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学者姓名：汤禹
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Abstract ：
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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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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Single-atom catalysts (SACs) enable atomic-level control over active sites, but orbital-level manipulation to steer catalytic behavior remains challenging. Here, we address this issue through d-orbital engineering of Cu SACs, achieving simultaneous control over coordination geometry (Cu-N3) and high metal loading (33.2 wt%) for direct benzene-to-phenol oxidation with H2O2. The tri-coordinated Cu SAC (Cu-N3-33.2) exhibits the highest performance with 85.8% benzene conversion and a turnover frequency of 680.3 h-1 at 60 oC, ranking it among the best metal-based catalysts. In-situ ATR-IR spectroscopy and DFT calculations reveal that dynamically formed Cu-O intermediates, driven by p-d orbital hybridization between Cu (d orbitals) and O (p orbitals), lower the H2O2 activation barrier by 0.98 eV compared to Cu-N4 sites. High-density atomic Cu sites prevent over-oxidation by consuming singlet oxygen (1O2). This work establishes a dual-parameter optimization paradigm, including orbital configuration and site density, redefining design principles for selective oxidation SACs.
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| GB/T 7714 | Li, Shuchun , Cao, Changsheng , Chen, Jiabin et al. Manipulating d-orbital of Cu single atom site by coordination engineering for selective oxidation of benzene [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
| MLA | Li, Shuchun et al. "Manipulating d-orbital of Cu single atom site by coordination engineering for selective oxidation of benzene" . | NATURE COMMUNICATIONS 16 . 1 (2025) . |
| APA | Li, Shuchun , Cao, Changsheng , Chen, Jiabin , Wen, Wen , Zhang, Xuefei , Cui, Longji et al. Manipulating d-orbital of Cu single atom site by coordination engineering for selective oxidation of benzene . | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
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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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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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Supported Pt catalysts often exhibit limited effectiveness in achieving complete methane oxidation, which restricts their commercial application. However, Pt catalysts are particularly attractive, especially in sulfur-containing environments, where commercial Pd catalysts are more susceptible to sulfur poisoning. Therefore, developing highly active Pt sites and gaining a deeper understanding of the intrinsic mechanisms governing methane combustion over Pt catalysts is essential. In this study, we present a highly active stannic oxide supported platinum catalyst (Pt/SnO2) for stable low-temperature methane combustion, achieving a T-90 as low as 390 degrees C at a high gas hourly space velocity (GHSV) of 60,000 mLg(cat)(-1)h(-1). This performance surpasses that of most other Pt catalysts as well as Pd/SnO2 and benchmark Pd/Al2O3. The superior SO2 tolerance of Pt/SnO2 was demonstrated by the stability of methane conversion at 500 degrees C, with only a minor reduction observed during the long-term online test. Characterization results indicate that the Pt atoms on SnO2 are electron-deficient and predominantly adopt a crowded configuration. In situ studies and density functional theory (DFT) calculations reveal that the electron-deficient, crowded Pt atoms enhance the chemisorption of CH4 molecules by withdrawing the electrons from CH4, resulting in activated CH4 with an elongated C-H bond. This work provides an in-depth understanding of the nature of Pt active sites for high-performance methane combustion, offering valuable insights for the rational design of Pt-based catalysts.
Keyword ：
crowding-atom sites crowding-atom sites electron-deficient electron-deficient methane combustion methane combustion platinum platinum SnO2 SnO2
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| GB/T 7714 | Wang, Ran , Li, Guobo , Zong, Xupeng et al. Electron Withdrawal from Methane by Pt Atoms on Stannic Oxide for Highly Active Low-Temperature Combustion [J]. | ENVIRONMENTAL SCIENCE & TECHNOLOGY , 2025 , 59 (24) : 12121-12131 . |
| MLA | Wang, Ran et al. "Electron Withdrawal from Methane by Pt Atoms on Stannic Oxide for Highly Active Low-Temperature Combustion" . | ENVIRONMENTAL SCIENCE & TECHNOLOGY 59 . 24 (2025) : 12121-12131 . |
| APA | Wang, Ran , Li, Guobo , Zong, Xupeng , Wang, Jiaxing , Xu, Yuanjie , Jin, Chengwen et al. Electron Withdrawal from Methane by Pt Atoms on Stannic Oxide for Highly Active Low-Temperature Combustion . | ENVIRONMENTAL SCIENCE & TECHNOLOGY , 2025 , 59 (24) , 12121-12131 . |
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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 , 68 (7) : 2867-2891 . |
| MLA | Xu, Yuanjie et al. "Recent progress in exploring heterogeneous catalyst surface chemistry with near ambient pressure XPS" . | SCIENCE CHINA-CHEMISTRY 68 . 7 (2025) : 2867-2891 . |
| APA | Xu, Yuanjie , An, Zemin , Tang, Yu . Recent progress in exploring heterogeneous catalyst surface chemistry with near ambient pressure XPS . | SCIENCE CHINA-CHEMISTRY , 2025 , 68 (7) , 2867-2891 . |
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NiFe-based (oxy)hydroxides are widely recognized as highly promising electrocatalysts for the alkaline oxygen evolution reaction (OER). Despite their potential, their low conductivity and sluggish charge transfer kinetics pose significant challenges to further enhancing their catalytic activity. Herein, a novel catalyst featuring Ru single-atoms (SAs) coordinately dispersed on nickel-iron vanadium layered triple hydroxides (Ru SAs@NiFeV-LTHs) to improve alkaline OER performance is reported. With a Ru loading of 0.33 wt.%, this catalyst demonstrates outstanding performance, with a low Tafel slope of 27.15 mV dec(-1) and minimal overpotentials of 221 and 269 mV to achieve current densities of 10 and 100 mA cm(-2), respectively, outperforming unmodified NiFeV-LTHs and most other layered hydroxides reported in the literature. Furthermore, the catalyst exhibits exceptional durability, maintaining stable overpotentials for 200 hours at current densities of 10 mA cm(-2), 100 mA cm(-2), and 500 mA cm(-2). Density functional theory (DFT) calculations, coupled with experimental observations, identify the presence of Ru SAs as the key factor, which not only serve as superior active sites but also as modifiers of the electronic properties of the support material, thereby improving the overall conductivity and enhancing the intrinsic activity of metal sites in the catalyst's support.
Keyword ：
electronic interactions electronic interactions layered triple hydroxides layered triple hydroxides oxygen evolution reaction oxygen evolution reaction Ru single-atoms Ru single-atoms
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| GB/T 7714 | Shi, Ningning , Xue, Weichao , Liu, Panpan et al. Atomically Dispersed Ru on NiFeV Layered Triple Hydroxides for Enhanced Water Oxidation [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (24) . |
| MLA | Shi, Ningning et al. "Atomically Dispersed Ru on NiFeV Layered Triple Hydroxides for Enhanced Water Oxidation" . | ADVANCED FUNCTIONAL MATERIALS 35 . 24 (2025) . |
| APA | Shi, Ningning , Xue, Weichao , Liu, Panpan , Zeng, Chaobin , Yue, Shengnan , Xie, Wangjing et al. Atomically Dispersed Ru on NiFeV Layered Triple Hydroxides for Enhanced Water Oxidation . | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (24) . |
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