JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Zhe Hu,Hanqing Dai,Wenjie Zhou,Jinxin Wei,Hongbin Zhang,Zhaoqi Ye,Yi Qiu,Yuanyuan Chen,Zhongtao Duan,Jing Wang,Wanlu Zhang,Fengxian Xie,Ruiqian Guo
The aggregation-induced quenching (AIQ) properties of the solid-state carbon dots (CDs) limit their wide-scale actual applications. Herein, a novel corrosion resistant solid-state CDs@Silicalite-1 (CDs@S-1) composite was synthesized via in situ embedding CDs into the S-1 matrix. Owing to the confinement effect, CDs are immobilized into the interrupted defects of the three-dimensional S-1 matrix. The as-prepared composite possesses high photoluminescence quantum yield (63%) and extra-high stability in common organic solvents and various pH solutions (pH=2–14). Moreover, the feasibility of the CDs@S-1 composite as a fluorescent label on various substrates was investigated. The results demonstrate the images with well-defined papillary ridges under ultraviolet (UV) light and show great potential for latent fingerprints detection in forensic science.
研究领域:
材料科学
·
法医学
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DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Limin Zhang,Huahua Fan,Miao Zhang,Haoqing Zhang,Hao Wang,Bangjian Liu,Jiaxing Zhang,Xiaowa Nie,Guanghui Zhang,Chunshan Song,Xinwen Guo
Cobalt-based catalysts have recently emerged as a promising frontier in propane dehydrogenation (PDH) research. Despite their potential, achieving selective suppression of nonselective metallic cobalt (Co0) species remains a critical challenge. In this work, we report a hollow zeolite architecture (Co@S-1-Hol) that effectively addresses this dilemma through spatial confinement engineering. Through depth-profiling XPS analysis complemented by H2-TPR and UV–vis spectroscopy characterization, we demonstrate a unique cobalt valence distribution where metallic Co0 species are preferentially encapsulated within hollow cavities, while Co2+ ions remain atomically dispersed in the zeolite shell matrix. DFT calculations coupled with kinetic studies reveal that the cavity-confined Co0 clusters serve as the predominant active centers for C–H bond activation. Notably, STEM-EDS mapping and TGA uncover a self-regulating mechanism: the hierarchical hollow structure facilitates rapid and selective coking on nonselective surface sites during initial reaction phases, effectively passivating undesirable side reactions while preserving intrinsic catalytic activity. This spatial engineering strategy endows the Co@S-1-Hol catalyst with superior PDH performance compared to the conventional impregnated Co/S-1 catalyst, exhibiting an enhanced C3H6 formation rate (21.6 mmol gcat–1 h–1, equivalent to 1330 mmol gCo–1 h–1) coupled with a significantly reduced deactivation rate. Under optimized conditions at 550 °C, the catalyst achieves 35% propane conversion with 95% propylene selectivity, representing state-of-the-art performance among reported cobalt-based PDH catalysts. This work not only provides fundamental insights into cobalt active site engineering but also establishes a paradigm for designing spatially modulated zeolite catalysts in alkane dehydrogenation applications.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Xu Wang,Qing You,Yushuai Wu,Chenyao Bi,Huiyong Chen,Chengyi Dai,Qingqing Hao,Jianbo Zhang,Xiaoxun Ma
A novel hierarchical tungsten-substituted Silicalite-1 zeolite with the highly interconnected hollow structure (HWS-1) was synthesized for the first time by post-treating the purely microporous tungsten-substituted Silicalite-1 (WS-1) through simultaneous desilication and tungstation, in which a combination of sodium hydroxide and tetrapropyl ammonium hydroxide (TPAOH) was used to achieve a systematic balance between dissolution and recrystallization and further promote the synchronous tungstation with using sodium tungstate dihydrate as a tungsten source. Under an optimum addition ratio of NaOH/TPAOH, the resulted HWS-1 exhibited not only well retained microporosity and crystallinity but also obviously enlarged external surface area and mesopore volume in contrast to the parent WS-1. Furthermore, the effective tungstation also facilitated the substitution and increased the amount of coordinated W species in zeolite frameworks. The catalytic performance of HWS-1 was evaluated by the epoxidation of cyclohexene with using H 2 O 2 as oxidant. Benefited by the highly interconnected hollow structure and more accessible active sites on the enlarged external surface, the HWS-1 catalyst revealed a higher catalytic activity with improved cyclohexene conversion than WS-1. Moreover, it was found that a significant positive effect on promoting epoxidation was achieved by tungsten-substituted Silicalite-1 (WS-1 and HWS-1) catalysts reflecting at a much higher selectivity of epoxide (>79%) in comparison with titanium-substituted Silicalite-1 (TS-1) (~50% selectivity of epoxide), due to their superior hydrophobicity and suitably weaker acidity, which further demonstrated the potential application of the developed hierarchical tungsten-substituted Silicalite-1 as a candidate catalyst for epoxidation and other selective oxidation reactions.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yongheng Ren,Yang Chen,Jiangfeng Yang,Jinping Li,Libo Li
