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学者姓名：汤禹
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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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Capture of acid gases holds crucial importance for addressing air pollution and climate change, where achieving a molar ratio for adsorption and separation of acid gases on an active site higher than 1.0 remains challenging. Herein, we demonstrate that three nitrogen-bonded one Zn sites within a single-crystalline-like porous carbon (Zn-N3@SC-PC) derived from controlled carbonization of ZIF-8-C equivalent to N with KCl, exhibit supra-multi-molar adsorption for CO2, COS, and H2S, even to 1:6 ratio for SO2 on the Zn-N3. This exceptional performance is attributed to the protruded structure in the Zn-N3@SC-PC for more coordination between Zn vacant orbital and acid gases evidenced by DFT calculation and in situ EXAFS. The high capacity for capturing acid gases on this adsorbent is crucial for future in carbon neutrality and environment protection.
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| GB/T 7714 | Zhang, Guanqing , Liu, Fengqing , Zhong, Shouchao et al. Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
| MLA | Zhang, Guanqing et al. "Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases" . | NATURE COMMUNICATIONS 16 . 1 (2025) . |
| APA | Zhang, Guanqing , Liu, Fengqing , Zhong, Shouchao , Liu, Fujian , Zhu, Qiliang , Tang, Yu et al. Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases . | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
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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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X-ray photoelectron spectroscopy (XPS) is a crucial surface analysis technique that has become a key tool in the study of heterogeneous catalysis. Detecting surface chemistry under conditions that closely mimic actual industrial catalytic processes is essential for understanding the mechanisms involved. In the past decade, near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) has been increasingly utilized to study the surface chemistry of catalysts during heterogeneous catalytic processes, offering insights into structure-performance correlations. This review begins with a brief overview of NAP-XPS instrumentation. Next, we discuss the application of NAP-XPS in the study of thermal catalysis reactions, followed by a summary of the research on catalyst restructuring under reaction conditions. Additionally, we address the challenges and future perspectives for the development and application of NAP-XPS. Catalysis is inherently dynamic, requiring an understanding of the real-time behavior of catalysts under varying conditions. Therefore, future improvements in the ability to probe reaction intermediates with higher spatial and temporal resolution under conditions that closely mimic industrial environments are needed.
Keyword ：
catalysis catalysis in situ/operando spectroscopy in situ/operando spectroscopy near ambient pressure XPS near ambient pressure XPS restructuring restructuring surface chemistry surface chemistry
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| GB/T 7714 | Xu, Yuanjie , An, Zemin , Tang, Yu . Recent progress in exploring heterogeneous catalyst surface chemistry with near ambient pressure XPS [J]. | SCIENCE CHINA-CHEMISTRY , 2025 . |
| MLA | Xu, Yuanjie et al. "Recent progress in exploring heterogeneous catalyst surface chemistry with near ambient pressure XPS" . | SCIENCE CHINA-CHEMISTRY (2025) . |
| APA | Xu, Yuanjie , An, Zemin , Tang, Yu . Recent progress in exploring heterogeneous catalyst surface chemistry with near ambient pressure XPS . | SCIENCE CHINA-CHEMISTRY , 2025 . |
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Using environmental scanning transmission electron microscopy and a global optimization algorithm, we unraveled the preoxidation dispersion and direct dispersion mechanisms in Pd-CeO2(100) systems, mediated by the behaviors of highly dispersed Pd species. At lower temperatures, Pd nanoparticles first undergo oxidation, followed by the dispersion of PdO nanoparticles. In contrast, at higher temperatures, Pd nanoparticles directly convert into highly distributed cationic Pd species. These distinct dispersion mechanisms are driven by the thermodynamic and kinetic differences of environment-dependent Pd1-2O and Pd1-4O species, providing a fundamental basis for precisely controlling catalyst dispersion states. © 2025 American Physical Society.
