APPLIED ORGANOMETALLIC CHEMISTRY
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2022
·Vol. 37
·期 1
·e6935
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IF 4.072
Yanyun Wang,Jiehua Bao,Changjiang Zuo,Guomeng Dong,Xiaoli Sheng,Yuzhong Huang,Yiwei Zhang,Yuming Zhou
Exploration of levulinic acid (LA) hydrogenation to γ-valerolactone (GVL) contributes to the conversion from carbohydrates to valuable fuels and chemicals. Here, we obtained a series of ultra-small PtNix bimetallic composite catalysts encapsulated in silicalite-1 zeolite (S-1) via a one-pot synthesis strategy protected by tetra(p-carboxyphenyl)porphyrin (TCPP) ligands. The catalytic results showed that PtNi 3 @S-1 (TCPP) exhibited the most active catalytic performance (95.7% LA conversion and 93.8% GVL selectivity) under optimized conditions. The characterization results indicate that ligand modification and bimetallic synergy play an important role in enhancing the catalytic activity. The introduction of TCPP provides a guarantee for the homogeneous encapsulation of PtNi 3 in S-1 zeolite at sub-nanometer size. The electronic interaction of PtNi bimetallic, high dispersibility of active components, improved surface acidity and excellent stability co-contribute to the satisfactory hydrogenation activity.
研究领域:
催化
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化学工程
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材料科学
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绿色化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 35
·11865-11875
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IF 6.4
Xiandi Yu,Yuchi Zhang,Le Han,Yan Xu
All-inorganic CsPbBr3 perovskite quantum dots (PQDs) show superior photophysical properties and great potential in various optoelectronic devices, but their low lattice formation energy and high delocalization of surface ions make them susceptible to ambient conditions. In this work, the hierarchical silicalite-1 zeolite co-templated by carbon nanotubes (CNTs) and tetrapropylammonium hydroxide (TPAOH) was applied to encapsulate CsPbBr3 PQDs. Particularly, distinct nanosized CNTs, mass ratios of zeolite to CsPbBr3, and thermal diffusion temperature were systematically studied to optimize the loading capacity and luminescence efficiency of CsPbBr3 PQDs. Consequently, the micro-/mesoporous silicalite-1 confined CsPbBr3 PQD nanocomposite obtained at 700 °C exhibited the best luminescence performance with a full-width at half-maximum (FWHM) of 25 nm, a high PLQY of ∼61.9% and an ultrahigh stability of >100 days in H2O. The CsPbBr3/silicalite-1 nanocomposite shows dual-mode temperature monitoring performance in terms of fluorescence emission intensity and spectral shift, rendering it a promising candidate for credible optical thermometry. Latent fingerprint identification and selective Fe3+ fluorescence sensing applicability of the CsPbBr3/silicalite-1 nanocomposite were then developed. Also, a reversible off/on switching of the green fingerprint image under UV-light irradiation can be easily modulated by spraying Fe3+ aqueous solution and pure H2O, respectively, achieving an effective anti-counterfeiting application.
研究领域:
材料科学
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光电技术
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纳米技术
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分析化学
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2020
·
IF 5.278
Lei Cai,Chao Chen,Wenjun Wang,Xiu Gao,Xiaoyan Kuang,Yan Jiang,Liang Li,Guoqiang Wu
Titanium silicalite-1 (TS-1) zeolite was successfully synthesized by hydrothermal method in the presence of the tetrapropylammonium hydroxide (TPAOH) template, and a series of TS-1 supported cadmium with different Cd loading ( x Cd/TS-1) catalysts were carefully prepared to produce epoxidized soybean oil (ESO) through the acid-free catalytic epoxidation of soybean oil (SO) with H 2 O 2 . These catalysts were fully characterized using various modern techniques and further evaluated systematically in this epoxidation reaction to understand the relationship between catalytic activity and structure of active components. The results show that the highly dispersed Cd species are introduced on the TS-1 support without affecting the coordination environment of tetrahedral Ti (framework Ti). Furthermore, the Cd species are coordinated with tetrahedral Ti species via O atom resulting in the weakness of the Ti–O bonds and facile attack of the Ti–O bonds by alcohol and H 2 O 2 , which can easily form the five-membered intermediate and promote the SO epoxidation process. Furthermore, the deactivation and regeneration behaviors of 2%Cd/TS-1 catalyst in SO epoxidation were also investigated, which reveal that the catalyst deactivation of coke deposition is due to the strong adsorption of the catalysts and SO molecules. But the spent 2%Cd/TS-1 can be completely regenerated by calcination method.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2021
·Vol. 2021
·期 23
·2201-2210
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IF 2.524
Shiwei Wang,Bo Yan,Juan Chai,Tianhao Li,Hongbo Yu,Tong Li,Peng Cao,Fan Yang,Xuemin Yuan,Hongfeng Yin
Graphical A prominently size-dependent intrinsic catalytic activity or structure-sensitive catalysis in N 2 O decomposition appeared over Rh encapsulated within silicalite-1 (Rh@S-1). The size of metal species plays a pivotal role in governing catalytic performance of supported metal catalysts. In this work, a series of Rh encapsulated within silicalite-1 catalysts with different sizes were prepared by one-pot hydrothermal method and employed to catalyze the decomposition of N 2 O. Detailed structure determinations by HAADF-STEM, XPS and CO-DRIFTS demonstrate that subtle modulation of the encapsulated Rh species were achieved easily from single-atom to nanoclusters and nanoparticles by controlling the loading and reduction conditions of Rh. The turnover frequency (TOF) of N 2 O decomposition showed a typical volcano-type dependence on Rh size. Kinetic studies revealed that this structure-sensitive catalysis was related to the difference in N 2 O and O 2 adsorption/desorption for various Rh species. Furthermore, a Rh@S-1 catalyst with a proper Rh size (ca. 1.6 nm) was identified as the best-performing catalyst with a maximum TOF (ca. 95 h −1 ), showing much superior activity than other reported Rh-based catalysts.
