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学者姓名：吴立志
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Abstract ：
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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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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Abstract ：
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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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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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 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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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 degrees 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 degrees 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 Ni-0 species.
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, Yuanjie , Yao, Jikang , Lin, Hongqiao 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, Yuanjie 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, Yuanjie , Yao, Jikang , Lin, Hongqiao , Lv, Qian , Liu, Bo , Wu, Lizhi 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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