CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Lijun Yan,Qing Wang,Wenqiang Qu,Tingting Yan,Hongrui Li,Penglu Wang,Dengsong Zhang
Promoting the ring-opening process is vital to increase the mineralization of aromatic volatile organic compounds. Rational regulation of metal-support interaction is essential for the opening of the aromatic ring over Pt/TiO 2 catalysts. Herein, the Pt/TiO 2 -C catalyst with Ti δ+ -Vo·-Pt δ+ interface obtained by reverse electron transfer is successfully regulated via reduction–oxidation treatment for efficient photocatalytic degradation of toluene. This structure accelerates the pre-activation of toluene to generate abundant reactive intermediate species for the photocatalysis reaction. On the other hand, the special interface endows Pt/TiO 2 -C the ability to produce more reactive oxygen species under illumination, which can synergistically promote the direct opening of benzene ring. The Pt/TiO 2 -C shows a stronger oxidation capacity and a mineralization rate 15% higher than the traditional Pt/TiO 2 . This work proves that reduction–oxidation treatment is an effective approach to modify catalysts for air purification and provides a novel idea for the degradation of other aromatic volatile organic pollutants.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
TOPICS IN CATALYSIS
·
2017
·Vol. 60
·期 12
·1009-1015
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IF 2.486
Guo Zhanglong,Huang Qingsong,Luo Shizhong,Chu Wei
A series of Pd/TiO 2 catalysts were prepared by incipient wetness impregnation method followed by atmospheric discharge plasma treatment. In order to study the influences of plasma treatment on the catalysts, the samples were characterized by XRD, TPR, TPD, XPS and TEM technologies. It was found that the plasma treatment catalysts possessed a higher acetylene conversion and ethylene selectivity compared to those of the untreated sample. The enhanced performance of the plasma treated catalyst was mainly dependent on two main effects. On one hand, the treated catalyst possessed a higher metal Pd dispersion, which resulted in the easier activation of acetylene. On the other hand, the surface electron density of metal Pd on the treated catalyst got enhanced compared to that of untreated sample, because of the stronger interaction between TiO 2 support and metallic Pd, helping the more desorption of ethylene species from the surface of catalyst.
研究领域:
催化化学
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材料科学
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物理化学
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工业催化
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纳米材料
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DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Jinshi Dong,Ting Li,Shengtong Li,Panpan Chang,Qianqian Jin,Jiaqiang Yang,Zhuangzhuang Lai
CO and C3H8, as typical inorganic and organic gaseous pollutants, respectively, require distinct oxidation catalysts for efficient conversion due to their unique properties. In this work, Pt catalysts with different crystal phases of TiO2 (anatase and rutile) as supports were fabricated and investigated for CO oxidation and C3H8 combustion. The surface nature of TiO2 dramatically affects the local environment and electronic properties of supported Pt. Pt-TiO2(R) exhibited superior activity for CO oxidation, whereas Pt-TiO2(A) showed higher reactivity for C3H8 total oxidation. It is concluded that Pt-TiO2(R) contains more oxygen vacancies at the interfacial Pt perimeter sites than Pt-TiO2(A) after reduction pretreatments, which facilitates CO oxidation through the Mars–van Krevelen (MvK) mechanism. The electron-deficient Pt in Pt-TiO2(A) promotes the adsorption and activation of C3H8, and the amount of charge transfer between Pt and adsorbate intermediates during C3H8 oxidation determines the preference of C-C cleavage or dehydrogenation. Lower charge transfer in Pt-TiO2(A) makes C–C cleavage more efficient and contributes to the total oxidation of C3H8. This work emphasizes the importance of engineering material’s local environment and electronic structure to design high-performance oxidation catalysts.