The removal of trace C 2 H 4 at high relative humidity has significant importance for the preservation of fruit; however, owing to the severe storage environment and competitive adsorption of high humidity water vapor and carbon dioxide, few suitable adsorbent materials are currently available for this application. Herein, silver-loaded silicalite-1 sorbent (S-1@Ag) was synthesized via an in-situ silver modification method to enhance its interaction with ethylene. By adjusting the amount of silver source to 0.94 wt%, the ethylene uptake of S-1@Ag at P/P 0 of 0.01 was sixteen times greater than unmodified silicalite-1. S-1@Ag prepared using the in-situ method exhibits a uniform distribution of Ag + that enhances the recognition of ethylene, resulting in an excellent ability to capture ethylene at low pressures. Crucially, S-1@Ag(0.94 %) was unaffected by the presence of water vapor and carbon dioxide in its application environment, and exhibits the best preferential adsorption of ethylene under low pressures. Dynamic breakthrough tests under humid conditions demonstrated that S-1@Ag(0.94 %) captures trace ethylene four times more effectively than S-1@Ag, even under different gas mixtures (C 2 H 4 /N 2 , 0.1/99.9, v/v; C 2 H 4 /CO 2 /N 2 , 0.1/0.1/99.8 and 0.1/1/98.9, v/v/v). Furthermore, banana storage experiments show that S-1@Ag(0.94 %) slows the decay time of the fruit and improves its storage life.
研究领域:
材料科学
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食品科学
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DOI
高影响因子
CRYSTAL GROWTH & DESIGN
·
2023
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IF 3.8
Shen Yu,Ming-Hui Sun,Yuan-Yuan Wang,Zhan Liu,Jia-Min Lyu,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Li-Hua Chen,Bao-Lian Su
The epoxidation reaction over titanium silicalite-1 (TS-1) zeolites is a green way to produce epoxides that are important intermediates for chemicals. Nevertheless, the conventional microporous TS-1 zeolite shows limited diffusion ability for bulky molecules, leading to poor activity and low selectivity. Constructing hierarchical porosity in microporous materials is an effective strategy to enhance the diffusion properties of catalysts. However, there are few reports on the design and synthesis of TS-1 zeolites with hierarchical structure featuring multilevels, interconnectivity, and regularity for efficient diffusion and epoxidations. Herein, hierarchical TS-1 zeolites with ordered macro–meso–microporosity (OMMM-TS-1) are obtained by a method combining a templated effect of ordered macro–mesoporous matrices and a confined in situ crystallization process. The OMMM-TS-1 possesses ordered macropores with tunable size (∼200–600 nm), ordered mesopores (∼8 nm), and intact micropores (∼0.5 nm). The OMMM-TS-1 achieves a cyclooctene conversion as 3.6 times and 1.8 times and a selectivity to epoxy product as 1.6 times and 1.3 times higher than the conventional TS-1 (C-TS-1) and nanosized TS-1 (Nano-TS-1) zeolites, respectively. The OMMM-TS-1 also outperforms the C-TS-1 and Nano-TS-1 zeolites in epoxidations of a series of alkenes. Such a novel hierarchical structure can be applied in the design and synthesis of many other catalysts.
研究领域:
化学
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材料科学
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催化
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2026
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IF 7.6
Yu Jiaojiao,Zuo Yi,Li Gudan,Cai Jiajun,Chen Yu,Guo Yuzhou,Xu Shutao,Li Lina,Guo Lingling,Yang Hong,Guo Xinwen
Titanium silicalite-1 (TS-1) attracts wide attention as an effective oxidative catalyst. However, the preparation of TS-1 typically requires rigorous synthesis procedures with a relatively long synthesis time and generates a substantial amount of wastewater. This study discovers that, in the presence of tetrapropylammonium hydroxide (TPAOH), Si and Ti sources can form a homogenous liquid solution that is highly stable although the two typically undergo hydrolysis at very different rates individually. With such understanding, this work develops a straightforward one-pot synthesis strategy that eliminates the cumbersome procedures aimed at suppressing the hydrolysis of the Ti source in TS-1 synthesis and demonstrates that the crystallization process of TS-1 can be accelerated by reducing the molar ratio of water to Si species ( n (H 2 O/Si)) in the synthesis solution. In propene epoxidation with H 2 O 2 , an excellent catalytic activity is obtained over the TS-1 synthesized at n (H 2 O/Si) = 3.5 and crystallized for only 6 h. This low n (H 2 O/Si) synthesis regime results in a significantly high yield per batch (12 g TS-1/100 mL batch) and, at the same time, produces almost no wastewater. The superior catalytic performance of TS-3.5-6 synthesized is attributed to its high total Ti content and the presence of catalytically active Ti(OSi) 2 (OH) 4 .
