchical silicalite-1@La2O3@silicalite-1 architecture, where single Cu atoms were confined in the micropores of surface silicalite-1 (S-1) zeolite nanoislands dispersed on the outer La2O3 layer encapsulating a hollow S-1 zeolite core. By modulating the content of Cu and La species, such a constructed multihierarchical Cu@S-1@La2O3@S-1 catalyst exhibited excellent performance in ethanol conversion to higher alcohols, along with an impressively high ethanol conversion of 74.9% and C4–10–OH selectivity of 85.0%, as well as an unprecedentedly high production rate of higher alcohols (10.575 mol·gCu–1·h–1) at 275 °C, far exceeding those over state-of-the-art Cu-based catalysts. It was elucidated that surface single-atom Cu sites first notably promoted the adsorption and activation of ethanol and thus initiated its dehydrogenation to produce acetaldehyde, and subsequently, acetaldehyde intermediates migrated to the outer La2O3 layer featuring abundant medium-strength basic and acidic sites, thereby facilitating the condensation of acetaldehydes and their further dehydration. This work provides an innovative approach for rationally designing high-performance supported Cu catalysts with a spatiotemporal decoupling structure applied in advanced heterogeneous tandem catalytic processes through the design of site-specific confinement within hierarchical structures.
✓ 已验证
DOI
PubMed
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Zhang Changsheng,Chu Shaoqi,Jiang Jie,Zhao Jinchong,Wen Song,Sun Bing,Xu Wei
Synthesis of zeolites in more efficient and greener methods is of great significance in both industrial and academic fields. However, the relative long time for zeolite crystallization and much consumption of water solvent make the target challengeable. Herein, a route for ultrafast synthesis of nano Silicalite-1 zeolites in 10 min with much less water consumption has been developed. Comprehensive characterizations, i.e., X-ray powder diffraction, N2 sorption, scanning electron microscope, and NMR, confirm the high quality of such obtained Silicalite-1 zeolites. In the catalytic deoxygenation of O2-containing ethylene (mixture of O2 and ethylene), these reported Silicalite-1 zeolite samples show the comparable performance with the conventional Silicalite-1 zeolites synthesized under hydrothermal conditions. This research therefore provides a new trial toward the ultrafast synthesis of zeolite materials in an environment-friendly route.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 12
·e18249
·
IF 3.7
Ying Zhang,Xiaofang Wang,Huihui Deng,Qin Sun,Baozhen Li,Wenchun Zheng,Zhuangzhuang Ren,Xiangqing Fang,Li Tan,Yu Tang,Lizhi Wu
Pt-based catalysts have been widely investigated in propane dehydrogenation (PDH) owing to their high activity in C H activation, while it suffers from Pt sintering and coke deposition. We develop a transition metal Fe and zeolite support synergistic-modified method to realize the highly dispersed and stable Pt species inside zeolite over Pt/Fe-silicate-1. And it shows the excellent PDH performance with propylene generation rate of 51.6 mol C 3 H 6 g Pt −1 h −1 and low deactivation rate constant k d of 0.017 h −1 as well as a high TOF Pt of 37.6 s −1 at 550°C. The systematic characterizations reveal the isolated Fe 3+ species could significantly improve Pt dispersity and regulate Pt electronic density to realize a more positive Pt δ+ species inside Silicalite-1 pore. And the further in situ DRIFTS experiments demonstrate that the synergistic effect between the appropriate acidic Fe sites and the highly dispersed Pt δ+ species around Fe species are responsible for the superior PDH performance.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huihui Deng,Baozhen Li,Wenchun Zheng,Qin Sun,Mengjia Zhu,Jun Zuo,Yu Tang,Lizhi Wu,Li Tan
Propane dehydrogenation is one of the most promising routes for propylene production due to its single reactant, product and high economic efficiency. For Co-based catalysts, the state of Co species is one of the important factors affecting the performance of propane dehydrogenation. Here, we designed zeolite Silicalite-1 (S-1) with different silanol nests content as support to investigate the effect of silanol nests content to form Td-Co(II) species. It is found that the content of silanol nests in the S-1 supports have a linear correlation with the formation of T d -Co(II) species and corresponding PDH catalytic activity through the study of the catalyst structure-performance relationship. And the silanol nests of S-1 could be fully coordinated with 0.5 wt% Co content over 0.5Co/S-1-1-HTS in the form of T d -Co(II) species to maximize the Co atomic utilization. Correspondingly, 0.5Co/S-1-1-HTS shows the most excellent catalytic activity and stability, with C 3 H 6 generation rate of 3014 mmol C 3 H 6 g Co −1 h −1 and deactivation rate of 0.07 h −1 at 550 °C.