Keyword ：
Nanoparticles Nanoparticles
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| GB/T 7714 | Zou, Chen , Liu, Wen , Chen, Shiyuan et al. Two Distinct Oxidation Dispersion Mechanisms in Pd-CeO2 Mediated by Thermodynamic and Kinetic Behaviors of Highly Dispersed Pd Species [J]. | Physical Review Letters , 2025 , 134 (21) . |
| MLA | Zou, Chen et al. "Two Distinct Oxidation Dispersion Mechanisms in Pd-CeO2 Mediated by Thermodynamic and Kinetic Behaviors of Highly Dispersed Pd Species" . | Physical Review Letters 134 . 21 (2025) . |
| APA | Zou, Chen , Liu, Wen , Chen, Shiyuan , Xu, Yuanjie , Tang, Yu , Li, Songda et al. Two Distinct Oxidation Dispersion Mechanisms in Pd-CeO2 Mediated by Thermodynamic and Kinetic Behaviors of Highly Dispersed Pd Species . | Physical Review Letters , 2025 , 134 (21) . |
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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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Developing active, stable, and cost-efficient electrocatalysts to replace platinum for the alkaline hydrogen evolution reaction (HER) is highly desirable yet represents a great challenge. Here, it is reported on a facile one-pot synthesis of RuxNi layered double hydroxides (RuxNi-LDHs) that exhibit remarkable HER activity and stability after an in-situ activation treatment, surpassing most state-of-the-art Ru-based catalysts as well as commercial Ru/C and Pt/C catalysts. The structural and chemical changes triggered by in-situ activation are systematically investigated, and the results clearly show that the pristine, less-active RuxNi-LDHs are transformed into a highly active catalyst characterized by raft-like, defect-rich Ru degrees particles decorated on the surface of RuxNi-LDHs. Density functional theory (DFT) calculations reveal that the defective Ru sites can effectively optimize the reaction pathway and lower the free energies of the elemental steps involved, leading to enhanced intrinsic activity. This work highlights the importance of the currently understudied strategy of defect engineering in boosting the HER activity of Ru-based catalysts and offers an effective approach involving in-situ electrochemical activation for the development of high-performance alkaline HER catalysts.
Keyword ：
alkaline HER alkaline HER defect engineering defect engineering defective Ru-degrees NPs defective Ru-degrees NPs first-principles calculations first-principles calculations RuxNi-LDHs RuxNi-LDHs
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| GB/T 7714 | Shi, Ningning , Ma, Ruijie , Lin, Linghui et al. In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution [J]. | SMALL , 2024 , 20 (27) . |
| MLA | Shi, Ningning et al. "In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution" . | SMALL 20 . 27 (2024) . |
| APA | Shi, Ningning , Ma, Ruijie , Lin, Linghui , Xie, Wangjing , Liu, Panpan , Li, Peng et al. In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution . | SMALL , 2024 , 20 (27) . |
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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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Developing highly effective catalysts for ammonia (NH3) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C-60) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The 'electron buffer' behaviour of C-60 balances the electron density at catalytic transition metal sites and enables the synergistic activation of nitrogen on transition metals in addition to the activation and migration of hydrogen on C-60 sites. As demonstrated in long-term, continuous runs, the C-60-promoting transition metal co-catalysts exhibit higher NH3 synthesis rates than catalysts without C-60. With the involvement of C-60, the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH2. C-60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.
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| GB/T 7714 | Zhang, Yangyu , Peng, Xuanbei , Tian, Han-Rui et al. Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis [J]. | NATURE CHEMISTRY , 2024 , 16 (11) . |
| MLA | Zhang, Yangyu et al. "Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis" . | NATURE CHEMISTRY 16 . 11 (2024) . |
| APA | Zhang, Yangyu , Peng, Xuanbei , Tian, Han-Rui , Yang, Bo , Chen, Zuo-Chang , Li, Jiejie et al. Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis . | NATURE CHEMISTRY , 2024 , 16 (11) . |
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