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学者姓名：陈雄
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Abstract ：
The selective oxidation of methane to value-added chemicals under mild conditions presents a sustainable yet challenging route, hindered by sluggish CH4 activation and overoxidation. Herein, we report a delicate strategy combining Ti doping and Au loading to construct a high-performance Au/Ti-CeO2 photocatalyst for ethane production from oxidative methane coupling. The optimized catalyst achieves a C2H6 production rate of 2971.4 μmol g−1 h−1 with 85.1 % C2+ selectivity, stably operating over 20 reaction cycles. In situ X-ray photoelectron spectroscopy, electron paramagnetic resonance, and diffuse reflectance infrared Fourier transform spectroscopy analyses reveal that Ti doping introduces impurity energy levels into CeO2, promoting directional electron migration to surface Au nanoparticles (NPs) via a built-in electric field. The Au NPs act as electron accumulation sites to activate O2, facilitate ∗CH3 radical coupling into C2H6, and stabilize reactive intermediates, thus enhancing charge separation and suppressing intermediate overoxidation. This study highlights the significance of synergistic modulation via elemental doping and cocatalyst engineering in tuning charge dynamics and surface reactivity for efficient photocatalytic methane conversion. © 2025 College of Chemistry and Molecular Engineering, Peking University
Keyword ：
CeO2 CeO2 Charge separation Charge separation Ethane production Ethane production Methane oxidation Methane oxidation Photocatalysis Photocatalysis Ti doping Ti doping
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| GB/T 7714 | Xu, X. , Lu, J. , Su, B. et al. Steering charge dynamics and surface reactivity for photocatalytic selective methane oxidation to ethane over Au/Ti-CeO2 [J]. | Acta Physico - Chimica Sinica , 2025 , 41 (11) . |
| MLA | Xu, X. et al. "Steering charge dynamics and surface reactivity for photocatalytic selective methane oxidation to ethane over Au/Ti-CeO2" . | Acta Physico - Chimica Sinica 41 . 11 (2025) . |
| APA | Xu, X. , Lu, J. , Su, B. , Chen, J. , Chen, X. , Wang, S. . Steering charge dynamics and surface reactivity for photocatalytic selective methane oxidation to ethane over Au/Ti-CeO2 . | Acta Physico - Chimica Sinica , 2025 , 41 (11) . |
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Covalent organic frameworks (COFs) have emerged as a compelling class of materials for active layers in memristors, yet the determinants of their electrical properties and effective tuning strategies remain elusive. Herein, the study unveils two novel pyrene-based COFs (Py-COFs)-the one-dimensional (1D) H-Py-BT COF and the two-dimensional (2D) Py-BT COF-crafted with structural kinship yet divergent dimensionalities via tailored pyrene monomer connectivity. The effect of structural and dimensional disparities on memristive device performance and image recognition precision is systematically investigated. Notably, the 1D H-Py-BT COF harnesses weak in-plane and interlayer hydrogen bonding interactions to enhance charge separation and promote directional electron transport. This unique configuration enables devices fabricated with the 1D H-Py-BT COF (101 nm thick) to deliver exceptional performance, evidenced by a high ON/OFF current ratio (approximate to 103.7) and an image recognition accuracy of 76%, outperforming those based on the 2D Py-BT COF. These findings underscore the pivotal role of COF dimensionality and molecular interactions in dictating device functionality, offering valuable insights for advancing COF-based memristive technologies.
