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学者姓名:谭理
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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 Td-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 Td-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 C3H6 generation rate of 3014 mmol C 3 H 6 g Co-1 h-1 and deactivation rate of 0.07 h-1 at 550 degrees C.
Keyword :
Hydrothermal treatment Hydrothermal treatment Propane dehydrogenation Propane dehydrogenation Silanol nests Silanol nests Silicalite-1 Silicalite-1 Td-Co(II) Td-Co(II)
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GB/T 7714 | Deng, Huihui , Li, Baozhen , Zheng, Wenchun et al. Regulation of silanol nests in zeolite to form stable Td-Co(II) species for efficient propane dehydrogenation [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 505 . |
MLA | Deng, Huihui et al. "Regulation of silanol nests in zeolite to form stable Td-Co(II) species for efficient propane dehydrogenation" . | CHEMICAL ENGINEERING JOURNAL 505 (2025) . |
APA | Deng, Huihui , Li, Baozhen , Zheng, Wenchun , Sun, Qin , Zhu, Mengjia , Zuo, Jun et al. Regulation of silanol nests in zeolite to form stable Td-Co(II) species for efficient propane dehydrogenation . | CHEMICAL ENGINEERING JOURNAL , 2025 , 505 . |
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The use of bifunctional catalysts, combining methanol synthesis and zeolite components, has been cleverly expanding to the hydrogenation of CO2 into liquefied petroleum gas (LPG). However, such catalysts in this reaction displayed low catalytic efficiency due to the mismatch of the two components. In this study, an efficient strategy was realized via physically coating beta zeolite onto the CuZnAl methanol catalyst, resulting in a shell thickness controllable core-shell encapsulated catalyst, denoted as CuZnAl@beta. Sufficient characterization proves that the micro-coupling structure between methanol active sites and zeolite acid sites is designed reasonably and successfully, as consequently, the zeolite capsule catalysts embody a significant improvement toward LPG selectivity. Hence, the CuZnAl@beta catalyst reached a high selectivity to LPG at 77.9% with 21.3% CO2 conversion, under a reaction pressure of 2.0 MPa and a temperature of 320 degrees C. The strategy employed in this study could offer valuable insights into guiding catalyst design.
Keyword :
beta zeolite beta zeolite Bifunctional active sites Bifunctional active sites Capsule catalyst Capsule catalyst CO2 hydrogenation CO2 hydrogenation Liquefied petroleum gas Liquefied petroleum gas
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GB/T 7714 | Zhang, Peipei , Huang, Xin , Qu, Shunli et al. Direct conversion of carbon dioxide into liquefied petroleum gas over zeolite capsule catalyst [J]. | RESEARCH ON CHEMICAL INTERMEDIATES , 2025 , 51 (2) : 675-693 . |
MLA | Zhang, Peipei et al. "Direct conversion of carbon dioxide into liquefied petroleum gas over zeolite capsule catalyst" . | RESEARCH ON CHEMICAL INTERMEDIATES 51 . 2 (2025) : 675-693 . |
APA | Zhang, Peipei , Huang, Xin , Qu, Shunli , Wang, Peng , Mi, Xiaotong , Li, Sixuan et al. Direct conversion of carbon dioxide into liquefied petroleum gas over zeolite capsule catalyst . | RESEARCH ON CHEMICAL INTERMEDIATES , 2025 , 51 (2) , 675-693 . |
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Significant progress has been evidenced in the development of the synergistic effect of the various active sites for selective catalyzing CO2 hydrogenation toward the target product. Unveiling the roles of different active sites is conducive to understanding the structure-activity relationship in complex reactions. In this study, the pretreatment atmosphere plays a pivotal role in modulating active site properties. The optimized Ar-pretreated Cu-UiO-66-Ar catalyst shows a high methanol space-time yield of 733 mu mol g(cat.)(-1)h(-1) at 200 degrees C, 3.0 MPa, which is 2.7 times than that of H-2-pretreated Cu-UiO-66-H-2 catalyst (274 mu mol g(cat.)(-1)h(-1)). We revealed the interface (Cu-O-Zr sites) and Cu nanoparticles (Cu-Cu sites) co-play a pivotal role in promoting CO2 conversion and H-2 dissociation via Cu-Cu sites feeds H* to Cu-O-Zr-anchored CO*/HCO* species. Rational contrast experiments of the in-situ DRIFTS highlight the accelerated elementary steps in the CO2 conversion process contact with the enhanced catalytic activity. Thus, this work is helpful to advance the understanding of the potential mechanism in a composite cross-reaction network.
