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学者姓名：汪思波
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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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Water electrolysis hydrogen production technology directly generates high-purity hydrogen through electrochemical water splitting, serving as a key technology for achieving zero-carbon emission hydrogen production. Alkaline water electrolysis demonstrates marked advantages in efficiency and rapidly developing anode catalysts in an alkaline medium. Nevertheless, the sluggish kinetics of the hydrogen evolution reaction (HER) at the cathode in an alkaline environment constitute a fundamental bottleneck that restricts the extensive application of this technology. Platinum, serving as the benchmark catalyst for the HER, is limited in its large-scale development due to its scarcity and high cost. In comparison, carbon-supported platinum-based catalysts exhibit exceptional HER catalytic activity and stability, driven by their unique electronic architecture and the synergistic effect with the support. In this review, we comprehensively examine the latest progress of carbon-supported platinum-based materials for the alkaline HER, summarize the factors contributing to the slow kinetics of the HER in an alkaline environment, and then focus on the strategies for modifying the carbon substrate and synthesizing carbon-supported platinum-based nanomaterials. Finally, the review critically evaluates existing challenges and proposes targeted research directions to advance Pt-based electrocatalysts for practical alkaline hydrogen evolution systems.
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| GB/T 7714 | Yang, Qiuyue , Zeng, Jilan , Yang, Guowei et al. Carbon-supported platinum-based electrocatalysts for alkaline hydrogen evolution [J]. | EES CATALYSIS , 2025 , 3 (5) : 972-993 . |
| MLA | Yang, Qiuyue et al. "Carbon-supported platinum-based electrocatalysts for alkaline hydrogen evolution" . | EES CATALYSIS 3 . 5 (2025) : 972-993 . |
| APA | Yang, Qiuyue , Zeng, Jilan , Yang, Guowei , Sun, Xinran , Lin, Xiahui , Liu, Kunlong et al. Carbon-supported platinum-based electrocatalysts for alkaline hydrogen evolution . | EES CATALYSIS , 2025 , 3 (5) , 972-993 . |
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Lattice oxygen-mediated photocatalytic ethane dehydrogenation represents a sustainable strategy for ethylene production, yet achieving a balance between high productivity, selectivity, and durability remains challenging. Here, we report a defective NiO-300 catalyst, where precisely engineered Ni vacancies activate lattice oxygen by weakening Ni-O bond and improving lattice oxygen mobility. This promotes efficient ethane activation and C-H bonds cleavage through photoinduced hole capture, intensifying ethane dehydrogenation via a light-boosted Mars-van Krevelen mechanism. The NiO-300 catalyst manifests a high ethylene yield of 604.5 mu mol g-1 h-1 with 100% selectivity and stability over 200 cycles. In situ spectroscopic and theoretical studies elucidate the generation of active oxygen species, the evolution of Ni coordination, the formation of key intermediates, and the underlying photocatalytic mechanism. Our findings highlight cation vacancy engineering as a powerful tactic to fully activate lattice oxygen for solar-driven alkene production from alkane dehydrogenation over oxide photocatalysts.
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| GB/T 7714 | Wei, Fen , Zhao, Jiwu , Liu, Yu-Chun et al. Photocatalytic ethylene production over defective NiO through lattice oxygen participation [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
| MLA | Wei, Fen et al. "Photocatalytic ethylene production over defective NiO through lattice oxygen participation" . | NATURE COMMUNICATIONS 16 . 1 (2025) . |
| APA | Wei, Fen , Zhao, Jiwu , Liu, Yu-Chun , Hsu, Yung-Hsi , Hung, Sung-Fu , Fu, Junwen et al. Photocatalytic ethylene production over defective NiO through lattice oxygen participation . | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
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Poly(triazine imide) (PTI) holds significant promise for photocatalytic CO2 reduction by addressing the limitations of conventional carbon nitrides. However, its practical application remains constrained by a narrow visible-light absorption. Herein, we report a barbituric acid (BA)-mediated copolymerization strategy to engineer pi-electron delocalization within the triazine framework for broadening light-harvesting spectrum and optimizing charge carrier transport. Under visible light irradiation (lambda >= 400 nm), the optimized PTI-BA(1.0) photocatalyst achieves a CO evolution rate of 10 mu mol h(-1) (333 mu mol g(-1) h(-1)) with 95% selectivity, representing a 5-fold enhancement over pristine PTI. Remarkably, the apparent quantum efficiency reaches 13.6% at 365 nm, underscoring its superior CO2 photoconversion capability. Mechanistic investigations via in situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculations elucidate the energetically favorable pathways for CO2 activation, reduction and CO desorption. This work not only provides a rational design strategy for modulating the optoelectronic properties of crystalline carbon nitride but also advances the development of high-performance photocatalysts for sustainable CO2 conversion.
