Chemistry-An Asian Journal
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2018
·Vol. 14
·期 3
·416-421
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IF 3.692
Qian Wang,Wei Sun,Tianying Xie,Limei Cao,Ji Yang
Graphical Carbon-coated catalysts : Octahedral Pt/ZrO 2 @C, prepared by direct carbonization of the precursor UiO-66-NH 2 (a zirconium-based metal–organic framework), exhibits improved catalytic activity for selective catalytic reduction with H 2 at ambient temperature, compared with that of other platinum-based catalysts with porous materials as supports (see figure). Selective catalytic reduction (SCR) of NO x with H 2 as a reductant is the most promising denitration technology at low temperature. Achieving the conversion of NO x into N 2 at ambient temperature not only prolongs the service life of the catalyst, but also provides more freedom for the arrangement of denitration units throughout the flue gas treatment equipment. However, the development of highly efficient, stable, and environmentally benign supported platinum-based catalysts for H 2 -SCR at ambient temperature is still a major challenge. Herein, a 0.5 wt % Pt/ZrO 2 @C catalyst, which was composed of carbon-coated octahedral ZrO 2 with highly dispersed Pt particles, was prepared by using a new stabilization strategy based on UiO-66-NH 2 (a zirconium metal–organic framework) as a template. The catalytic performance of this Pt/ZrO 2 @C in H 2 -SCR was tested and confirmed to achieve near 100 % NO x conversion at 90 °C. Also, 70 % N 2 selectivity of the catalyst was achieved. The morphology, structure, and porous properties of the as-synthesized nanocomposites were characterized by using data obtained from field-emission SEM, TEM, XRD, Raman spectroscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy, and N 2 adsorption–desorption isotherms. The results show that residual carbon formed by pyrolysis treatment is coated on octahedral ZrO 2 , and effectively prevents the agglomeration of platinum particles on the surface.
研究领域:
化学工程
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材料科学
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环境科学
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Shuxing Zhang,Xiaoshu Ding,Yanji Wang
5-Amino-1-pentanol is an important pharmaceutical intermediate used in the synthesis of anti-inflammatory and anticancer drugs. The direct hydrogenolysis of furfurylamine to 5-amino-1-pentanol has the advantages of a simple process route and high atom utilization. In this paper, for Pt/ZrO2 catalysts, the effects of different Pt loading and calcination temperatures on catalyst activity, selectivity, and surface properties such as Pt nanoparticle size, acidity and alkalinity, and the ratio of Pt0/(Pt0+Pt2+) were investigated. Through the study of the relationship between catalyst preparation conditions, furfurylamine hydrogenolysis reaction performance, and surface properties, it was found that moderate Pt nanoparticle size, higher Pt0/(Pt0+Pt2+) ratio, and more acidic sites favored furfurylamine hydrogenolysis. The higher number of basic sites favors the dispersion of Pt metal. The results of in situ FTIR show that the amino group of furfurylamine is adsorbed on the acidic site of Pt/ZrO2, and the furan ring is adsorbed on Pt nanoparticles, which is beneficial to the hydrogenolysis of furfurylamine.
研究领域:
催化化学
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药物合成
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Ning Lu,Shurui Fan,Yaxu Zhao,Boxuan Yang,Zhongqiu Hua,Yi Wu
In this work, a selective methane gas sensor was prepared based on In 2 O 3 to eliminate the serious cross-sensitive sensitivity to VOCs, NO 2 , and CO, which are typical interfering gases for methane detection in domestic. The catalytic films of Pt-TiO 2 , Pt-CeO 2 , and Pt-ZrO 2 were placed on the top of the sensing layer, i.e., In 2 O 3 loaded with Pd. Catalytic films were designed as filters to catalytically oxidize the interfering gases, such as VOCs, to prevent them reaching the surface of the sensitive layers. Thanks to this design, our sensors showed a high selectivity to methane, even in the presence of ethanol, CO, and NO 2 . In addition, we confirmed via the power-law response of oxygen that the basic sensing mechanism between Pd-In 2 O 3 and the sensor-printed catalytic films are kept the same. Both follow the general model with MOS sensors, which involves an electron transfer process resulting from the adsorption of oxygen on the surface and interaction with methane molecules. The present study showed that catalytic filter films (Pt-TiO 2 , Pt-CeO 2 , and Pt-ZrO 2 ) printed on Pd-In 2 O 3 sensors could enhance the selective response to methane for methane monitoring.
研究领域:
材料科学
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化学传感器
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气体传感技术
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Yao-Dong Hao,Jing-Jing Huang,Xiao-dong Wang,Xi Zhao,Wen-Xia Zhang,Cen Tang,Lu Liu,Wen-Zhi Jia,Meng-Fei Luo,Jian Chen
Developing efficient and durable catalysts for catalytic oxidation reaction remains a major challenge. In this work, we found that Pt/ZrO 2 catalyst demonstrated superior performance compared to Pt sites supported on other oxides (e.g., Pt/Al 2 O 3 , Pt/CeO 2 and Pt/Ce 0.6 Zr 0.4 O 2 ) for styrene combustion. To further understand the active sites in Pt/ZrO 2 catalyst, a series of Pt/ZrO 2 catalysts were synthesized via wet impregnation and calcined at different temperatures (250, 300, 500, 700 and 900 °C). Among them, Pt/ZrO 2 -300 (calcined at 300 °C) exhibited the superior performance for styrene combustion. Comprehensive characterizations revealed that the calcination temperature critically influences the geometric and electronic structures of Pt sites, thus governing the generation of Pt σ+ -ZrO 2 interfacial active sites. A moderate calcination temperature is crucial for forming such interfacial active sites, lower temperatures fail to generate them, while higher temperatures result in nanoparticle sintering and a consequent diminution of these sites. Pt/ZrO 2 -300 features small Pt nanoparticles and a higher concentration of active Pt σ+ species, beneficial for the generation of interfacial active sites. In addition, our findings demonstrate that the superior performance of Pt/ZrO 2 -300 in styrene adsorption and oxygen activation stems from its abundant Pt σ+ -ZrO 2 interfacial active sites. Therefore, this work provides valuable insights for the rational design of robust catalysts with interfacial active sites.