Keyword ：
1D covalent organic framework 1D covalent organic framework intermolecular hydrogen bonding intermolecular hydrogen bonding memristors memristors neuromorphic computing neuromorphic computing synaptic mimicry synaptic mimicry
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| GB/T 7714 | Huang, Yuxing , Yang, Wanxiang , Zhou, Pan-Ke et al. Intermolecular Hydrogen-Bond Stabilized 1D Pyrene-Based Covalent Organic Framework for Advanced Memory Devices and Neuromorphic Computing [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Huang, Yuxing et al. "Intermolecular Hydrogen-Bond Stabilized 1D Pyrene-Based Covalent Organic Framework for Advanced Memory Devices and Neuromorphic Computing" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Huang, Yuxing , Yang, Wanxiang , Zhou, Pan-Ke , Liu, Nengyi , Xu, Shumeng , Qiu, Jiawen et al. Intermolecular Hydrogen-Bond Stabilized 1D Pyrene-Based Covalent Organic Framework for Advanced Memory Devices and Neuromorphic Computing . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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The indirect anthraquinone method is currently used to produce H2O2, but it leads to high energy consumption and a large amount of chemical waste. Alternatively, water oxidation reactions offer a potential green approach for H2O2 production, although it is constrained by low selectivity. Herein, the functional photoanodes are rationally designed for H2O2 production via photocatalytic water oxidation. Specifically, P/Mo co-doped BiVO4 films are achieved on a conductive glass to serve as the photocatalytic layer, which is coated with an ultrathin amorphous TiO2 film to achieve good stability. Importantly, metal-free P-doped polymeric carbon nitride dots are deposited on the photoanode, acting as the reaction centres. This innovative approach moves away from the traditional reliance on inorganic materials as co-catalysts in order to suppress the thermodynamically favoured O-2 evolution, which, in turn, significantly enhances the selectivity, efficiency and stability of H2O2 production. Consequently, an optimal selectivity of approximate to 64% for H2O2 production is achieved at an applied voltage bias of 1.7 V versus RHE in a 1.0 m KHCO3 solution, achieving a yield of approximate to 34.2 mu mol hr(-1) cm(-2). This research offers a novel strategy for developing photocatalytic films with optimised co-catalysts for a photoanode in photocatalytic H2O2 synthesis.
Keyword ：
BiVO4 BiVO4 H2O2 synthesis H2O2 synthesis photoanode photoanode polymeric carbon nitride dots polymeric carbon nitride dots water oxidation water oxidation
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| GB/T 7714 | Wang, Yankun , Xu, Yuntao , Zhang, Xirui et al. Integrating P-Doped Carbon Nitride Dots as Active Sites on P/Mo Co-Doped BiVO4 Photoanodes Promotes H2O2 Production [J]. | SMALL , 2025 , 21 (21) . |
| MLA | Wang, Yankun et al. "Integrating P-Doped Carbon Nitride Dots as Active Sites on P/Mo Co-Doped BiVO4 Photoanodes Promotes H2O2 Production" . | SMALL 21 . 21 (2025) . |
| APA | Wang, Yankun , Xu, Yuntao , Zhang, Xirui , Qian, Rong , Chen, Xiong , Chen, Qiao et al. Integrating P-Doped Carbon Nitride Dots as Active Sites on P/Mo Co-Doped BiVO4 Photoanodes Promotes H2O2 Production . | SMALL , 2025 , 21 (21) . |
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Kinetic factors frequently emerge as the primary constraints in photocatalysis, exerting a critical influence on the efficacy of polymeric photocatalysts. The diverse conjugation systems within covalent organic frameworks (COFs) can significantly impact photon absorption, energy level structures, charge separation and migration kinetics. Consequently, these limitations often manifest as unsatisfactory kinetic behavior, which adversely affects the photocatalytic activity of COFs. To address these challenges, we propose a methoxy (-OMe) molecular engineering strategy designed to enhance charge carrier kinetics and mitigate mass transfer resistance. Through strategic modulation of the position and quantity of -OMe units, we can effectively manipulate the p-pi conjugation, thereby enhancing charge separation and migration. Moreover, COFs enriched with -OMe moieties exhibit enhanced mass transfer dynamics due to the hydrophilic nature of methoxy groups, which facilitate the diffusion of reactants and products within the porous structure. This approach is hypothesized to drive an efficient photocatalytic hydrogen evolution reaction.
Keyword ：
Charge separation Charge separation Covalent Organic Framework Covalent Organic Framework Hydrogen evolution Hydrogen evolution Photocatalysis Photocatalysis p-pi resonance effect p-pi resonance effect
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| GB/T 7714 | Luo, Zhipeng , Zhu, Shipeng , Xue, Huanglan et al. Manipulating p-π Resonance through Methoxy Group Engineering in Covalent Organic Frameworks for an Efficient Photocatalytic Hydrogen Evolution [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (6) . |
| MLA | Luo, Zhipeng et al. "Manipulating p-π Resonance through Methoxy Group Engineering in Covalent Organic Frameworks for an Efficient Photocatalytic Hydrogen Evolution" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 6 (2025) . |
| APA | Luo, Zhipeng , Zhu, Shipeng , Xue, Huanglan , Yang, Wanxiang , Zhang, Fengtao , Xu, Fei et al. Manipulating p-π Resonance through Methoxy Group Engineering in Covalent Organic Frameworks for an Efficient Photocatalytic Hydrogen Evolution . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (6) . |
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The rapid evolution of neuromorphic devices seeks to bridge biological neural networks and artificial systems, enabling energy-efficient and scalable computing for next-generation artificial intelligence. Herein, we introduce methyl-engineered one-dimensional covalent organic framework (1D COF)-based memristors as a transformative platform for reconfigurable neuromorphic computing. The incorporation of methyl groups enhances localized polarization effects within the COF framework, effectively mitigating random Ag+ migration/diffusion and stabilizing conductive filament morphology. This strategic modification yields devices with exceptional multilevel storage capabilities, exhibiting superior stability, linearity, and reproducibility. Moreover, the highly ordered architecture and customizable chemical environment of the methyl-functionalized 1D COF allows for precise control over resistive switching behaviors, facilitating the emulation of synaptic functions and the development of artificial neural network architectures. Demonstrating exceptional performance in neuromorphic tasks such as high-accuracy image recognition, these devices showcase significant promise as the foundation for energy-efficient, next-generation neuromorphic computing systems.