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
AICHE JOURNAL
·
2021
·Vol. 67
·期 7
·e17295
·
IF 3.993
Bofeng Zhang,Guozhu Li,Ziwei Zhai,Dali Chen,Yajie Tian,Ruoou Yang,Li Wang,Xiangwen Zhang,Guozhu Liu
Propane dehydrogenation (PDH) is one of the most effective methods to produce propylene. But the industrial Pt-based catalysts often suffer from short-term stability under the high temperature reaction environment (500–700°C) via sintering and coke deposition. Herein, stable PDH reaction in high propylene yield has been achieved by the confinement of Pt–Zn intermetallic alloys (IMAs) in the channels of silicalite-1. Single-site Zn in the MFI framework was found to play a key role on assisting and stabilizing the PtZn IMAs for efficient PDH. By the cooperative action of the spatial confined PtZn IMAs and the lattice confined framework Zn, high propylene selectivity (>99%) without obvious deactivation was realized on the as-developed catalyst (PtZn@S-1) under 600°C even after 90 h. The low deactivation constant (0.003 h −1 ) was 6 times lower than that of the industrial PtSn catalyst.
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
AICHE JOURNAL
·
2018
·Vol. 65
·期 1
·196-206
·
IF 3.326
Fusheng Pan,Weidong Li,Ye Zhang,Jie Sun,Meidi Wang,Hong Wu,Zhongyi Jiang,Ligang Lin,Baoyi Wang,Xingzhong Cao,Peng Zhang
Hollow monocrystalline silicalite-1 (HMS) nanoparticles were successfully synthesized and firstly incorporated into poly(ether- block -amide) (Pebax) to prepare hybrid membranes. The uniformly dispersed HMS in Pebax matrix interrupt the crystalline region and optimize the free volume property. The micropores on the HMS shell enhance the selectivity because of sieving effect, whereas the inner cavity benefits the rapid diffusion of penetrant and elevates the flux. When the content of HMS (200 nm) is 20 wt %, the hybrid membrane possesses a permeation flux of 20.63 kg/(m 2 h) and an enrichment factor of 6.11 (82% and 23% higher than that of Pebax membrane, respectively), which surpass the upper bound of the state-of-the-art reported polymeric membranes. Moreover, the hybrid membranes display the remarkable antiswelling and long-term operation stability. This is a step forward in fabricating the hybrid membranes with superior separation performance by incorporating porous fillers with hollow structure. © 2018 American Institute of Chemical Engineers AIChE J , 65: 196–206, 2019
研究领域:
化学工程
·
材料科学
·
膜技术
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2023
·Vol. 16
·期 8
·10881-10889
·
IF 9.9
Wei Xueer,Cheng Jiawei,Li Yubing,Cheng Kang,Sun Fanfei,Zhang Qinghong,Wang Ye
The noble metal-based bimetallic clusters with high atom utilization and surface energy have been widely applied in heterogeneous catalysis, but the stabilization of these metastable clusters in harsh reaction conditions is quite challenging. Herein, we synthesize a series of Pt-, Pd-, and Ru-based clusters promoted by a second non-noble metal (Zn, Cu, Sn, and Fe), which are confined inside silicalite-1 (pure silica, S-1) crystals by a ligand-protected method. The second metal could well stabilize and disperse the noble atoms inside the rigid S-1 zeolites via Si-O-M bonds, thus enabling to lower the usage of expensive noble metals in catalysts. The as-synthesized bimetallic catalysts exhibited excellent performance in non-oxidative propane dehydrogenation (PDH) reaction, which is typically operated above 500 °C. The PtZn@S-1, PtCu@S-1, and PtSn@S-1 with only a ∼ 0.17 wt.% Pt loading offer a significant enhancement in PDH performance compared with the conventional PtSn/Al 2 O 3 catalyst with a 0.5 wt.% Pt loading prepared by impregnation method. Notably, the PtSn@S-1 provides a propane conversion of 45% with a 99% propylene selectivity at 550 °C, close to the thermodynamic equilibrium. Furthermore, the PtSn@S-1 exhibits excellent stability during 300 h on stream and high tolerance to regeneration by a simple calcination step.
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
危险品化学品经营许可证（带存储）