Keyword :
Bynergistic effect Bynergistic effect CO2hydrogenation CO2hydrogenation Cu nanoparticles Cu nanoparticles Interface Interface Methanol Methanol
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GB/T 7714 | Cao, Fenghai , Liu, Junhao , Xu, Kaizhuang et al. Optimized Active Structure Configuration of the MOF Derived Cu-based Catalysts via Different Atmospheres for Selective CO2 Hydrogenation [J]. | APPLIED SURFACE SCIENCE , 2025 , 698 . |
MLA | Cao, Fenghai et al. "Optimized Active Structure Configuration of the MOF Derived Cu-based Catalysts via Different Atmospheres for Selective CO2 Hydrogenation" . | APPLIED SURFACE SCIENCE 698 (2025) . |
APA | Cao, Fenghai , Liu, Junhao , Xu, Kaizhuang , Tang, Yu , Wu, Lizhi , Wang, Peng et al. Optimized Active Structure Configuration of the MOF Derived Cu-based Catalysts via Different Atmospheres for Selective CO2 Hydrogenation . | APPLIED SURFACE SCIENCE , 2025 , 698 . |
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Alkali metal promoted Zn/SSZ-13 catalysts were investigated for ethane dehydrogenation (EDH) and CO2assisted oxidative ethane dehydrogenation (CO2-EDH). The Zn/Na/K/SSZ-13 demonstrated enhanced ethane dehydrogenation performance, achieving 0.381 mol C2H4 gZn 0.04 h-1 in the CO2-EDH process after 440 min time on stream, compared to the unmodified Zn/SSZ-13 catalyst. Comprehensive characterizations revealed that the isolated Zn2+ species serve as the active sites for dehydrogenation, while the addition of alkali metals compensate the acid sites of SSZ-13, effectively suppressing the side reactions such as cracking. Moreover, the introduction of CO2 mitigates Zn loss and enhances catalyst activity and stability by coupling with the reverse water gas shift reaction (RWGS), which also suppress the coke deposition. Investigation of vary CO2 content indicated that higher CO2 concentrations significantly suppress Zn loss and increase the proportion of the RWGS reaction, thereby improving CO2-EDH catalytic performance. This work elucidates the active phase of ethane dehydrogenation and highlights the role of alkali metals and CO2 in the CO2-EDH process over Zn/Na/K/SSZ-13, providing valuable insights for designing high-performance CO2EDH catalysts.
Keyword :
Alkaline metal Alkaline metal Carbon dioxide Carbon dioxide Ethane Ethane Ethylene Ethylene Oxidative dehydrogenation Oxidative dehydrogenation Reverse water-gas shift Reverse water-gas shift Zeolite Zeolite Zinc Zinc
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GB/T 7714 | Wu, Lizhi , Zheng, Wenchun , Wang, Xiaofang et al. Mechanistic interpretations and insights for the oxidative dehydrogenation of ethane with CO2 over alkali metal modified Zn/SSZ-13 catalyst [J]. | MOLECULAR CATALYSIS , 2025 , 579 . |
MLA | Wu, Lizhi et al. "Mechanistic interpretations and insights for the oxidative dehydrogenation of ethane with CO2 over alkali metal modified Zn/SSZ-13 catalyst" . | MOLECULAR CATALYSIS 579 (2025) . |
APA | Wu, Lizhi , Zheng, Wenchun , Wang, Xiaofang , He, Juncheng , Zou, Caixin , Zhu, Mengjia et al. Mechanistic interpretations and insights for the oxidative dehydrogenation of ethane with CO2 over alkali metal modified Zn/SSZ-13 catalyst . | MOLECULAR CATALYSIS , 2025 , 579 . |
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Ethane dehydrogenation to aromatics (EDA) is one of the most promising routes to produce aromatics. Herein, the tandem of dehydrogenation component and acidic zeolite are prepared and investigated for EDA. Pt/Fe-S-1 coupled with ZSM-5 of Si/Al of 14 via mixing homogeneously shows excellent EDA performance with 54.0% ethane conversion, 61.5% aromatics selectivity as well as a deactivation rate constant of 0.00010 h-1. According to catalysts characterizations and controlled experiments, it is confirmed the highly dispersed positive Pt delta+ species around Fe species over Pt/Fe-S-1 is the active sites for ethane dehydrogenation to ethylene and subsequent naphthenes dehydrogenation to aromatics, Br & oslash;nsted acid sites of ZSM-5 and MFI pore are responsible for ethylene oligomerization and cyclization to naphthenes and further naphthenes dehydrogenation to aromatics. The short spatial space between dehydrogenation active sites and acid sites is beneficial for EDA. And the ethylene generation rate is the rate-determining step of EDA.
