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学者姓名：刘锟隆
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Abstract ：
The industrially important selective hydrogenation of alpha,beta-unsaturated aldehydes to allyl alcohol is still challenging to realize using heterogenous hydrogenation catalysts. Supported Cu catalysts have shown moderate selectivity, yet low activity for the reaction, due to the electronic structure of Cu. By anchoring atomically dispersed Pd atoms onto the exposed Cu surface of Cu@CeO2, we report in this work that hydrogen spillover activates the inert metal-oxide interfaces of Cu@CeO2 into highly effective and selective catalytic sites for hydrogenation under mild reaction conditions. The as-prepared catalysts exhibit much higher catalytic activity in the selective hydrogenation of acrolein than Cu@CeO2. Comprehensive studies reveal that atomically dispersed Pd species are critical for the activation and homolytic splitting of H2. The activated H atoms easily spill to the Cu-O-Ce interfaces as Cu-H delta-and interfacial Ce-O-H delta+ species, making them the active sites for hydrogenation of polar C=O bonds. Moreover, the weak adsorption of allyl alcohol on the Pd and Cu-O-Ce interfacial sites prevents deep hydrogenation, leading to selective hydrogenation of several alpha,beta-unsaturated aldehydes. Overall, we demonstrate here a synergic effect between single atom alloy and the support for activation of an inert metal- oxide interface into selective catalytic sites.
Keyword ：
Hydrogen spillover Hydrogen spillover Metal-oxide interface Metal-oxide interface Selective hydrogenation Selective hydrogenation Single-atom alloy Single-atom alloy Spillover hydrogenation Spillover hydrogenation
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| GB/T 7714 | Cui, Jinyuan , Yang, Tingting , Xu, Teng et al. Hydrogen spillover enhances the selective hydrogenation of α,β-unsaturated aldehydes on the Cu-O-Ce interface [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2025 , 44 (1) . |
| MLA | Cui, Jinyuan et al. "Hydrogen spillover enhances the selective hydrogenation of α,β-unsaturated aldehydes on the Cu-O-Ce interface" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 44 . 1 (2025) . |
| APA | Cui, Jinyuan , Yang, Tingting , Xu, Teng , Lin, Jin , Liu, Kunlong , Liu, Pengxin . Hydrogen spillover enhances the selective hydrogenation of α,β-unsaturated aldehydes on the Cu-O-Ce interface . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2025 , 44 (1) . |
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Among the current industrial hydrogen production technologies, electrolysis has attracted widespread attention due to its zero carbon emissions and sustainability. However, the existence of overpotential caused by reaction activation, mass/charge transfer, etc. makes the actual water splitting voltage higher than the theoretical value, severely limiting the industrial application of this technology. Therefore, it is particularly important to design and develop highly efficient electrocatalysts to reduce overpotential and improve energy efficiency. Among the various synthesis methods of electrocatalysts, electrochemical synthesis stands out due to its simplicity, easy reaction control, and low cost. This review article classifies and summarizes the electrochemical synthesis techniques (including electrodeposition, electrophoretic deposition, electrospinning, anodic oxidation, electrochemical intercalation, and electrochemical reconstruction), followed by their application in the field of water electrolysis. In addition, some challenges currently faced by electrochemical synthesis in electrocatalytic hydrogen production, and their potential solutions are discussed to promote the practical application of electrochemical synthesis in water electrolysis.Graphical AbstractThis review summarizes and classifies commonly used electrochemical synthesis techniques, followed by the application of electrochemical synthesis methods in research on water electrolysis. Additionally, some challenges faced by electrochemical synthesis in the field of water electrolysis and possible solutions are discussed.
Keyword ：
Electrocatalysts Electrocatalysts Electrochemical synthesis Electrochemical synthesis Green hydrogen Green hydrogen Water splitting Water splitting
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| GB/T 7714 | Wu, Yang , Xiao, Boxin , Liu, Kunlong et al. Electrochemical Synthesis of High-Efficiency Water Electrolysis Catalysts [J]. | ELECTROCHEMICAL ENERGY REVIEWS , 2025 , 8 (1) . |
| MLA | Wu, Yang et al. "Electrochemical Synthesis of High-Efficiency Water Electrolysis Catalysts" . | ELECTROCHEMICAL ENERGY REVIEWS 8 . 1 (2025) . |
| APA | Wu, Yang , Xiao, Boxin , Liu, Kunlong , Wang, Sibo , Hou, Yidong , Lu, Xue Feng et al. Electrochemical Synthesis of High-Efficiency Water Electrolysis Catalysts . | ELECTROCHEMICAL ENERGY REVIEWS , 2025 , 8 (1) . |
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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. © 2025 American Chemical Society.