Keyword ：
carbon nitride carbon nitride CO2 reduction CO2 reduction copolymerization copolymerization photocatalysis photocatalysis poly(triazineimide) poly(triazineimide)
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| GB/T 7714 | Liu, Feng , Xie, Zongyuan , Su, Bo et al. Enhancing Visible Light CO2 Reduction via π-Electron Delocalization in Barbituric Acid-Modified Poly(triazine imide) Crystals [J]. | ACS CATALYSIS , 2025 , 15 (17) : 15033-15042 . |
| MLA | Liu, Feng et al. "Enhancing Visible Light CO2 Reduction via π-Electron Delocalization in Barbituric Acid-Modified Poly(triazine imide) Crystals" . | ACS CATALYSIS 15 . 17 (2025) : 15033-15042 . |
| APA | Liu, Feng , Xie, Zongyuan , Su, Bo , Guo, Binbin , Lin, Xiahui , Xing, Wandong et al. Enhancing Visible Light CO2 Reduction via π-Electron Delocalization in Barbituric Acid-Modified Poly(triazine imide) Crystals . | ACS CATALYSIS , 2025 , 15 (17) , 15033-15042 . |
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Photocatalytic O-2 reduction to H2O2 is a green and promising technology with advantages in cost-effectiveness, sustainability, and environmental friendliness, but its efficiency is constrained by limited selectivity for the two-electron oxygen reduction reaction (ORR) pathway. Here, we anchored isolated Cu atoms with tunable oxidation states onto WO3 as effective active centers to enhance photocatalytic H2O2 production. Due to the charge compensation between single atoms and the support, the oxidation state of Cu species exhibited a loading-dependent transition between +2 and +1 valence. Experimental and theoretical analyses indicate that Cu(I) sites exhibit outstanding O-2 adsorption and activation capabilities, transforming the thermodynamically unfavorable hydrogenation of the *OOH intermediate (the rate-determining step in the two-electron ORR pathway) into an exothermic process, thereby significantly improving selectivity and efficiency. The Cu(I)-SA/WO3 photocatalyst exhibited a H2O2 production rate of 102 mu mol h(-1) under visible light irradiation, much higher than other reported photocatalysts. More importantly, it achieves an impressive apparent quantum efficiency of 30% at 420 nm, making a significant breakthrough in this field. This work provides novel perspectives for designing single-atom catalysts for efficient H2O2 synthesis via electronic state modulation.