Keyword :
dehydroaromatization dehydroaromatization Pt/Fe-S-1 Pt/Fe-S-1 the tandem catalysis the tandem catalysis ZSM-5 ZSM-5
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GB/T 7714 | Wu, Lizhi , Zhang, Ying , Zou, Caixin et al. Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization [J]. | AICHE JOURNAL , 2025 , 71 (5) . |
MLA | Wu, Lizhi et al. "Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization" . | AICHE JOURNAL 71 . 5 (2025) . |
APA | Wu, Lizhi , Zhang, Ying , Zou, Caixin , Sun, Qin , Li, Baozhen , Zheng, Wenchun et al. Integration of Pt/Fe-silicalite-1 and acidic zeolite as a bifunctional catalyst for boosting ethane dehydroaromatization . | AICHE JOURNAL , 2025 , 71 (5) . |
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The utilization of Cu-based catalysts in the low-temperature catalytic conversion of CO2 to methanol is the focus of industrial processes. However, the metastable nature of highly dispersed Cu active sites causes it easy to sinter, which leads to the decline of activity and methanol selectivity. Herein, an approach involving the incorporation of highly dispersed La species into Cu-ZnO-Al2O3 (CZAL-x) through one-pot synthesis, benefits dispersing and stabilizing Cu0/Cu+ active sites. Consequently, a CO2 conversion reaches 22.4 % with a 75.0 % methanol selectivity of the optimizing CZAL-2.5 catalyst in a stable reaction for 100 h. When the space velocity is 16,000 mL g cat.- 1 h- 1 , the space-time yield of methanol reached the highest value of 814.9 g MeOH kg cat1 h- 1 , significantly outperforming the CZA catalyst. Systematic characterizations reveal the introduction of LaOx enhanced the interaction between Cu active sites and carrier, which effectively improved the sintering resistance of copper nanoparticles.
Keyword :
Anti-sintering Anti-sintering CO2 hydrogenation reaction CO2 hydrogenation reaction Highly dispersed LaOx Highly dispersed LaOx Methanol selectivity Methanol selectivity Robust Cu active sites Robust Cu active sites
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GB/T 7714 | Zhang, Peipei , Wang, Wenbo , Wang, Peng et al. Tuning catalytic performance of CuZnOx catalyst via functional LaOx for catalyzing CO2 hydrogenation reaction [J]. | MOLECULAR CATALYSIS , 2025 , 573 . |
MLA | Zhang, Peipei et al. "Tuning catalytic performance of CuZnOx catalyst via functional LaOx for catalyzing CO2 hydrogenation reaction" . | MOLECULAR CATALYSIS 573 (2025) . |
APA | Zhang, Peipei , Wang, Wenbo , Wang, Peng , Mi, Xiaotong , Xin, Jing , Li, Sixuan et al. Tuning catalytic performance of CuZnOx catalyst via functional LaOx for catalyzing CO2 hydrogenation reaction . | MOLECULAR CATALYSIS , 2025 , 573 . |
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Direct conversion of CO2 into light olefins (C2-C4=) offers a promising approach to mitigating CO2 emissions and lessening reliance on feedstock derived from petroleum-based feedstocks while generating high value-added chemicals. Achieving an effective synergy between Fe3O4 and Fe5C2 is crucial for the hydrogenation of CO2. However, the mechanisms underlying this synergy and strategies for its optimization remain inadequately explored. Herein, we clearly addressed this issue by