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高影响因子
Molecular Catalysis
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2024
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IF 3.9
Wen-Xia Zhang,Xi Zhao,Lin-Ya Xu,Shuang Xia,Yu-Fen Zhou,Chong-Lai Chen,Hai-Hua He,Meng-Fei Luo,Jian Chen
The surface Pt species and adsorbed oxygen on the Pt/ZrO 2 catalyst were successfully modulated by altering the preparation methods, resulting in distinct catalytic behaviors for CO, n-heptane, and toluene oxidation. The Pt/ZrO 2 catalyst was initially prepared via wetness impregnation and subsequently reduced in an H 2 atmosphere to obtain the Pt/ZrO 2 -R catalyst. In contrast, the Pt/ZrO 2 -E catalyst was synthesized using ethanol solvent (also serving as a reducing agent) instead of water during wetness impregnation. Moreover, the pre-prepared Pt nanoparticles were loaded onto the ZrO 2 surface using polyvinylpyrrolidine (as a protective and structure directing agent) dissolved in ethanol solvent to fabricate the Pt/ZrO 2 -EP catalyst. Among these catalysts, the Pt/ZrO 2 -R exhibits superior catalytic activity towards CO oxidation due to its abundant metallic Pt species. It is found that activity of Pt/ZrO 2 catalyst for n-heptane oxidation is positively correlated with its surface adsorbed oxygen concentration, thus the highest activity is achieved over the Pt/ZrO 2 -EP catalyst possessing a higher concentration of surface adsorbed oxygen species. Unlike CO and n-heptane oxidation, toluene oxidation activity is affected by multiple factors, it is primarily promoted by synergistic catalysis between metallic Pt species (Pt 0 ) and surface adsorbed oxygen species over the Pt/ZrO 2 -EP catalyst. Our preliminary findings underscore that precise modulation of sensitive active sites on surfaces plays a critical role in specific catalytic reactions.
研究领域:
催化化学
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材料科学
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环境科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Shiqi Peng,Rong Li,Yu Huang,Yufei Zhang,Jun-ji Cao,Shuncheng Lee
Producing the strong metal-support interaction (SMSI) interface and highly reactive oxygen species is a great challenge for catalytic oxidation of formaldehyde (HCHO) at room temperature over supported metal catalysts. Herein, we report a conceptual oxygen vacancy ( V O ) associated SMSI interface of Pt-ZrO 2 nanoparticles for HCHO catalysis at room temperature, exhibiting interfacial dependent reactive oxygen species (O*) formation. The V O on the ZrO 2 support captures and activates the molecular O 2 , then proceeds to generating the reactive oxygen atom (O*) with a lower activation barrier of 0.3 eV. The generated O* tends to link the (1 1 0) surface of ZrO 2 and the (1 1 1) surface of Pt as an electronic transmission channel for the selective catalytic oxidation of HCHO adsorbed on the (1 1 0) surface of ZrO 2 , accelerating the direct generation of formate species and mineralization of HCHO. The Pt- V O -ZrO 2 achieves high HCHO removal and HCHO conversion (>95%) at 20 °C. These findings will consolidate the fundamental theories of room temperature catalytic reactions via constructing the SMSI interface engineering for wide environmental applications.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
高影响因子
Molecular Catalysis
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2023
·
IF 4.6
Shuxing Zhang,Jiali Zheng,Zhihui Li,Xiaoshu Ding,Yanji Wang
Herein, we reported a green catalytic reaction system for the synthesis of 5-amino-1-pentanol with furfural and ionic liquid hydroxylamine salt as the initial raw material. In addition, the method can obtain 2-furonitrile and furfurylamine in high yields. The reaction system comprises three new reactions, including the reaction of furfural with ionic liquid hydroxylamine salt to synthesize 2-furonitrile, the hydrogenation of 2-furonitrile to prepare furfurylamine, and the hydrogenolysis of furfurylamine to prepare 5-amino-1-pentanol. For the synthesis of 2-furonitrile, ionic liquid hydroxylamine salt (NH 2 OH) 2 ·[HSO 3 - b - mim ]·HSO 4 was prepared. The ionic liquid as co-solvents, catalysts, and hydroxylamine stabilizer has recovery and reusability. For the hydrogenation of 2-furonitrile to furfurylamine, high-efficiency Ru/g-C 3 N 4 catalyst was prepared. For the hydrogenolysis of furfurylamine to 5-amino-1-pentanol, high-efficiency Pt/ZrO 2 catalyst was prepared. Finally, the yield of 5-amino-1-pentanol based on furfural was 48.7%. A potential pathway for preparing drugs from biomass has been identified in this work.
研究领域:
化学工程
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催化
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绿色化学
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有机合成
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生物质转化
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产品关联
DOI
高影响因子