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学者姓名:吴立志
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Cyclopentanone (CPO) is a high-value platform chemical widely used in fuel, fragrances, and polymers, yet its sustainable production from biomass remains challenging. This work addresses this gap by developing efficient Ni/TiO2 catalysts through crystal phase engineering of TiO2 supports (anatase, rutile, mixed-phase P25) for aqueous-phase hydrogenative ring-rearrangement of furfural (FAL) to CPO. Crucially, the TiO2 phase dictates the Ni-O-Ti interface structure, governing nickel speciation and reactivity. Ni supported on mixed-phase P25 achieves exceptional performance under industrially relevant conditions: 91.1% FAL conversion, 89.3% CPO selectivity, and specific rate of 71.6 h(-1), surpassing catalysts on pure anatase (9.1% conversion) or rutile (55.8% conversion). Physical mixture experiments confirm this superiority stems from the intrinsic interface of P25, not component blending. Characterization reveals that P25 stabilizes a multifunctional surface ensemble: metallic Ni-0 (18.0% by XPS) enables hydrogenation, while cationic Ni2+ facilitates acid-catalyzed dehydration and ring rearrangement. Simultaneously, sufficient metal-support interaction permits in situ regeneration of active sites. The optimized 1Ni/P25 demonstrates robust stability over five cycles with retained selectivity (>90%), showcasing practical durability. This study provides a scalable design strategy-support crystal phase tuning-to engineer cost-effective, multifunctional catalysts for industrial biomass upgrading, advancing green manufacturing of cyclic ketones without precious metals.
Keyword :
Cyclopentanone Cyclopentanone Furfural Furfural Metal-support interaction Metal-support interaction Ni-O-Ti interface Ni-O-Ti interface TiO2 crystal phase TiO2 crystal phase
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GB/T 7714 | Tang, Yu , Xu, Kaiyang , Weng, Lingfeng et al. Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural [J]. | CHEMCATCHEM , 2025 . |
MLA | Tang, Yu et al. "Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural" . | CHEMCATCHEM (2025) . |
APA | Tang, Yu , Xu, Kaiyang , Weng, Lingfeng , Xu, Yuanjie , Tan, Li , Wu, Lizhi . Crystal Phase of TiO2 Determines Ni-O-Ti Interface and Enables Nickel Catalysts in Aqueous-Phase Cyclopentanone Synthesis from Furfural . | CHEMCATCHEM , 2025 . |
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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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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 utilization of Rh-based catalysts in the direct production of ethanol from CO2 has been a subject of significant interest. However, to date, the precise active sites responsible for ethanol generation and the C-C coupling mechanism remain elusive. In this study, we present a Rh-based catalyst featuring nanoscale Rh-Fe alloy sites, which achieved an ethanol selectivity of 49.1% among all hydrocarbon and oxygenate products (CO excluded) under relatively mild reaction conditions (3.0 MPa, 200 degrees C, with a low metal loading of <= 1 wt %). The formation of ethanol proceeds via the HCOO* pathway with a CO insertion mechanism occurring at the alloy sites with a specific cluster size, where CH2* and CO* act as the crucial intermediates for C-C coupling. The electron interaction within the Rh-Fe alloy sites effectively reduces the energy barrier for the formation of the CH2CO* intermediate, thereby facilitating the production of ethanol. In contrast to the Rh-Fe alloy sites, the geminal-dicarbonyl binding configuration of CO* intermediates on Rh single sites favors the generation of byproducts such as methane and methanol, rather than ethanol. This research offers insights into the active sites and reaction mechanism of hydrogenation of CO2 to ethanol, thus enhancing the efficient utilization of Rh-based catalysts.
Keyword :
C-C coupling C-C coupling CO2 hydrogenation CO2 hydrogenation ethanol ethanol Rh-Fealloy Rh-Fealloy thermal catalysis thermal catalysis
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GB/T 7714 | Chen, Yang , Zhou, Diwen , Chang, Yongli et al. Rh-Based Bimetallic Alloys: Unraveling the Synergistic Catalysis in CO2 Hydrogenation to Ethanol [J]. | ACS CATALYSIS , 2025 , 15 (12) : 10068-10081 . |
MLA | Chen, Yang et al. "Rh-Based Bimetallic Alloys: Unraveling the Synergistic Catalysis in CO2 Hydrogenation to Ethanol" . | ACS CATALYSIS 15 . 12 (2025) : 10068-10081 . |
APA | Chen, Yang , Zhou, Diwen , Chang, Yongli , Xu, Yunzhao , Lin, Hongqiao , Wu, Lizhi et al. Rh-Based Bimetallic Alloys: Unraveling the Synergistic Catalysis in CO2 Hydrogenation to Ethanol . | ACS CATALYSIS , 2025 , 15 (12) , 10068-10081 . |
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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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Tuning metal-support interactions in catalysts represents a promising strategy for optimizing the catalytic activity of CO2 hydrogenation. Here, CuZnZr ternary catalysts with varied interfacial structures were fabricated by altering the metal loading sequence to elucidate the interactions between different counterparts. Compared to reference catalysts with different interfaces (Cu-ZnZr, Zn-CuZr and Zr-CuZn), CuZnZr synthesized via the coprecipitation method (CZZ) displays the highest catalytic performance, achieving a CO2 conversion rate of 13.3 %, methanol selectivity of 71.3 %, and a STY of 12.2 mmolMeOH center dot gcat-1 center dot h-1 under optimal conditions. Extensive characterization results indicate that this exceptional activity originates from the synergistic optimization of both structure and reaction mechanism, driven by the interface confinement effect (ICE) enabled by abundant interfacial sites. Specifically, the surface of CZZ shows high density of highly dispersed Cu0 nanoparticles and rich oxygen vacancy sites, which is beneficial to the activation of H2 and the adsorption of CO2. In-situ DRIFTS further revealed that, compared to reference catalysts, CO2 hydrogenation on CZZ follows both the HCOO* and COOH* pathways, leading to a substantial improvement in overall catalytic activity. In summary, this study provides a deeper understanding of the ICE and their impacts on catalytic performance, offering a valuable theoretical insight for the design of high-performance catalysts in future research.