synthesizing a range of FeNa/NC-x catalysts, wherein the precise control of the Fe5C2/Fe3O4 ratio was manipulated through the adjustment of the initial amount of Fe precursor (denoted by x in the catalysts' names). Among the synthesized catalysts, FeNa/NC-0.6, with the Fe5C2/ Fe3O4 ratio of 2.4, displays the superior CO2 conversion (32.6 %) and STYC2-C4= (54.6 mu molCO2 gFe- 1 s- 1). Moreover, its remarkable C2-C4 = selectivity (47.6 %) and ultra-high STYC2-C4= both fall into a high level among reported Fe-based catalysts for CO2 hydrogenation to light olefins. The excellent catalytic performance can be attributed to the optimized synergistic effect of Fe3O4 and Fe5C2. Reducing the initial amount of Fe precursor weakens the metal-support interaction, which in turn increases the Fe5C2/Fe3O4 ratio. This adjustment results in a perfect balance between the density of CO* intermediates and the quantity of Fe5C2 active sites when the ratio reaches 2.4, thereby enhancing the Fischer-Tropsch synthesis (FTS) process and ultimately improving the catalytic efficiency for CO2 hydrogenation. This paper offers a strategy to optimize synergy of Fe3O4 and Fe5C2 for enhancing catalytic performance and a mechanistic insight, which can be utilized in designing efficient catalysts for other heterogeneous catalytic reactions.
Keyword :
CO 2 hydrogenation CO 2 hydrogenation Iron carbides Iron carbides Iron oxides Iron oxides Light olefins Light olefins Synergistic effect Synergistic effect
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GB/T 7714 | Liu, Yunhao , Cheng, Qingpeng , Xiong, Shaohui et al. Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides [J]. | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2025 , 104 : 66-75 . |
MLA | Liu, Yunhao et al. "Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides" . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 104 (2025) : 66-75 . |
APA | Liu, Yunhao , Cheng, Qingpeng , Xiong, Shaohui , Zhang, Yingtian , Tan, Li , Song, Song et al. Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides . | INTERNATIONAL JOURNAL OF HYDROGEN ENERGY , 2025 , 104 , 66-75 . |
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The preparation of Co-based catalysts with a single, highly dispersed active site is challenging and crucial for the high-performance propane dehydrogenation (PDH) owing to harsh reaction conditions. Herein, the synergetic strategies including catalyst hydrothermal treatment and CO2 introduction are adopted to realize the highly dispersed and stable T-d-Co(II) site and applied for PDH. According to systematic characterizations and catalytic performance evaluation, the facial hydrothermal treatment improves the C3H6 formation rate from 456 to 771 mmol C3H6 g(Co)(-1) h(-1) and catalyst stability via the transformation of Co3O4 species to the T-d-Co(II) species. Meanwhile, the further introduction of CO2 into the PDH system as a protective reagent for Co state would facilitate PDH with superior catalytic performance with TOF of 700 h(-1) and C3H6 formation rate of 970 mmol C3H6 g(Co)(-1) h(-1). It is revealed that the introduction of CO2 maintains Co state with the T-d-Co(II) species via inhabiting the generation of metallic Co spices.