Keyword ：
Localized polarization effects Localized polarization effects Memristors Memristors Multilevelmemory device Multilevelmemory device Neuromorphic computing Neuromorphic computing One-dimensional covalent organic frameworks One-dimensional covalent organic frameworks
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| GB/T 7714 | Zhou, Pan-Ke , Yu, Ziyue , Zeng, Tao et al. Reconfigurable Neuromorphic Computing Using Methyl-Engineered One-Dimensional Covalent Organic Framework Memristors [J]. | NANO LETTERS , 2025 , 25 (14) : 5891-5898 . |
| MLA | Zhou, Pan-Ke et al. "Reconfigurable Neuromorphic Computing Using Methyl-Engineered One-Dimensional Covalent Organic Framework Memristors" . | NANO LETTERS 25 . 14 (2025) : 5891-5898 . |
| APA | Zhou, Pan-Ke , Yu, Ziyue , Zeng, Tao , Zhang, Cong , Huang, Yuxing , Chen, Qian et al. Reconfigurable Neuromorphic Computing Using Methyl-Engineered One-Dimensional Covalent Organic Framework Memristors . | NANO LETTERS , 2025 , 25 (14) , 5891-5898 . |
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The development of stimuli-responsive switching memory devices and the elucidation of their switching mechanisms in specific environments are crucial for advancing the field of molecular electronics. Herein, we propose two distinct two-dimensional covalent organic frameworks (COFs), namely Py-EDA and Py-BDA, incorporating acetylene (-C equivalent to C-) or diacetylene (-C equivalent to C-C equivalent to C-) moieties, respectively, targeting fabricate memory devices exhibiting stimuli-responsive switching behavior. Our findings demonstrate that the incorporation of acetylene units effectively modulates the electronic band structure and enhances the degree of pi-conjugation, resulting in devices that exhibit typical bipolar nonvolatile memory performance. Notably, upon thermal treatment, the memory behavior of the ITO/Py-BDA/Ag device transitions to a write-once-read-many-times (WORM) mode, displaying decreased SET voltage, increased ON/OFF current ratio, and remarkable retention reliability and cycle stability. This switching behavior is attributed to the occurrence of interlayer solid-state topological polymerization at 350 degrees C, leading to the transformation of diacetylene columnar arrays into enyne chains within Py-BDA, thereby further promoting interlayer charge transfer and separation.
Keyword ：
memory device memory device stimuli-response stimuli-response switching mechanism switching mechanism topological polymerization topological polymerization two-dimensional covalent organic frameworks two-dimensional covalent organic frameworks
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| GB/T 7714 | Zhou, Pan-Ke , Huang, Yuxing , Yu, Ziyue et al. Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties [J]. | SCIENCE CHINA-CHEMISTRY , 2025 , 68 (7) : 3230-3237 . |
| MLA | Zhou, Pan-Ke et al. "Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties" . | SCIENCE CHINA-CHEMISTRY 68 . 7 (2025) : 3230-3237 . |
| APA | Zhou, Pan-Ke , Huang, Yuxing , Yu, Ziyue , Zhang, Cong , Chen, Qian , Li, Yiping et al. Thermally triggered topological polymerization in diacetylene-functionalized covalent organic framework toward enhanced memristive properties . | SCIENCE CHINA-CHEMISTRY , 2025 , 68 (7) , 3230-3237 . |
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Multifunctional memristors with a high memory density, low power consumption, flexibility, programmability, and environmental robustness are essential for next-generation memories. In this work, a titanocene-polysulfide complex (Cp2TiS5) with strong SS interactions and hydrogen bonds was synthesized and integrated with TiO2 to create a novel Cu/TiO2/Cp2TiS5/Ag memristor. This device shows bipolar nonvolatile memory performance with a remarkable ON/OFF ratio (104.8), low switching voltages (V SET, -0.16 V; V RESET, +0.15 V), and low power consumption (2.7 x 10-4 mu W). It exhibits multilevel memory behavior, flexibility, optical modulation (V SET decreases from -1.35 to -0.17 V with decreasing irradiation wavelength), and thermal tolerance (up to 200 degrees C). The electron-rich Cp2TiS5 layer protects the Ag-CFs, while TiO2's oxygen vacancies and unsaturated Ti atoms interact with sulfur from Cp2TiS5, lowering the Schottky barrier and facilitating charge transport. This work offers promising opportunities in flexible memristive devices for neuromorphic computing under extreme conditions.