Keyword :
CO 2 hydrogenation CO 2 hydrogenation Cu-based catalysts Cu-based catalysts Methanol Methanol Ternary interface Ternary interface
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GB/T 7714 | Chang, Yongli , Liu, Weiling , Chen, Yang et al. Boosting CO2 hydrogenation to methanol via ternary Cu-Zn-Zr catalyst: The critical role of interface confinement effect (ICE) [J]. | MOLECULAR CATALYSIS , 2025 , 584 . |
MLA | Chang, Yongli et al. "Boosting CO2 hydrogenation to methanol via ternary Cu-Zn-Zr catalyst: The critical role of interface confinement effect (ICE)" . | MOLECULAR CATALYSIS 584 (2025) . |
APA | Chang, Yongli , Liu, Weiling , Chen, Yang , Zhang, Yong , Li, Ruoyu , Xu, Xiaoyang et al. Boosting CO2 hydrogenation to methanol via ternary Cu-Zn-Zr catalyst: The critical role of interface confinement effect (ICE) . | MOLECULAR CATALYSIS , 2025 , 584 . |
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As a model compound for lignin derivatives, anisole and its conversion are crucial for the upgrading of biomass resources. Anisole molecule contains a characteristic aryl ether bond (C-aryl-O-CH3); therefore, the selective cleavage of the C-O bond to efficiently produce high-value chemicals poses a significant challenge. Constructing bimetallic synergistic active sites through tuning the metal-support interface is considered an effective strategy. In this work, the WO3-promoted Pt/SiO2 catalysts were investigated to enhance the performance of anisole hydrodeoxygenation (HDO) to hydrocarbons. Experimental results demonstrate that WO3 significantly promotes HDO selectivity, increasing from 37.8% to 86.8% at 250 degrees C. Moreover, moderate doping improves low-temperature (<250 degrees C) HDO activity, confirming the presence of synergistic effects. In contrast, excessive WO3 suppresses anisole conversion. Characterization results reveal that WO3 stabilizes metallic Pt and facilitates H2 dissociation. Concurrently, strong hydrogen spillover between Pt and WO3 promotes oxygen vacancy formation on WO3. This transforms disordered adsorption of anisole on SiO2 into directed adsorption of the anisole's oxygen species onto WO3. This work achieves high anisole HDO selectivity through the Pt-WO3 interface tuning, offering novel insights for efficient lignin conversion.
Keyword :
anisole anisole biomass biomass hydrodeoxygenation hydrodeoxygenation interfacial modulation interfacial modulation metal-support interactions metal-support interactions platinum platinum
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GB/T 7714 | Yan, Wanru , Li, Jiating , Ma, Nan et al. Investigation on Pt-WO3 Catalytic Interface for the Hydrodeoxygenation of Anisole [J]. | CATALYSTS , 2025 , 15 (9) . |
MLA | Yan, Wanru et al. "Investigation on Pt-WO3 Catalytic Interface for the Hydrodeoxygenation of Anisole" . | CATALYSTS 15 . 9 (2025) . |
APA | Yan, Wanru , Li, Jiating , Ma, Nan , An, Zemin , Xu, Yuanjie , Wu, Lizhi et al. Investigation on Pt-WO3 Catalytic Interface for the Hydrodeoxygenation of Anisole . | CATALYSTS , 2025 , 15 (9) . |
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PtSn bimetallic catalysts applied in propane dehydrogenation (PDH) reaction suffer from deactivation at high temperatures (500-700 degrees C) due to metal segregation and Sn-rich cluster formation. This study demonstrates that supporting PtSn catalysts on Silicalite-1 zeolite (S-1) enhances Sn dispersion through interactions with silanol hydroxyl groups, enabling effective regeneration of Pt-rich PtSn clusters even after 15 reaction-regeneration cycles. Comprehensive characterizations reveal that silanol nests play a critical role in redispersing metal species during regeneration, minimizing aggregation, and maintaining catalytic activity. The enhanced metalsupport interactions significantly improve catalyst regenerability and stability, addressing key challenges in industrial PDH processes. This work highlights the importance of Sn dispersion and metal-support interactions in designing durable and efficient PtSn catalysts, offering practical insights for sustainable propylene production.
Keyword :
Catalyst regeneration Catalyst regeneration Propane dehydrogenation Propane dehydrogenation Propylene Propylene PtSn catalyst PtSn catalyst Silanol Silanol
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GB/T 7714 | Chen, Rong , Wang, Peng , Wu, Lizhi et al. Silanol nest-driven redispersion of sintered PtSn clusters in zeolite for regenerable propane dehydrogenation [J]. | MOLECULAR CATALYSIS , 2025 , 583 . |
MLA | Chen, Rong et al. "Silanol nest-driven redispersion of sintered PtSn clusters in zeolite for regenerable propane dehydrogenation" . | MOLECULAR CATALYSIS 583 (2025) . |
APA | Chen, Rong , Wang, Peng , Wu, Lizhi , Tan, Li , Tang, Yu . Silanol nest-driven redispersion of sintered PtSn clusters in zeolite for regenerable propane dehydrogenation . | MOLECULAR CATALYSIS , 2025 , 583 . |
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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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