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学者姓名:谭理
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This review provides a comprehensive overview of the distinguished academic career and scientific accomplishments of Prof. Noritatsu Tsubaki at the University of Toyama. For over 35 years, he has dedicated himself to the research field of one-carbon (C1) chemistry, including catalytic conversion of C1 molecules to valuable chemicals and superclean fuels, innovative catalyst and reactor development, and the design of new catalytic reactions and processes. Organized chronologically, this review highlights Prof. Tsubaki's academic contributions from 1990, when he studied and worked at The University of Tokyo, to his current role as a full professor at the University of Toyama. The academic section of this review is divided into three main parts, focusing on Prof. Tsubaki's pioneering work in C1 chemistry. We believe that this review will serve as a highly valuable reference for colleagues in the fields of C1 chemistry and catalysis, and inspire the development of more original and groundbreaking research. © 2023
Keyword :
Bimodal catalysts Bimodal catalysts Capsule Catalysts Capsule Catalysts Fischer-Tropsch Synthesis Fischer-Tropsch Synthesis Low-temperature methanol Low-temperature methanol Tandem catalysis Tandem catalysis
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GB/T 7714 | Yao, J. , Cao, F. , Han, Y. et al. C1 Chemistry: The Stories of Research and Applications from Toyama [J]. | Resources Chemicals and Materials , 2024 , 3 (1) : 62-92 . |
MLA | Yao, J. et al. "C1 Chemistry: The Stories of Research and Applications from Toyama" . | Resources Chemicals and Materials 3 . 1 (2024) : 62-92 . |
APA | Yao, J. , Cao, F. , Han, Y. , Wang, Y. , Tan, L. , Sun, J. et al. C1 Chemistry: The Stories of Research and Applications from Toyama . | Resources Chemicals and Materials , 2024 , 3 (1) , 62-92 . |
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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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Lignin derivatives are one class of attractive alternative feedstocks for the production of renewable biofuels. Herein, hydrodeoxygenation (HDO) of lignin derivatives was carried out using a single-atom catalyst (SAC) comprised of Ni-1 SAC on beta-Mo2C. A number of lignin-derived compounds have been investigated, and nearly 100% yield of biofuel molecules was converted from various lignin derivatives through the HDO reaction, demonstrating that Ni-1/beta-Mo2C has remarkable potential for the production biofuels through catalytic hydrodeoxygenation of lignin derivatives. The reaction mechanism of DHE over single-atom catalyst Ni-1/beta-Mo2C was confirmed based on comprehensive characterizations of catalysts and DFT calculations. Interestingly, the Ni single-atom active sites alter the reaction pathway by shifting the geometry of the adsorbed intermediate from a vertical to horizontal conformation, which lowered the reaction energy barrier and improved the selectivity to biofuel molecules, resulting in extraordinary catalytic activity. This study suggests an avenue for single-atom catalysis in chemical transformations of lignin derivatives into biofuels.
Keyword :
biomass biomass carbide carbide catalysis catalysis hydrodeoxygenation hydrodeoxygenation single-atom catalyst single-atom catalyst
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GB/T 7714 | Guo, Haoquan , Zhao, Jiwu , Chen, Yu et al. Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C [J]. | ACS CATALYSIS , 2024 , 14 (2) : 703-717 . |
MLA | Guo, Haoquan et al. "Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C" . | ACS CATALYSIS 14 . 2 (2024) : 703-717 . |
APA | Guo, Haoquan , Zhao, Jiwu , Chen, Yu , Lu, Xinyu , Yang, Yue , Ding, Chenrong et al. Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C . | ACS CATALYSIS , 2024 , 14 (2) , 703-717 . |
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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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Introducing a new metal into the metal center of metal-organic framework materials (MOFs) to alter their original electron transfer pathway to improve photocatalytic performance is a promising approach at present. Here, we report a one-pot method to introduce Ni2+ into the metal-centered Zr-O clusters of UiO-66-NH2 (UN) to create a series of Ni2+-doped bimetallic materials (xNi-UN). Experimental results showed that the 0.5Ni-UN exhibited the highest photocatalytic CO2 reduction activity, with a CO yield of 9.01 mu mol g-1h-1 under visible light irradiation, which was 2.46 times higher than that of UN (3.67 mu mol g-1h-1). Through a number of characterization analyses, we find that the doped Ni2+ replaced the part of original metal center Zr4+ to form a bimetallic UiO-66-NH2 (Zr/Ni), which changed the energy band gap of UiO-66-NH2 and improved the charge transfer. More importantly, the introduction of Ni2+ enhanced the efficiency of interfacial charge transfer from the organic ligand (2-aminoterephthalic acid) to the Zr-O cluster, enabling a metal-to-metal charge transfer (MMCT) pathway, which exhibited higher photocatalytic CO2 to CO reduction activity.