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高影响因子
Clean Energy
·
2025
·Vol. 9
·期 5
·114-124
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IF 3.7
Zhang Yakun,Li Ruilong,Yong Xiaojing,Guan Chong,Zhang Yi
The effects of different promoters (including Sn, In, Ga, and K) on the activity, ethylene selectivity, and stability of the encapsulated Pt@silicalite-1 for ethane dehydrogenation were investigated. The dual-promoter catalysts, KPtIn@S-1 and KPtSn@S-1, exhibited high ethane initial conversions, high ethylene selectivity at 550°C, and high stability, with almost no deactivation during 30 hours on stream and the deactivation constants as low as 0.0003 and 0.0002 hour−1, respectively. Combining the characterization and performance evaluation results, it could be deduced that the introduction of Sn and In promoters plays an important role in diluting Pt, resulting in the reduced average Pt particle size. Moreover, the Sn introduced in KPtSn@S-1 led to the formation of a Si–O–Sn interaction structure between Sn and S-1 zeolite framework, resulting in the anchoring effects of Sn (II) on Pt sites. In the KPtIn@S-1 sample, the strong interaction between Pt and In also played a role in anchoring Pt species, which greatly reduced the formation of carbon deposition and inhibited the production of graphitic carbon deposits.
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
·
IF 9
Wei Chen,Pengfei Wang,Weike Jia,Huidan Zeng
Membrane-based pervaporation process is the most time- and energy-saving method for the separation of xylene isomers. However, developing easily prepared membrane with a high separation factor still remains a significant challenge. Herein, the silicalite-1/polyvinyl alcohol (PVA) mixed matrix membrane (MMM) (SPMMM) with enhanced xylene isomers pervaporation separation performance was successfully fabricated via solution scraping method. The compactness and compatibility of the SPMMM were effectively tuned by optimizing the zeolite content and selecting appropriate cross-linker. Results showed that the SPMMM with 40 % zeolite content, cross-linked with fumaric acid (SPMMM-Fu), exhibited the densest and most continuous membrane structure, the lowest swelling degree and the best xylene compatibility. Pervaporation experiments demonstrated that the SPMMM-Fu exhibited superior xylene isomers selective separation performance compared to the templated-silicalite-1/α-Al 2 O 3 membrane. For the SPMMM-Fu, the maximum separation factor was achieved in binary xylene isomer solutions containing 10 % p-X. The total permeate fluxes in the aforementioned binary p-X/o-X and p-X/m-X isomer solutions were about 43.20 g m −2 h −1 and 34.66 g m −2 h −1 , respectively. The corresponding separation factors of p-X/o-X and p-X/m-X were about 34.65 and 39.73, respectively. The third-stage separation experiment demonstrated that the SPMMM-Fu could produce p-X with a purity ≥99.7 % from binary p-X/o-X isomer solutions. Long-term and variable-temperature pervaporation experiments suggested the SPMMM-Fu had excellent structural stability. Furthermore, reproducibility tests conducted on multiple batches of the SPMMM indicated that the SPMMM-Fu could be produced stably. The scalable experiment demonstrated that our strategy could produce large-area SPMMM-Fu (25 × 40 cm 2 ), exhibiting separation performance similar to that of small membrane coupons. This work presented a potentially low-cost and scalable approach for producing highly dense SPMMM with exceptional xylene compatibility, enabling efficient pervaporation separation of xylene isomers from their mixtures.