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2021
·Vol. 96
·期 6
·1553-1560
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IF 3.174
Sibo Li,Jiaxun Zhang,Hualiang An,Guirong Wang,Xinqiang Zhao,Yanji Wang
BACKGROUND The reaction integration of butanal self-condensation and successive hydrogenation (that is, one-step synthesis of 2-ethylhexanol from butanal) is an efficiency way to simply process flow and reduce energy consumption for the commercial manufacture of 2-ethylhexanol (2EHO). In the present work, a NiO-MnO 2 /Nb 2 O 5 -TiO 2 catalyst was prepared for the integration reaction to reach a high 2-ethylhexanol selectivity. Furthermore, the reaction integration was investigated kinetically for the next scale-up. RESULTS A 2EHO selectivity of 90.0% was achieved at a complete conversion of butanal with the help of reduction-in-reaction technique in this reaction integration. The reaction rate of butanal is determined by the reversible aldol self-condensation reaction and its direct hydrogenation reaction. The reaction order with respect to butanal in the two reactions is, respectively, 2.004 and 1.004. The activation energy of the hydrogenation reaction is higher than that of the forward reaction of the self-condensation, suggesting the suppressive effect the reaction integration on the direct hydrogenation. CONCLUSION The reaction integration promotes butanal self-condensation and successive hydrogenation and it suppresses butanal direct hydrogenation by using NiO-MnO 2 /Nb 2 O 5 -TiO 2 catalyst with the help of reduction-in-reaction technique, giving rise to a pretty high selectivity of 2-ethylhexanol. The establishment of the integration reaction kinetics will lay the foundation for reactor design and analysis. © 2021 Society of Chemical Industry
研究领域:
化学工程
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催化化学
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反应动力学
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DOI
高影响因子
FUEL
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2022
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IF 8.035
Zhuojie Zhong,Junxuan Li,Minyin Jian,Riyang Shu,Zhipeng Tian,Chao Wang,Ying Chen,Ning Shi,Yanxue Wu
Hydrodeoxygenation (HDO) reaction is a necessary refinery process for lignin-derived phenolic compounds to be used as high quality liquid fuels. Catalyst morphology makes a big difference on the HDO performance through changing the properties of metal site and acid site, while the catalytic mechanism is still not very clear. In this work, four kinds of Ru/TiO 2 catalysts with different morphology were prepared by photochemical method and all of them achieved a high Ru metal dispersion. A series of catalyst characterizations were carried out, including XRD, BET, SEM, TEM, H 2 -TPD and NH 3 -TPD, in order to explore the crystal structure, surface property, Ru metal dispersion, hydrogen adsorption capacity as well as acid properties. Results showed that Ru/TNP catalyst possessed a large surface area, an abundance of medium strength acid sites and a good hydrogen adsorption capacity. The HDO performances on lignin-derived phenolic compounds were also compared, in which Ru/TNP catalyst presented the best HDO performance. The guaiacol conversion and the selectivity of cyclohexane product were both close to 100 % at 250 °C under 1 MPa hydrogen pressure. Moreover, the content of hydrocarbons increased from 11.1 % to 60.8 % in the lignin-oil upgrading process.
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
Catalysts
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2021
·Vol. 11
·期 4
·445
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IF 4.146
Yangyang Guo,Xiaofei Xu,Hong Gao,Yang Zheng,Lei Luo,Tingyu Zhu
Ca poisoning behavior is inevitable for high-calcium content flue gas, so V2O5-WO3/TiO2(VWT) and V2O5-WO3-CeO2/TiO2(VWCeT) catalysts with different vanadium content have been prepared and the Ca-doped catalysts are compared in this manuscript. The result shows Ce addition can both promote the NO conversion and the alkali resistance. Lower Ca addition for 0.1VWCeT catalyst promotes its oxidability and Ce modification is more suitable for low vanadium catalysts. The total acidity and the reducibility of catalysts decline after Ca doping, and the reducibility of the active species on catalysts has been strengthened by Ce addition. CeO2based catalysts with lower Ca loading struggle to resist sulfur poisoning, while higher Ca loading favors SO2adsorption and also physically reduces the cerium acidification process. In the presence of SO2, additional Brønsted acid sites are formed in Ca rich catalyst. The dynamic NH3adsorption has been investigated, shows that Ca doping content on catalyst is critical for SCR reaction, and the catalyst is more susceptible to SO2initially in alkali flue gas during the actual application, but the sulfur resistance may increase with the alkali-poisoning effect aggravated by Ca doping.Keywords:Ca-poisoning;SCR reaction;NO reduction;V2O5-WO3/TiO2and V2O5-WO3-CeO2/TiO2catalysts;SO2and water;NO removal efficiency
研究领域:
环境科学
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催化化学
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DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
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2019
·Vol. 128
·期 2
·681-693
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IF 1.428
Xie Chong,Yang Shenghui,Shi Jian-Wen,Niu Chunming
A novel MnO x –TiO 2 catalyst with hollow silkworm structure was synthesized successfully via an ethanol-thermal strategy by using activated carbon fiber felt as template for the first time. The silkworm-like MnO x –TiO 2 catalyst (MnTi) exhibited higher NO x conversion in the whole experimental temperature region (90–330 °C) under a high space velocity of 36,000 h −1 in comparison with the common MnO x –TiO 2 catalyst without hollow silkworm structure (MnTi-B). The excellent catalytic performance of MnTi can be attributed to its high specific surface area, large content of active surface oxygen species (O S ), and more surface acid sites. In addition, the MnTi catalyst also exhibited excellent resistance to water or SO 2 poisoning.