Keyword :
Charge transfer Charge transfer CO 2 reduction CO 2 reduction Photocatalysis Photocatalysis UiO-66-NH2 UiO-66-NH2
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GB/T 7714 | Zhu, Pengfei , Cao, Heyang , Yang, Hua et al. One-pot synthesis of Ni(II)-doped UiO-66-NH2 for enhanced photocatalytic CO2 reduction to CO with efficient charge transfer [J]. | APPLIED SURFACE SCIENCE , 2024 , 652 . |
MLA | Zhu, Pengfei et al. "One-pot synthesis of Ni(II)-doped UiO-66-NH2 for enhanced photocatalytic CO2 reduction to CO with efficient charge transfer" . | APPLIED SURFACE SCIENCE 652 (2024) . |
APA | Zhu, Pengfei , Cao, Heyang , Yang, Hua , Geng, Mengrong , Qin, Shuang , Tan, Li et al. One-pot synthesis of Ni(II)-doped UiO-66-NH2 for enhanced photocatalytic CO2 reduction to CO with efficient charge transfer . | APPLIED SURFACE SCIENCE , 2024 , 652 . |
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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 μmolCO2 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. © 2024
Keyword :
CO2 hydrogenation CO2 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, Y. , Cheng, Q. , Xiong, S. et al. Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides [J]. | International Journal of Hydrogen Energy , 2024 . |
MLA | Liu, Y. et al. "Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides" . | International Journal of Hydrogen Energy (2024) . |
APA | Liu, Y. , Cheng, Q. , Xiong, S. , Zhang, Y. , Tan, L. , Song, S. et al. Enhancing CO2 hydrogenation performance via the synergistic effects of iron carbides and iron oxides . | International Journal of Hydrogen Energy , 2024 . |
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The PtIn nanoalloys with high surface energy are generally in a metastable state during harsh reaction conditions, and the ordered alloy structure is not conducive to exposure of surface Pt active sites. Herein, a strategy for restructuring the unfavorable PtIn alloy structure via heteroatom (Ce) doping is applied to advance an isolated Pt delta+ confined by the InCeOx nanoislands supported on SiO2. The as-synthesized catalyst with optimizing PtIn(Ce) ternary components exhibits similar to 92.2% selectivity toward propylene and a stable propane conversion of similar to 67.1% at 550 degrees C (k(d) of 0.010 h(-1)). As demonstrated by the comprehensive characterizations, the introduced proper amount of Ce species leads to the reorganization of the disadvantaged PtIn nanoalloy structure into the robustness of the isolated Pt delta+ site confined by the InCeOx nanoislands via inhibiting the In-0 species generation. The introduced Ce species modulate the electronic interaction between Pt, In, and carrier, stimulating the capability to activate reactive molecules and at the same time acting as spatial physical barriers to restrict the migration of the isolated Pt delta+ species. This work proposed a facile and efficient strategy to promote the capability against sintering and coking of the Pt-based catalyst in propane dehydrogenation.
Keyword :
confinementeffect confinementeffect heteroatom doping heteroatom doping InCeO x nanoislands InCeO x nanoislands isolated Pt sites isolated Pt sites propane dehydrogenation propane dehydrogenation PtIn alloy PtIn alloy
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GB/T 7714 | Wang, Peng , Liao, Huafei , Chen, Yang et al. Enhanced PtIn Catalyst via Ce-Assisted Confinement Effect in Propane Dehydrogenation [J]. | ACS CATALYSIS , 2024 , 14 (11) : 8116-8129 . |
MLA | Wang, Peng et al. "Enhanced PtIn Catalyst via Ce-Assisted Confinement Effect in Propane Dehydrogenation" . | ACS CATALYSIS 14 . 11 (2024) : 8116-8129 . |
APA | Wang, Peng , Liao, Huafei , Chen, Yang , Tao, Xiaoxia , Gan, Yuyan , Deng, Huihui et al. Enhanced PtIn Catalyst via Ce-Assisted Confinement Effect in Propane Dehydrogenation . | ACS CATALYSIS , 2024 , 14 (11) , 8116-8129 . |
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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 high activity of ethyl acetate (EA) combustion is studied over the CuO/CeO2 catalysts which are prepared by the ball milling method, and the relationships between catalytic activity and active sites of CuO and Cu-O-Ce structure are investigated. The finely dispersed CuO particles (around 1.0 nm) and Cu-O-Ce structure are prepared in the CuO/CeO2 catalysts when 5 wt% Cu loading is acquired with the calcination temperature at 500 degrees C. Complete conversion of ethyl acetate to CO2 is achieved at 210 degrees C. Via controlling calcination temperatures and treatments by alkaline/acid, it is demonstrated that the synergistic effect between highly dispersed CuO and Cu-O-Ce structure results in a better ability of oxygen activation and catalytic activity for the 5-CuO/CeO2(500) catalyst. This study provides a feasible strategy for designing an efficient CuO/CeO2 catalyst and an insight into the structure-activity relationship.
