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学者姓名：吴立志
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Abstract ：
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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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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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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The surface properties of heterogeneous catalysts regulated by the modified support are considered to be the key factors in determining catalytic performance. In propane dehydrogenation, PtZn catalysts have poor catalytic life due to the structural instability of Zn species although it owns high intrinsic activity. Herein, the dealuminated Beta zeolite is harnessed for chemically confining the introduced Zn species, the formed functional ZnOx (0 < x < 2) islands are further responsible for anchoring Pt1Zn1 alloys. According to the comprehensive characterization, the modifying surface defects on the Beta support can provide benign metal-support interaction and modulate the electronic structure of supported metal species. Hence, the Pt/ZnOx-SiBeta catalyst embodies 59.5 % propane conversion with a high propylene selectivity of 99.2 % and no obvious deactivation undergoing 100 h of dehydrogenation reaction. The optimal electronic interaction exists between ZnOx and SiBeta, which inhibits the aggregation of Pt sites and the coking formation.
Keyword ：
Beta Zeolite Beta Zeolite Confinement effect Confinement effect Dealumination Dealumination Propane dehydrogenation Propane dehydrogenation Propylene Propylene
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| GB/T 7714 | Liao, Huafei , Tao, Xiaoxia , Wu, Lizhi et al. Anchoring Pt sites via chemical confining functional ZnOx islands in propane dehydrogenation [J]. | FUEL , 2024 , 369 . |
| MLA | Liao, Huafei et al. "Anchoring Pt sites via chemical confining functional ZnOx islands in propane dehydrogenation" . | FUEL 369 (2024) . |
| APA | Liao, Huafei , Tao, Xiaoxia , Wu, Lizhi , Tang, Yu , Wang, Peng , Tan, Li . Anchoring Pt sites via chemical confining functional ZnOx islands in propane dehydrogenation . | FUEL , 2024 , 369 . |
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Selective hydrodeoxygenation of biomass and its derivatives to produce chemicals and biofuels is an effective upgrading strategy to achieve global sustainable development goals. Through the development and utilization of renewable resources, sustainable consumption and production patterns can be promoted and climate change and its impacts can be addressed. Herein, selective hydrodeoxygenation (HDO) of vanillin was conducted by utilizing a Pd/α-MoC catalyst modified with solvent water. The water modification induced the formation of a thin layer of molybdenum oxide on the Pd/α-MoC catalyst surface, which significantly promotes the selective hydrodeoxygenation of vanillin. The conversion of vanillin over the modified Pd/α-MoC catalyst reached 99.9 %, while the selectivity to 4-methyl-2-methoxyphenol (MMP) reached 99.9 % at 0.3 MPa H2 and 80 °C. Comprehensive characterizations elucidate that the heterogeneous layer on the surface of the modified catalyst significantly increases the acidity of the catalyst and improves the removal efficiency of hydroxyl groups, thus improving the high selectivity to the desired product. Moreover, the side reactions are inhibited due to the using of water as the solvent, which contributes a high carbon balance. The modified Pd/α-MoC catalyst exhibits efficient hydrodeoxygenation of vanillin under mild conditions, which suggests an avenue for chemical transformations of biomass derivatives into high value chemicals. © 2024 Elsevier B.V.
Keyword ：
Biomass Biomass Carbides Carbides Catalyst selectivity Catalyst selectivity Climate change Climate change Indicators (chemical) Indicators (chemical) Molybdenum oxide Molybdenum oxide Water treatment Water treatment
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| GB/T 7714 | Guo, Haoquan , Chen, Yu , Yang, Junye et al. Water treatment induced formation of surface oxide layers of Pd/α-MoC catalyst to enhance the selective hydrodeoxygenation of vanillin [J]. | Chemical Engineering Journal , 2024 , 493 . |
| MLA | Guo, Haoquan et al. "Water treatment induced formation of surface oxide layers of Pd/α-MoC catalyst to enhance the selective hydrodeoxygenation of vanillin" . | Chemical Engineering Journal 493 (2024) . |
| APA | Guo, Haoquan , Chen, Yu , Yang, Junye , Wu, Lizhi , Tan, Li , Yang, Guohui et al. Water treatment induced formation of surface oxide layers of Pd/α-MoC catalyst to enhance the selective hydrodeoxygenation of vanillin . | Chemical Engineering Journal , 2024 , 493 . |
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Enhancing catalyst durability is a critical concern in the partial oxidation of methane (POM) to syngas since the reaction is operated at high temperatures (>600 °C). Alongside sintering and coke deposition, the deactivation of the supported Ni catalyst is often due to the in situ oxidation of active metallic nanoparticles into inactive cations during the POM reaction. Herein, a Ni/BN catalyst was developed by introducing functional CeOx as a promoter to stabilize the Ni sites. The optimized 4Ni/7.5Ce/BN catalyst, comprising 4 wt % Ni and 7.5 wt % Ce on BN, exhibits enhanced stability during continuous testing at 600 °C for 125 h without any deactivation, which is comparable to that of noble metal catalysts. Comprehensive investigations reveal that maintaining the metallic state of Ni under reaction atmosphere is crucial for the stability of the catalyst. The construction of CeOx on BN effectively inhibits migration and oxidation of the catalytically active Ni0 species. © 2024 American Chemical Society.