研究领域:
催化化学
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环境科学
✓ 已验证
DOI
高影响因子
Industrial Chemistry & Materials
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2025
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IF 11.9
Yan-Chao Qu,Guangyue Xu,Chen Chen,Jianhua Guo,Dingjia Liu,Haiwei Jia,Haonan Guo,Shuya Jia,Jiazhen Jia,Ying Zhang,Lifeng Yan
The development of novel low-temperature selective catalytic reduction (SCR) denitrification catalysts is a crucial research direction for reducing pollution and carbon emissions. Although V2O5-MoO3/TiO2 catalysts have been widely used in commercial applications, achieving effective SCR denitrification for low-temperature flue gases remains a significant challenge. In this study, the catalytic efficiency of the catalysts was systematically investigated and optimized by constructing Pearson linear correlation coefficient models between catalytic activity and different pore structures, substrate crystal planes, and active site components and properties, etc. Through comprehensive characterizations and experiments, anatase TiO2 loaded with 3% V2O5 and 10% MoO3 was developed and demonstrated excellent catalytic activity and stability even in high sulfur content and low-temperature environments. The catalyst was deployed in a pilot plant for over two years, consistently achieving a monthly average denitrification efficiency of over 67% and maintaining an outlet NOx concentration below 50 mg/Nm³. This study provides a robust and efficient low-temperature catalyst for SCR denitrification and offers valuable insights for future catalyst optimization.
研究领域:
环境科学
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催化
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化学工程
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材料科学
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产品关联
DOI
高影响因子
Nature Catalysis
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2020
·Vol. 3
·期 2
·170-178
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IF 30.471
Huang Zhipeng,Zhao Zhitong,Zhang Chaofeng,Lu Jianmin,Liu Huifang,Luo Nengchao,Zhang Jian,Wang Feng
The decarboxylation of bio-derived fatty acids provides a sustainable pathway for the production of alkane products under mild conditions; however, products are generally obtained in low selectivity due to the uncontrollable reactivity of radical intermediates. Here we demonstrate that photogenerated radicals can be rapidly terminated by surface hydrogen species during photocatalytic decarboxylation of fatty acids on a hydrogen-rich surface that is constructed by the interactions between H 2 and Pt/TiO 2 catalyst, thereby greatly inhibiting oligomerization; C n – 1 alkanes can therefore be obtained from bio-derived C 12 –C 18 fatty acids in high yields (≥90%) under mild conditions (30 °C, H 2 pressure ≤0.2 MPa) and 365 nm light-emitting dode irradiation. Industrial low-value fatty acid mixtures (namely, soybean and tall oil fatty acids) can be transformed into alkane products in high yields (up to 95%). Our research introduces an efficient biomass-upgrading approach that is enabled by subtle control of the radical intermediate conversion on a heterogeneous surface.
研究领域:
化学工程
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催化
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
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IF 7.5
Zhangkai Qian,Jia-qi Bai,Mei Ma,Huangfei Liu,Mengdie Cai,Jingshuai Chen,Song Sun
N -methylation of amines, nitro compounds and nitriles with CO 2 and H 2 offers a promising strategy for CO 2 utilization. However, developing highly efficient and stable Cu-based catalysts for selective mono- N -methylation of aniline remains challenging. Herein, we report the successful synthesis of a Cu-ZnO/TiO 2 catalyst, with the optimized 5 %Cu-7.5 %ZnO/TiO 2 catalyst achieving a 96.7 % yield of N -methylaniline (MA) and an initial turnover frequency (TOF) of 7.4 h −1 after 6 h under 453 K, 2 MPa CO 2 and 4 MPa H 2 . This performance surpasses all reported Cu-based catalysts and rivals noble metal-based systems. The catalyst demonstrated reusability at least four cycles and versatility in the N -methylation of various amines, nitro compounds, and nitriles. Kinetic studies revealed reaction orders of 0 with respect to aniline concentration and CO 2 pressure, and 1 with respect to H 2 pressure. Based on kinetics and extensive characterization, we propose a reaction mechanism over 5 %Cu-7.5 %ZnO/TiO 2 , identifying Cu nanoparticles as the active sites. The process proceeds via N -phenylcarbamic acid and N -phenylformamide intermediates, with the hydrogenation of N -phenylcarbamic acid as the rate-determining step.