Keyword ：
flexible memory flexible memory interfacial engineering interfacial engineering memristor memristor multilevel memory multilevel memory titanocene-polysulfide titanocene-polysulfide
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| GB/T 7714 | Zhou, Panke , Lin, Xi , Gao, Yiqun et al. Engineering Titanium Dioxide/Titanocene-Polysulfide Interface for Flexible, Optical-Modulated, and Thermal-Tolerant Multilevel Memristor [J]. | NANO LETTERS , 2025 , 25 (7) : 2741-2748 . |
| MLA | Zhou, Panke et al. "Engineering Titanium Dioxide/Titanocene-Polysulfide Interface for Flexible, Optical-Modulated, and Thermal-Tolerant Multilevel Memristor" . | NANO LETTERS 25 . 7 (2025) : 2741-2748 . |
| APA | Zhou, Panke , Lin, Xi , Gao, Yiqun , Lin, Xiaoli , Zeng, Tao , Li, Haohong et al. Engineering Titanium Dioxide/Titanocene-Polysulfide Interface for Flexible, Optical-Modulated, and Thermal-Tolerant Multilevel Memristor . | NANO LETTERS , 2025 , 25 (7) , 2741-2748 . |
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Metal-organic frameworks (MOFs) composed of infinite metal units exhibit enhanced electron transport and charge migration capabilities compared to discrete metal units. Herein, three underdeveloped isomorphic MOFs featuring 3D infinite zinc units are designed and synthesized. The Lewis acidity and photocatalytic activity of these MOFs are fine-tuned through atomic-level engineering of nitrogen atoms of ligands and the resultant change of charge transfer modes. These MOFs are promising catalysts in the photocatalytic monooxygenation of sulfenamides with molecular oxygen. Mechanistic investigations suggest that the uneven charge distribution and large dipole moment at the pyridine center of 1-PTB and the infinite Zn unit frameworks of degenerate energy levels are key to its excellent photocatalytic activity.
Keyword ：
aerobic photooxidation aerobic photooxidation atomic-scale regulation atomic-scale regulation CO2 cycloaddition CO2 cycloaddition infinite trinuclear Zn units infinite trinuclear Zn units metal-organic frameworks metal-organic frameworks
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| GB/T 7714 | He, Xinglei , Yu, Chunlong , Zhang, Fengtao et al. Ligand-Engineered Metal-Organic Frameworks of 3D Infinite Trinuclear Zinc Units for Photocatalytic Monooxygenation of Sulfenamides [J]. | ADVANCED SCIENCE , 2025 , 12 (33) . |
| MLA | He, Xinglei et al. "Ligand-Engineered Metal-Organic Frameworks of 3D Infinite Trinuclear Zinc Units for Photocatalytic Monooxygenation of Sulfenamides" . | ADVANCED SCIENCE 12 . 33 (2025) . |
| APA | He, Xinglei , Yu, Chunlong , Zhang, Fengtao , Gong, Chenxu , Li, Jingheng , Zeng, Ding-Bo et al. Ligand-Engineered Metal-Organic Frameworks of 3D Infinite Trinuclear Zinc Units for Photocatalytic Monooxygenation of Sulfenamides . | ADVANCED SCIENCE , 2025 , 12 (33) . |
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Polymeric carbon nitrides (PCNs), usually the melon phase, have been extensively applied as photocatalysts for CO2 reduction; however, their performance is still unsatisfactory. The condensed allotrope, namely, poly(triazine imide) (PTI) with extended conjugation and a crystallized structure, indeed holds more favorable compositional and structural advantages for photocatalytic CO(2)reduction but remains to be fully exploited. Herein, hexagonal prism-shaped PTI crystals were synthesized and developed as a high-performance photocatalyst for CO2 reduction. With Co(bpy)(3) (2+) as a cocatalyst, the PTI crystals exhibit a CO evolution rate of 44 mu mol h(-1) (i.e., 1467 mu mol g(-1) h(-1)) with 93% selectivity, markedly superior to that of the melon counterpart. Moreover, PTI crystals manifest an apparent quantum efficiency of 12.9% at 365 nm, representing the state-of-the-art value by PCN photocatalysts for CO2-to-CO reduction without using noble metals. The surface pyridine N species of PTI are exposed as active sites to dominate CO2 activation and conversion, which, together with the high crystallinity to facilitate charge separation and transport, endows high CO2 reduction efficiency. In situ diffuse reflectance infrared Fourier transform spectroscopy determines the key intermediates during the CO2 reduction reaction and, consequently, constructs the possible reaction mechanism.