Keyword ：
boron nitride boron nitride catalyst deactivation catalyst deactivation ceria ceria methane reforming methane reforming nickel nickel partial oxidation of methane partial oxidation of methane strong metal support interaction strong metal support interaction syngas syngas
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| GB/T 7714 | Xu, Y. , Yao, J. , Lin, H. et al. Functional CeOx Stabilized Metallic Ni Catalyst Supported on Boron Nitride for Durable Partial Oxidation of Methane to Syngas at High Temperature [J]. | ACS Catalysis , 2024 , 14 (15) : 11845-11856 . |
| MLA | Xu, Y. et al. "Functional CeOx Stabilized Metallic Ni Catalyst Supported on Boron Nitride for Durable Partial Oxidation of Methane to Syngas at High Temperature" . | ACS Catalysis 14 . 15 (2024) : 11845-11856 . |
| APA | Xu, Y. , Yao, J. , Lin, H. , Lv, Q. , Liu, B. , Wu, L. et al. Functional CeOx Stabilized Metallic Ni Catalyst Supported on Boron Nitride for Durable Partial Oxidation of Methane to Syngas at High Temperature . | ACS Catalysis , 2024 , 14 (15) , 11845-11856 . |
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The catalytic conversion of methane into value-added products under mild reaction conditions presents a key challenge in heterogeneous catalysis. In this study, we investigate the conversion of methane to acetic acid (CH3COOH) and other methyl oxygenates by using molecule CO as the promoter on Ir/ZSM-5 catalyst. An optimum space–time yield of 7.4 mmol·gcat−1·h−1 to acetic acid was achieved under mild conditions (2.5 MPa CH4, 2.5 MPa CO, 80 °C). The influence of CO on methane conversion was investigated across various transition metals. Ir, Fe, Rh, and Pd showed promotion towards oxygenated compound formation, while Cu and Cr exhibited inhibition. Sequential charging of CH4 and CO experiments reveal the critical role of CO in acetic acid production. Furthermore, the role of CO was further investigated by in situ Raman, in-situ FTIR and EPR. This work shows the role of CO in mild conversion of CH4 to CH3COOH on Ir catalyst. © 2024 Elsevier Inc.
Keyword ：
Acetic acid Acetic acid Carbon monoxide Carbon monoxide C–H bond C–H bond Iridium Iridium Methane Methane Zeolite Zeolite
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| GB/T 7714 | Liu, B. , Xiang, C. , Yang, J. et al. The promoting role of carbon monoxide in mild conversion of methane to acetic acid on atomically dispersed Ir catalyst anchored in ZSM-5 [J]. | Journal of Catalysis , 2024 , 438 . |
| MLA | Liu, B. et al. "The promoting role of carbon monoxide in mild conversion of methane to acetic acid on atomically dispersed Ir catalyst anchored in ZSM-5" . | Journal of Catalysis 438 (2024) . |
| APA | Liu, B. , Xiang, C. , Yang, J. , Sun, P. , Yang, Y. , Xu, Y. et al. The promoting role of carbon monoxide in mild conversion of methane to acetic acid on atomically dispersed Ir catalyst anchored in ZSM-5 . | Journal of Catalysis , 2024 , 438 . |
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The optimizing utilization of carbon resources has drawn wide attention all over the world, while exploiting the high-efficiency catalytic routes remains a challenge. Here, a direct methanol synthesis route is realized from pure CO and H2O over 10%Cu/t-ZrO2 catalyst, where the time yield of methanol is 144.43 mmol molCu1 h-1 and the methanol selectivity in hydrocarbons is 100%. The Cu species highly dispersed in the t-ZrO2 support lead parts of them in the cationic state. The Cu+ sites contribute to the dissociation of H2O, providing the H* source for methanol synthesis, while the formed Cu0 sites promote the absorption and transfer of H* during the reaction. Moreover, the H2O is even a better H resource than H2 due to its better dissociation effectivity in this catalytic system. The present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor. (c) 2024 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
Keyword ：
CO CO Cu-based catalysts Cu-based catalysts H 2 O H 2 O Methanol Methanol t-ZrO2 t-ZrO2
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| GB/T 7714 | Fang, Yuan , Wang, Fan , Chen, Yang et al. Realizing methanol synthesis from CO and water via the synergistic effect of Cu0/Cu+ over Cu/ZrO2 catalyst [J]. | JOURNAL OF ENERGY CHEMISTRY , 2024 , 93 : 126-134 . |
| MLA | Fang, Yuan et al. "Realizing methanol synthesis from CO and water via the synergistic effect of Cu0/Cu+ over Cu/ZrO2 catalyst" . | JOURNAL OF ENERGY CHEMISTRY 93 (2024) : 126-134 . |
| APA | Fang, Yuan , Wang, Fan , Chen, Yang , Lv, Qian , Jiang, Kun , Yang, Hua et al. Realizing methanol synthesis from CO and water via the synergistic effect of Cu0/Cu+ over Cu/ZrO2 catalyst . | JOURNAL OF ENERGY CHEMISTRY , 2024 , 93 , 126-134 . |
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