Keyword :
carbon dioxide carbon dioxide Co/S-1 Co/S-1 hydrothermal treatment hydrothermal treatment propane dehydrogenation propane dehydrogenation T-d-Co(II) T-d-Co(II)
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GB/T 7714 | Deng, Huihui , Sun, Qin , Zheng, Wenchun et al. Obtaining highly stable Td-Co(II) site by coupling hydrothermal method and CO2 introduction for propane dehydrogenation [J]. | AICHE JOURNAL , 2024 , 70 (5) . |
MLA | Deng, Huihui et al. "Obtaining highly stable Td-Co(II) site by coupling hydrothermal method and CO2 introduction for propane dehydrogenation" . | AICHE JOURNAL 70 . 5 (2024) . |
APA | Deng, Huihui , Sun, Qin , Zheng, Wenchun , Li, Baozhen , Zhuo, Zuoxi , Wang, Xiaofang et al. Obtaining highly stable Td-Co(II) site by coupling hydrothermal method and CO2 introduction for propane dehydrogenation . | AICHE JOURNAL , 2024 , 70 (5) . |
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The direct activation of methane under mild condition to achieve highly selective of oxygenates is a challenging project. In this study, a well dispersed silver supported ZnTiO 3 catalyst was prepared to achieve selective preparation of methanol from methane and water under mild condition. X-ray diffraction, transmission electron microscopy and X-ray photoelectron spectroscopy characterizations demonstrate that silver species are uniformly dispersed on ZnTiO 3 surface in the form of metallic silver nanoparticles. The photoelectric characterizations reveal that the addition of silver species enhances light absorption and promotes charge separation of the catalysts. Under the reaction conditions of 50 degrees C and 3 MPa, the methanol is obtained as the only liquid product over the designed Ag/ZnTiO 3 catalyst under light irradiation. In this photocatalytic process, the holes generated by ZnTiO 3 activate water to produce intermediate center dot OH, which further reacts with methane to synthesize methanol. The silver species as co -catalysts extend the light absorption range of ZnTiO 3 as well as promote charge separation. (c) 2024 Chinese Society of Rare Earths. Published by Elsevier B.V. All rights reserved.
Keyword :
Methane oxidation Methane oxidation Methanol Methanol Photocatalytic Photocatalytic Silver Silver Zinc titanate Zinc titanate
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GB/T 7714 | Gan, Yuyan , Huang, Jinbi , Lv, Qian et al. Photocatalytic oxidation of methane to methanol over zinc titanate supported silver catalysts [J]. | JOURNAL OF RARE EARTHS , 2024 , 42 (5) : 899-906 . |
MLA | Gan, Yuyan et al. "Photocatalytic oxidation of methane to methanol over zinc titanate supported silver catalysts" . | JOURNAL OF RARE EARTHS 42 . 5 (2024) : 899-906 . |
APA | Gan, Yuyan , Huang, Jinbi , Lv, Qian , Li, Yanru , Wu, Lizhi , Tang, Yu et al. Photocatalytic oxidation of methane to methanol over zinc titanate supported silver catalysts . | JOURNAL OF RARE EARTHS , 2024 , 42 (5) , 899-906 . |
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Doping is a recognized method for enhancing catalytic performance. The introduction of strains is a common consequence of doping, although it is often overlooked. Differentiating the impact of doping and strain on catalytic performance poses a significant challenge. In this study, Cu-doped Bi catalysts with substantial tensile strain are synthesized. The synergistic effects of doping and strain in bismuth result in a remarkable CO2RR performance. Under optimized conditions, Cu-1/6-Bi demonstrates exceptional formate Faradaic efficiency (>95%) and maintains over 90% across a wide potential window of 900 mV. Furthermore, it delivers an industrial-relevant partial current density of -317 mA cm(-2) at -1.2 V-RHE in a flow cell, while maintaining its selectivity. Additionally, it exhibits exceptional long-term stability, surpassing 120 h at -200 mA cm(-2). Through experimental and theoretical mechanistic investigations, it has been determined that the introduction of tensile strain facilitates the adsorption of *CO2, thereby enhancing the reaction kinetics. Moreover, the presence of Cu dopants and tensile strain further diminishes the energy barrier for the formation of *OCHO intermediate. This study not only offers valuable insights for the development of effective catalysts for CO2RR through doping, but also establishes correlations between doping, lattice strains, and catalytic properties of bismuth catalysts.
Keyword :
bismuth bismuth CO2 reduction CO2 reduction doping doping strain strain synergistic effect synergistic effect
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GB/T 7714 | Wei, Yang , Xu, Xin , Shi, Dehuan et al. Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction [J]. | SMALL , 2024 , 20 (34) . |
MLA | Wei, Yang et al. "Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction" . | SMALL 20 . 34 (2024) . |
APA | Wei, Yang , Xu, Xin , Shi, Dehuan , Jiang, Yaming , Zheng, Chaoyang , Tan, Li et al. Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction . | SMALL , 2024 , 20 (34) . |
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