Keyword :
Catalytic oxidation Catalytic oxidation Cu-O-Ce Cu-O-Ce Ethyl acetate Ethyl acetate Highly dispersed CuO Highly dispersed CuO Synergistic effect Synergistic effect
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GB/T 7714 | Ye, Yuchuan , Wang, Qing , Chen, Han et al. Investigation on synergistic effect of CuO and Cu-O-Ce on efficient oxidation of ethyl acetate over CuO/CeO2 catalysts [J]. | RESEARCH ON CHEMICAL INTERMEDIATES , 2024 , 50 (7) : 3351-3368 . |
MLA | Ye, Yuchuan et al. "Investigation on synergistic effect of CuO and Cu-O-Ce on efficient oxidation of ethyl acetate over CuO/CeO2 catalysts" . | RESEARCH ON CHEMICAL INTERMEDIATES 50 . 7 (2024) : 3351-3368 . |
APA | Ye, Yuchuan , Wang, Qing , Chen, Han , Chen, Liqiao , Wang, Luhui , Mo, Liuye et al. Investigation on synergistic effect of CuO and Cu-O-Ce on efficient oxidation of ethyl acetate over CuO/CeO2 catalysts . | RESEARCH ON CHEMICAL INTERMEDIATES , 2024 , 50 (7) , 3351-3368 . |
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Catalyst interface determines the activity and stability of partial oxidation of methane (POM) toward syngas under high temperatures crucially. Herein, Ni catalysts supported on CeO 2 were prepared under different pretreatment atmospheres to construct an optimal and robust interface. Ni/CeO 2 catalyst pretreated in H 2 (Ni/CeO 2 - H 2 ) exhibits the higher activity and the better stability than Ni/CeO 2 -Ar and Ni/CeO 2 -air catalysts. The Ni -O -Ce interfacial site in Ni/CeO 2 -H 2 catalyst shows the lower reduction temperature, indicating the enhanced Hspillover effect and enhanced oxidation resistance of Ni under POM conditions. Moreover, the XPS and in situ Raman results show that Ni/CeO 2 -H 2 contains more surface oxygen vacancies for adsorbing and activating oxygen, further contributing to the reaction activity. The in situ DRIFTS results indicate that the CH 4 could react with the lattice oxygen to form formate and carbonate, and further decompose to CO and CO 2 . These findings deepen the fundamental understanding of Ni/CeO 2 catalysts for POM reaction.
Keyword :
Ceria Ceria DRIFTS DRIFTS In-situ Raman In-situ Raman Interface Interface Metal support interaction Metal support interaction Methane reforming Methane reforming Nickel Nickel Oxygen vacancy Oxygen vacancy Partial oxidation of methane Partial oxidation of methane Pretreatment Pretreatment Syngas Syngas
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GB/T 7714 | Xu, Yuanjie , Chen, Rong , Lin, Hongqiao et al. Constructing the Ni-O-Ce interface to enhance the activity and stability for partial oxidation of methane to syngas under high temperatures [J]. | JOURNAL OF CATALYSIS , 2024 , 435 . |
MLA | Xu, Yuanjie et al. "Constructing the Ni-O-Ce interface to enhance the activity and stability for partial oxidation of methane to syngas under high temperatures" . | JOURNAL OF CATALYSIS 435 (2024) . |
APA | Xu, Yuanjie , Chen, Rong , Lin, Hongqiao , Lv, Qian , Liu, Bo , Wu, Lizhi et al. Constructing the Ni-O-Ce interface to enhance the activity and stability for partial oxidation of methane to syngas under high temperatures . | JOURNAL OF CATALYSIS , 2024 , 435 . |
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