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| GB/T 7714 | Yang, Fan , Feng, Chengyang , Zuo, Shouwei et al. Photocatalytic H2O2 Production with >30% Quantum Efficiency via Monovalent Copper Dynamics [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (20) : 17112-17120 . |
| MLA | Yang, Fan et al. "Photocatalytic H2O2 Production with >30% Quantum Efficiency via Monovalent Copper Dynamics" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 20 (2025) : 17112-17120 . |
| APA | Yang, Fan , Feng, Chengyang , Zuo, Shouwei , Wang, Qingxiao , Wei, Fen , Hu, Miao et al. Photocatalytic H2O2 Production with >30% Quantum Efficiency via Monovalent Copper Dynamics . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (20) , 17112-17120 . |
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Lattice oxygen (LO)-mediated photothermal dry reforming of methane (DRM) presents a promising approach to syngas production. However, realizing high DRM efficiency and durability remains challenging due to the difficulty in activating LOs in catalysts. Herein, we demonstrate that partially substituting Fe sites in perovskite ferrite (LaFeO3) by Mn triggers LOs, bestowing the catalyst with superior activity and stability for photothermal DRM after modification with Ru. The Mn exchange induces a charge transfer from La to Mn, which combined with the incoming photoexcited electrons reconstructs the perovskite's electronic structure, weakening the La-O-Mn bonds and facilitating the LO migration. Meanwhile, photogenerated holes migrate to surface LOs, further enhancing their reactivity to mediate DRM. Under light irradiation, the catalyst exhibits an outstanding syngas production rate (H2: 42.89 mol gRu -1 h-1, CO: 54.92 mol gRu -1 h-1) while stably operating over 150 h. It also achieves a methane turnover frequency of 0.9 s-1 and a light-to-chemical energy efficiency of 15.3%, setting a benchmark for light-driven DRM performance. This work underscores the significance of exact site doping in metal oxides to fine-tune LO activity, providing valuable guidance for fabricating efficient catalysts for solar-powered redox reactions proceeded via the light-supported Mars-van Krevelen mechanism.
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| GB/T 7714 | Li, Jilong , Zhao, Jiwu , Wang, Sibo et al. Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (17) : 14705-14714 . |
| MLA | Li, Jilong et al. "Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 17 (2025) : 14705-14714 . |
| APA | Li, Jilong , Zhao, Jiwu , Wang, Sibo , Peng, Kang-Shun , Su, Bo , Liu, Kunlong et al. Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (17) , 14705-14714 . |
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Elevating the long-wavelength activation of photocatalysts represents a formidable approach to optimizing sunlight utilization. Polythiophene (PTh), although renowned for its robust light absorption and excellent conductivity, is largely overlooked for its potential as a photocatalyst due to the swift recombination of photogenerated charge carriers. Herein, we unveil that the strategic introduction of an aromatic ring containing varying nitrogen content into PTh instigates polarized charge distribution and facilitates the narrowing of the band gap, thereby achieving efficient photocatalytic activities for both hydrogen and hydrogen peroxide generation. Notably, the best sample, PTh-N2, even demonstrates photocatalytic activity in the red light region (600-700 nm). This study offers a promising avenue for the development of polymer photocatalysts with efficient photocatalytic performance for red light-induced photocatalysis.
Keyword ：
Hydrogen evolution Hydrogen evolution Hydrogen peroxide evolution Hydrogen peroxide evolution Polarized charge distribution Polarized charge distribution Polythiophene derivatives Polythiophene derivatives Red light-induced photocatalysis Red light-induced photocatalysis
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| GB/T 7714 | Chen, Qian , Tian, Lin , Ren, Wei et al. Nitrogen Modified Linear Polythiophene Derivatives with Polarized Charge Distribution for Red Light-Induced Photocatalysis [J]. | CHEMSUSCHEM , 2025 , 18 (10) . |
| MLA | Chen, Qian et al. "Nitrogen Modified Linear Polythiophene Derivatives with Polarized Charge Distribution for Red Light-Induced Photocatalysis" . | CHEMSUSCHEM 18 . 10 (2025) . |
| APA | Chen, Qian , Tian, Lin , Ren, Wei , Zhang, Xirui , Li, Guosheng , Wang, Sibo et al. Nitrogen Modified Linear Polythiophene Derivatives with Polarized Charge Distribution for Red Light-Induced Photocatalysis . | CHEMSUSCHEM , 2025 , 18 (10) . |
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As a crystalline allotrope of carbon nitrides, poly (heptazine imide) (PHI) exhibits great potential for photocatalytic reforming of biomass-derived alcohols. However, its activity is greatly constrained due to insufficient charge migration and severe non-radiative recombination. To address this issue, PHI with high interlayer stacking orderliness is fabricated through a facile ion exchange strategy. Characterizations reveal that rational modification of the interlayer stacking mode of PHI could efficiently suppress non-radiative recombination and improve charge transfer efficiency. Accordingly, the optimal sample exhibits high photocatalytic reforming activity for H2 evolution, which is up to 2.16 mmolg-1h-1, and with a quantum efficiency reaches 26.7% at 400 nm.