研究领域:
化学
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材料科学
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催化反应
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Hongyu Qu,Xiangcheng Li,Xiao Han,Xinqiang Feng,Junjie Li,Zhendong Wang,Weimin Yang
The upgrading and utilization of 5-hydroxymethylfurfural (HMF) as a platform chemical for the manufacture of biofuels and biopolymers have drawn a lot of attention, especially for the selective hydrogenation of HMF to the biobased polymeric monomer tetrahydrofuran-2,5-dimethanol (THFDM). However, the catalytic hydrogenation of HMF with sustainability remains challenging. Herein, we report the synthesis of the Ni@U-Silicalite-1 catalyst, which shows a satisfying selectivity to THFDM (95.6%) under mild reaction conditions (1.5 MPa H2 and 130 °C). Characterization results show that the U-Silicalite-1 zeolite has a short b-axis, a flat reaction surface, and enlarged mesopores, which facilitate the accessibility to active sites of HMF. Meanwhile, the high distribution and small size of Ni nanoparticles contribute to the excellent catalytic efficiency and recyclability. Moreover, the strong interaction between Ni species and U-Silicalite-1 zeolite prevents the aggregation and leaching of Ni nanoparticles and endows the Ni@U-Silicalite-1 catalyst with good stability.
研究领域:
催化化学
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生物质转化
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绿色化学
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产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 12
·1625
·
IF 4.501
Bo Chen,Zhi-Ze Cao,Zhi-Jun Diao,Liang-Qiu Huang,Si-Jia Zhao,Hong Yuan,Jia-Meng He
Hydrogenolysis via targeted depolymerization of C–O linkages is a techno-economic beneficial process for converting lignin into highly valuable chemicals and clean fuels. In this work, a macroporous silicalite-1 (S-1) array-supported Ru-Ni metallic phosphide composite (Ru-Ni12P5/S-15) was prepared as a catalyst and hydrogenolysis activity under relative mild conditions was investigated using a series of compounds containing ether linkages as lignin-related model compounds. The Lewis acid sites originating from the unreduced Ru species and the macroporous geometry of S-1 significantly influenced hydrogenolysis activity and product selectivity. Analysis of the mechanism demonstrated that both the aryl ether and aliphatic ether linkages were directly hydrogenated over Ru-Ni12P5/S-15. 2D-HSQC-NMR spectroscopy demonstrated that the ether linkages of lignin were efficiently cleaved by Ru-Ni12P5/S-15. Furthermore, the obtained liquid hydrogenolysis products are high value-added chemicals used for pharmaceutical production and can be facilely tuned via the reaction conditions.
研究领域:
催化化学
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可再生资源转化
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Shichao Han,Pan Liu,Ye Ma,Qinming Wu,Xiangju Meng,Feng-Shou Xiao
Calcination-free fabrication of highly b-oriented silicalite-1 (S-1) zeolite films in the absence of organic structure-directing agents (OSDAs) is attractive but still challenging. Herein, for the first time, we show a novel route for calcination-free synthesis of a b-oriented S-1 zeolite film in the absence of OSDAs. The key to this success is a rational secondary growth of zeolite crystals on the surface of supports by avoidance of the formation of zeolite nuclei in the system due to the absence of OSDAs. Because of OSDA-free synthesis of S-1, it not only reduces the cost of zeolite films but also avoids the calcination of OSDAs in the synthesis, thus avoiding the formation of cracks in the zeolite films. In addition, the calcination-free fabrication is favorable for reduction of zeolite film defects such as a terminal OH group. As a result, the zeolite films obtained from this work exhibit higher hydrophobicity than the conventional one. Furthermore, the current polarization curve of this S-1 zeolite film shows excellent corrosion resistance. The aforementioned features would be potentially important for industrial application of zeolite films in the near future.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
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