研究领域:
化学工程
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材料科学
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Hui Wang,Yutao Liu,Yongheng Ren,Siyuan Peng,Jiayou Liao,Jinping Li,Libo Li
Membrane technology is a promising candidate for ethylene/ethane (C 2 H 4 /C 2 H 6 ) separation, but the separation factor and long-term stability of commercially available polymer membranes remain still insufficient to meet industrial requirements. Incorporating facilitated metal-ion carriers or unsaturated metal sites of fillers into polymers shows exceptional C 2 H 4 /C 2 H 6 separation efficiency due to the intensified olefin-favorable sorption . However, their separation performance usually dropped within a few hours due to the inactivation of the facilitated transport carrier or poisoning of unsaturated sites in presence of water vapor . Herein, we adopt a facile and effective method to prepare long-term stable Silicalite-1@Ag (S-1@Ag) mixed matrix membranes (MMM) by in-situ embedding the vulnerable carrier Ag + into the pores of the hydrophobic zeolite to protect the Ag + from deactivation. The 12 wt% S-1@Ag filler uniformly dispersing within the commercial 6FDA-DAM exhibits superior separation performance that surpasses the 2013 upper bound in terms of C 2 H 4 permeability of 29.74 barrer and C 2 H 4 /C 2 H 6 selectivity up to 7.66 for equimolar mixed gas. Furthermore, the hydrophobicity nature and framework shielding towards Ag + of S-1 guarantees the excellent almost 2-months stable separation of C 2 H 4 /C 2 H 6 by S-1@Ag MMMs under the high relative humidity conditions, demonstrating its potential for industrial applications.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
Particuology
·
2017
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IF 2.621
Rongjie Ling,Wu Chen,Jin Hou
Modified nanosized MFI (ZSM-5 and silicalite-1) zeolites were successfully synthesized by a hydrothermal method using aluminum isopropoxide and tetraethylorthosilicate as the raw materials. The synthetic zeolites were characterized by X-ray diffraction, energy dispersion spectroscopy, and scanning electron microscopy. The ZSM-5 and silicalite-1 zeolites exhibited ellipse-like and cubic columns, respectively. The K + ion-exchange equilibrium and ion-exchange capacity of the synthetic zeolites in seawater were investigated. The K + ion-exchange of synthetic zeolites was rapid and reached an ion-exchange balance in approximately 20 min. The K + ion-exchange capacity of ZSM-5 and silicalite-1 in seawater was 56.7 and 48.7 mg/g, respectively. The synthetic zeolites have high selectivity toward K + , and therefore, they can be used to selectively extract potassium from seawater.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jie Zhou,Hao Liu,Chao Xiong,Peng Hu,Hao Wang,Xuyu Wang,Hongbing Ji
Propane dehydrogenation (PDH) has been a promising method to satisfy the increasing demand for propylene, but Pt-based catalysts always suffer from sintering and coke formation. Developing stable and efficient catalysts for PDH is of great significance for the industry. Herein, the paper reports that a catalyst with potassium-promoted Pt-In bimetallic clusters encapsulated in silicalite-1 (S-1) zeolite works as an efficient and stable catalyst for PDH. The catalyst achieves a propane conversion of 43.73 % with 97.14 % selectivity of propene and an extremely high propylene productivity of 20.33 mol g Pt -1 h -1 with a weight hourly space velocity (WHSV) of 6.75 h −1 . No obvious deactivation occurs after 48 h on stream, affording an extremely low deactivation constant of 0.0025 h −1 . The introduction of indium species greatly improves the propene selectivity and restricts the coke formation. The introduction of K + into S-1 can significantly enhance the catalytic activity and the stability of the catalyst. The catalyst with excellent activity and stability is potential for industrial application.
研究领域:
催化
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化学工程
·
材料科学
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DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Meiyu Liu,Xinyu Sun,Yiming Zhang,Ye Yang,Yucai Qin,Binbin He,Yi Mei,Yun Zu
Propane dehydrogenation (PDH) is one of the most effective methods for intentional (“on-purpose”) propylene production. Isolated Sn sites on open supports exhibit considerable PDH performance comparable to that of industrial Pt- and Cr-based catalysts, but the loss of Sn is inevitable. Herein, highly dispersed and stable NiSn subnanoclusters encapsulated within the channels of silicalite-1 zeolite are fabricated through a one-step hydrothermal synthesis in this work. The as-prepared Ni 1 Sn 1 @S-1 zeolite catalyst exhibits outstanding PDH performance with considerable propylene formation rate (ca. 12.3 mmol∙g cat -1 ∙h −1 ) and high propylene selectivity (>88 %). Most significantly, no Sn loss is detected after three regeneration cycles. Structural elucidation of NiSn sites on catalysts, by HRTEM, H 2 -TPR, FTIR and XPS characterizations confirms that the Ni sites embedded in the geminal silanols of zeolitic framework play a vital role in anchoring Sn species and preventing the active sites from losing and sintering. The cooperative action of robust NiSn subnanoclusters is conducive to the selective C–H activation and the propylene desorption. A plausible dehydrogenation mechanism is revealed by in situ infrared spectroscopy. This study on siliceous zeolite confined NiSn catalysts delivers an insight into the nature of selective and stable NiSn sites involved in the PDH reaction.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）