Keyword ：
active sites active sites carbon nitride carbon nitride CO2 reduction CO2 reduction photocatalysis photocatalysis poly(triazineimide) poly(triazineimide) pyridine nitrogen pyridine nitrogen
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| GB/T 7714 | Liu, Feng , Deng, Jing , Su, Bo et al. Poly(triazine imide) Crystals for Efficient CO2 Photoreduction: Surface Pyridine Nitrogen Dominates the Performance [J]. | ACS CATALYSIS , 2025 , 15 (2) : 1018-1026 . |
| MLA | Liu, Feng et al. "Poly(triazine imide) Crystals for Efficient CO2 Photoreduction: Surface Pyridine Nitrogen Dominates the Performance" . | ACS CATALYSIS 15 . 2 (2025) : 1018-1026 . |
| APA | Liu, Feng , Deng, Jing , Su, Bo , Peng, Kang-Shun , Liu, Kunlong , Lin, Xiahui et al. Poly(triazine imide) Crystals for Efficient CO2 Photoreduction: Surface Pyridine Nitrogen Dominates the Performance . | ACS CATALYSIS , 2025 , 15 (2) , 1018-1026 . |
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Photocatalytic CO2 conversion with H2O to carbonaceous fuels is a desirable strategy for CO2 management and solar utilization, yet its efficiency remains suboptimal. Herein, efficient and durable CO2 photoreduction is realized over a Ru-NPs/Ru-PHI catalyst assembled by anchoring Ru single atoms (SAs) and nanoparticles (NPs) onto poly(heptazine imide) (PHI) via the in-plane Ru-N-4 coordination and interfacial Ru-N bonds, respectively. This catalyst shows an unsurpassed CO production (32.8 mu mol h(-1)), a record-high apparent quantum efficiency (0.26%) beyond 800 nm, and the formation of the valuable H2O2. Ru SAs tune PHI's electronic structure to promote in-plane charge transfer to Ru NPs, forming a built-in electron field at the interface, which directs electron-hole separation and rushes excited electron movement from Ru-PHI to Ru NPs. Simultaneously, Ru SAs introduce an impurity level in PHI to endow long-wavelength photoabsorption, while Ru NPs strengthen CO2 adsorption/activation and expedite CO desorption. These effects of Ru species together effectively ensure CO2-to-CO conversion. The CO2 reduction on the catalyst is revealed to follow the pathway CO2 -> *CO2 -> *COOH -> *CO -> CO, based on the intermediates identified by in situ diffuse reflectance infrared Fourier transform spectroscopy and further supported by density functional theory calculations.
Keyword ：
Carbon nitrides Carbon nitrides CO2 reduction CO2 reduction Photocatalysis Photocatalysis Poly (heptazine imide) Poly (heptazine imide)
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| GB/T 7714 | Su, Bo , Wang, Sibo , Xing, Wandong et al. Synergistic Ru Species on Poly(heptazine imide) Enabling Efficient Photocatalytic CO2 Reduction with H2O beyond 800 nm [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (27) . |
| MLA | Su, Bo et al. "Synergistic Ru Species on Poly(heptazine imide) Enabling Efficient Photocatalytic CO2 Reduction with H2O beyond 800 nm" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 27 (2025) . |
| APA | Su, Bo , Wang, Sibo , Xing, Wandong , Liu, Kunlong , Hung, Sung-Fu , Chen, Xiong et al. Synergistic Ru Species on Poly(heptazine imide) Enabling Efficient Photocatalytic CO2 Reduction with H2O beyond 800 nm . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (27) . |
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