研究领域:
化学工程
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催化科学
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环境科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Guang Gao,Zelun Zhao,Jia Wang,Yongjie Xi,Peng Sun,Fuwei Li
ABSTRACT Engineering the surface microenvironment by tuning the binary interactions between a supported metal with a secondary metal oxide (MO x ) or support has been a common method for improving the catalytic performance of supported metal catalysts. However, few studies have investigated the ternary interactions among the metal, MO x , and support. Here, we report for the first time the formation of metal-MO x -support interaction (MMSI) in reducible TiO 2 -supported PtReO x catalysts, affording 87% yield and 100% ee in the tandem hydrogenation of an aqueous chiral cyclohexane-1,2-dicarboxylic acid into the corresponding diol; the catalytic activity is eight times higher than that obtained with non-reducible support counterparts in the same reaction via traditional batch synthesis with multiple steps and unfriendly reagents. Detailed experimental and computational studies suggest that the TiO 2 crystalline phase-dependent density of the oxygen vacancies induces different Pt-ReO x -TiO 2 interactions, which dominate the electron transfer therein and tune the adsorption strength of the carbonyl moiety of the substrate/intermediate, thus promoting the hydrogenation activity and selectivity. In addition, the strong MMSI endows the optimal rutile TiO 2 supported PtReO x catalyst with an outstanding lifetime of 400 h in a fixed-bed reactor under acidic aqueous conditions and ensures efficient applications in the selective hydrogenation of aliphatic dicarboxylic acids and functional carboxylic acids. This work provides a promising strategy for the development of efficient and stable supported catalysts for the selective hydrogenation of diverse C–O and C=O bonds.
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
ACS Catalysis
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2019
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IF 12.221
Xiaoqiang Zhang,Peifang Yan,Bin Zhao,Kairui Liu,Mayfair C. Kung,Harold H. Kung,Shanyong Chen,Z. Conrad Zhang
The catalytic properties of physical mixtures of Ni particles (100–200 nm) with nanoparticles of anatase TiO2 (TiO2-A), ZrO2, Al2O3, rutile TiO2 (TiO2-R), and CeO2 were investigated for the hydrodeoxygenation (HDO) of guaiacol. High selectivities to phenolics were obtained only for Ni mixed with anatase TiO2 (Ni and TiO2-A), while saturated hydrocarbons were the main products for the mixtures with other supports. By thermal treatment in hydrogen gas only at 300 °C or higher and subsequently separating the large Ni particles from the TiO2-A particles with a magnet, it was further discovered that there was migration of TiO2 from TiO2-A onto the large Ni particles, resulting in an amorphous TiO2 overlayer on the Ni particles as evidenced by high-resolution TEM, and vice versa, migration of Ni onto TiO2-A. The TiO2 overlayer rendered the Ni particles completely inactive as a hydrogenation/hydrodeoxygenation catalyst. Conversely, the small amounts of Ni (<1.5 wt %) migrated onto TiO2-A formed highly dispersed Ni, undetectable by high-resolution TEM (<2 nm), that were remarkably highly active for HDO of guaiacol, producing selectively phenolics. Such highly selective HDO catalysts could also be formed by incipient wetness impregnation of Ni in loadings above 2 wt % onto the TiO2-A, but it was essential to pretreat the sample in H2 at 300 °C or higher. Pretreatment in H2 at 200 °C generated catalysts that produced saturated ring products. The activity of the impregnated catalysts, as measured by guaiacol conversion, increased linearly with Ni loading below 0.5 wt %. The activity continued to increase with Ni loading but more slowly up to 2 wt %, beyond which there was little further change. The results suggested that two types of Ni species existed on the TiO2-A surface. One type consisted of a cluster of Ni atoms that were dominant on larger Ni particles that were active in aromatic ring hydrogenation and hydrodeoxygenation. They were readily covered by reducible TiO2-A at 300 °C or higher due to the traditional strong metal support interaction (SMSI) effect and became inactive. Another type was clusters of a very small number of Ni atoms, perhaps one atom, that were present as highly dispersed Ni clusters interacting strongly with the defect sites of TiO2-A. The strong interaction of this type of Ni with the TiO2 defect deterred TiOx migration allowing surface exposed Ni atoms to catalyze the HDO of guaiacol with very high selectivities that were not characteristic of typical Ni particles.
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）