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学者姓名：吴立志
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Abstract ：
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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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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Abstract ：
Mo/HMCM-22 is one of the candidate catalysts for methane dehydroaromatization (MDA) reaction. However, serious coke deposition would deactivate the catalyst, resulting in a rapid decrease of aromatics yield. Here, we adjusted the acidity of MCM-22 zeolite by doping boron into the framework. Boron species replace some of framework aluminum and prompt aluminum to locate in sinusoidal channel. It optimizes the ratio of strong/weak Brønsted acid, as well as enhances the interaction between molybdenum and HMCM-22 to facilitate the dispersion of molybdenum species. After 10 h of MDA reaction, the yield of aromatics over Mo/H[B]MCM-22 (SBR 30) is 3.5 times higher than that of Mo/H[B]MCM-22 (SBR 5). It decreases by only 4.8 % in comparison to the initial yield. Meanwhile, Mo/H[B]MCM-22 (SBR 30) shows significantly better resistance to coke deposition. Therefore, the established structure–activity relationships provide valuable insights for future research on the modification of zeolite acidity in methane dehydroaromatization reaction. © 2024 Elsevier Ltd
Keyword ：
Aluminum Aluminum Boron Boron Catalysts Catalysts Coke Coke Deposition Deposition Methane Methane Molybdenum Molybdenum Zeolites Zeolites
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| GB/T 7714 | Gan, Yuyan , Xu, Yunzhao , Zhang, Peipei et al. Boron doped Mo/HMCM-22 catalyst for improving coke resistance in methane dehydroaromatization [J]. | Chemical Engineering Science , 2024 , 299 . |
| MLA | Gan, Yuyan et al. "Boron doped Mo/HMCM-22 catalyst for improving coke resistance in methane dehydroaromatization" . | Chemical Engineering Science 299 (2024) . |
| APA | Gan, Yuyan , Xu, Yunzhao , Zhang, Peipei , Wang, Weihao , Liu, Weiling , Li, Ruoyu et al. Boron doped Mo/HMCM-22 catalyst for improving coke resistance in methane dehydroaromatization . | Chemical Engineering Science , 2024 , 299 . |
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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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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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Abstract ：
Mo/HMCM-22 is one of the candidate catalysts for methane dehydroaromatization (MDA) reaction. However, serious coke deposition would deactivate the catalyst, resulting in a rapid decrease of aromatics yield. Here, we adjusted the acidity of MCM-22 zeolite by doping boron into the framework. Boron species replace some of framework aluminum and prompt aluminum to locate in sinusoidal channel. It optimizes the ratio of strong/ weak Br & oslash;nsted acid, as well as enhances the interaction between molybdenum and HMCM-22 to facilitate the dispersion of molybdenum species. After 10 h of MDA reaction, the yield of aromatics over Mo/H[B]MCM-22 (SBR 30) is 3.5 times higher than that of Mo/H[B]MCM-22 (SBR 5). It decreases by only 4.8 % in comparison to the initial yield. Meanwhile, Mo/H[B]MCM-22 (SBR 30) shows significantly better resistance to coke deposition. Therefore, the established structure-activity relationships provide valuable insights for future research on the modification of zeolite acidity in methane dehydroaromatization reaction.
Keyword ：
Boron doping Boron doping Br & oslash;nsted acid Br & oslash;nsted acid MCM-22 zeolite MCM-22 zeolite Methane dehydroaromatization Methane dehydroaromatization Mo-based catalyst Mo-based catalyst
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| GB/T 7714 | Gan, Yuyan , Xu, Yunzhao , Zhang, Peipei et al. Boron doped Mo/HMCM-22 catalyst for improving coke resistance in methane dehydroaromatization [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 299 . |
| MLA | Gan, Yuyan et al. "Boron doped Mo/HMCM-22 catalyst for improving coke resistance in methane dehydroaromatization" . | CHEMICAL ENGINEERING SCIENCE 299 (2024) . |
| APA | Gan, Yuyan , Xu, Yunzhao , Zhang, Peipei , Wang, Weihao , Liu, Weiling , Li, Ruoyu et al. Boron doped Mo/HMCM-22 catalyst for improving coke resistance in methane dehydroaromatization . | CHEMICAL ENGINEERING SCIENCE , 2024 , 299 . |
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Cyclohexanone is a key raw material for manufacturing nylon and other chemicals. The sustainable conversion of biomass-derived phenol to cyclohexanone meets the requirements of sustainable development goal but still be challenging. Herein, a catalyst containing isolated Pd cations in zeolite, namely Pd1/ZSM-5, is investigated for the partial hydrogenation of phenol to cyclohexanone. Under 140 degrees C and 1.5 MPa of initial hydrogen pressure, the conversion of phenol reaches 95.6% with the selectivity to cyclohexanone of 99.9%. Besides, the turnover rate (TOR) of partial hydrogenation of phenol reaches 382.7 h- 1. The mild adsorption affinity of cyclohexanone on catalytic sites leads to the high selectivity. Moreover, as unveiled by surface reactivity of phenol monitored by in-situ infrared spectrum, the oxygen atom of phenol hydroxyl group is adsorbed on the Bronsted acid site of Pd1/ ZSM-5 as the key reaction step. The reaction intermediate involves the partial hydrogenation of benzene ring of phenol.
Keyword ：
Cyclohexanone Cyclohexanone Hydrogenation Hydrogenation Palladium Palladium Phenol Phenol Single atom catalyst Single atom catalyst Zeolite Zeolite
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| GB/T 7714 | Xu, Kaiyang , Weng, Lingfeng , Wu, Lizhi et al. Hydrogenation of phenol to cyclohexanone catalyzed by isolated Pd cations in the micropores of zeolite [J]. | APPLIED CATALYSIS O: OPEN , 2024 , 193 . |
| MLA | Xu, Kaiyang et al. "Hydrogenation of phenol to cyclohexanone catalyzed by isolated Pd cations in the micropores of zeolite" . | APPLIED CATALYSIS O: OPEN 193 (2024) . |
| APA | Xu, Kaiyang , Weng, Lingfeng , Wu, Lizhi , Tan, Li , Tang, Yu . Hydrogenation of phenol to cyclohexanone catalyzed by isolated Pd cations in the micropores of zeolite . | APPLIED CATALYSIS O: OPEN , 2024 , 193 . |
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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/alpha-MoC catalyst modified with solvent water. The water modification induced the formation of a thin layer of molybdenum oxide on the Pd/alpha-MoC catalyst surface, which significantly promotes the selective hydrodeoxygenation of vanillin. The conversion of vanillin over the modified Pd/alpha-MoC catalyst reached 99.9 %, while the selectivity to 4-methyl-2-methoxyphenol (MMP) reached 99.9 % at 0.3 MPa H2 and 80 degrees 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/alpha-MoC catalyst exhibits efficient hydrodeoxygenation of vanillin under mild conditions, which suggests an avenue for chemical transformations of biomass derivatives into high value chemicals.
Keyword ：
Biomass Biomass Carbide Carbide Hydrodeoxygenation Hydrodeoxygenation Restructuring Restructuring Vanillin Vanillin 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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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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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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