Keyword ：
Biomass conversion Biomass conversion Hydrogen production Hydrogen production Interlayer stacking modes Interlayer stacking modes Nonradiative recombination Nonradiative recombination Poly heptazine imide Poly heptazine imide
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| GB/T 7714 | Sun, Qiqi , Cheng, Xiaohong , Qie, Mingyang et al. Photocatalytic Reforming of Methanol Over Poly Heptazine Imide: Interlayer Stacking Modification Induced Rapid Charge Transfer [J]. | CHEMCATCHEM , 2025 , 17 (10) . |
| MLA | Sun, Qiqi et al. "Photocatalytic Reforming of Methanol Over Poly Heptazine Imide: Interlayer Stacking Modification Induced Rapid Charge Transfer" . | CHEMCATCHEM 17 . 10 (2025) . |
| APA | Sun, Qiqi , Cheng, Xiaohong , Qie, Mingyang , Pan, Zhiming , Li, Guosheng , Zhang, Xirui et al. Photocatalytic Reforming of Methanol Over Poly Heptazine Imide: Interlayer Stacking Modification Induced Rapid Charge Transfer . | CHEMCATCHEM , 2025 , 17 (10) . |
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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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Achieving intimate interfacial contact between a hydrogen evolution photocatalyst (HEP) and an oxygen evolution photocatalyst (OEP) is crucial for efficient charge carrier transfer, which in turn enhances overall water splitting (OWS) performance. However, traditional metal oxide-based photocatalysts often possess intrinsic limitations. In this study, carbon nitride (CN) with tunable electrostatic properties is employed to form a heterostructure with metal oxides through self-assembly. As such, protonated polymeric CN nanosheets functioned as the HEP, while NiTiO3 nanoparticles served as the OEP, resulting in a photocatalytic system for OWS, exhibiting H-2 and O-2 evolution rates of 35.6 and 17.7 mu mol h(-)(1), respectively. The corresponding apparent quantum yield is 2.7% at an incident wavelength of 365 nm. These results outperform those of individual photocatalysts. This study introduces a universally applicable electrostatic self-assembly strategy for using CN to construct redox-mediator-free heterojunctions, thereby advancing applications in various fields, particularly the hydrogen evolution reaction via photocatalytic OWS.
Keyword ：
electrostatic self-assemblies electrostatic self-assemblies heterojunctions heterojunctions internal electric fields internal electric fields NiTiO3 NiTiO3 overall water splittings overall water splittings
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| GB/T 7714 | Wang, Long , Wu, Haihua , Lin, Yifan et al. Electrostatic Self-Assembly of NiTiO3 on Carbon Nitride as a Photocatalyst for Visible-Light-Driven Overall Water Splitting [J]. | CHEMSUSCHEM , 2025 , 18 (13) . |
| MLA | Wang, Long et al. "Electrostatic Self-Assembly of NiTiO3 on Carbon Nitride as a Photocatalyst for Visible-Light-Driven Overall Water Splitting" . | CHEMSUSCHEM 18 . 13 (2025) . |
| APA | Wang, Long , Wu, Haihua , Lin, Yifan , Wang, Mingyue , Wang, Zilong , Xing, Wandong et al. Electrostatic Self-Assembly of NiTiO3 on Carbon Nitride as a Photocatalyst for Visible-Light-Driven Overall Water Splitting . | CHEMSUSCHEM , 2025 , 18 (13) . |
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