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| GB/T 7714 | Li, J. , Zhao, J. , Wang, S. 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 . |
| MLA | Li, J. et al. "Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane" . | Journal of the American Chemical Society (2025) . |
| APA | Li, J. , Zhao, J. , Wang, S. , Peng, K.-S. , Su, B. , Liu, K. et al. Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane . | Journal of the American Chemical Society , 2025 . |
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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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Semihydrogenation is a crucial industrial process. Noble metals such as Pd have been extensively studied in semihydrogenation reactions, owing to their unique catalytic activity toward hydrogen activation. However, the overhydrogenation of alkenes to alkanes often happens due to the rather strong adsorption of alkenes on Pd active phases. Herein, we demonstrate that the incorporation of Pd active phases as single-atom sites in perovskite lattices such as SrTiO3 can greatly alternate the electronic structure and coordination environment of Pd active phases to facilitate the desorption of alkenes rather than further hydrogenation. Furthermore, the incorporated Pd sites can be well stabilized without sintering by a strong host-guest interaction with SrTiO3 during the activation of H species in hydrogenation reactions. As a result, the Pd incorporated SrTiO3 (Pd-SrTiO3) exhibits an excellent time-independent selectivity (>99.9 %) and robust durability for the photocatalytic semihydrogenation of phenylacetylene to styrene. This strategy based on incorporation of active phases in perovskite lattices will have broad implications in the development of high-performance photocatalysts for selective hydrogenation reactions.
Keyword ：
Metal-substituted perovskites Metal-substituted perovskites Pd single sites Pd single sites Photocatalysis Photocatalysis Semihydrogenation Semihydrogenation SrTiO3 SrTiO3
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| GB/T 7714 | Yang, Baoying , Liu, Kunlong , Ma, Yuhui et al. Incorporation of Pd Single-Atom Sites in Perovskite with an Excellent Selectivity toward Photocatalytic Semihydrogenation of Alkynes [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (42) . |
| MLA | Yang, Baoying et al. "Incorporation of Pd Single-Atom Sites in Perovskite with an Excellent Selectivity toward Photocatalytic Semihydrogenation of Alkynes" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 42 (2024) . |
| APA | Yang, Baoying , Liu, Kunlong , Ma, Yuhui , Ma, Jian-Jie , Chen, Yi-Yu , Huang, Meirong et al. Incorporation of Pd Single-Atom Sites in Perovskite with an Excellent Selectivity toward Photocatalytic Semihydrogenation of Alkynes . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (42) . |
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The photocatalytic selective oxidation of CH4 to value-added higher hydrocarbons presents a promising avenue for the sustainable development of the chemical industry; however, the mild activation and conversion of CH4 remain great challenges. Herein, a novel Au/Zn2Ti3O8 hybrid photocatalyst is assembled from supporting Au nanoparticles (NPs) on the surface of Zn2Ti3O8 nanospheres. The Zn2Ti3O8 semiconductor with Zn2+ active sites drives the CH4 coupling reaction, while the Au NPs promote the separation and migration of charge carriers. When irradiated with a 365 LED light, the 1.0%-Au/Zn2Ti3O8 catalyst exhibits high activity and stability for selective CH4 coupling with O-2, affording an optimal C2H6 yield of 609.49 mu mol g(-1) h(-1) with 80.18% selectivity, which is among the state-of-the-art values under comparable conditions. Besides, the 1.0%-Au/Zn2Ti3O8 sample affords a turnover number (TON) of 239.1 and an apparent quantum efficiency (AQE) of 1.05% at 365 nm. Studies reveal that the Schottky junction interface strongly promotes photoinduced electrons to be transferred to Au from Zn2Ti3O8, realizing directed separation and migration of charge carriers for high photocatalytic activity. Various in situ spectroscopy analyses expose that the key (CH3)-C-center dot species in CH4-to-C2H6 conversion are stabilized by the surface Au sites for the subsequent coupling reaction to form C2H6, which prevents the undesirable overoxidation reaction to afford high C2H6 selectivity. A possible photocatalytic oxidative CH4 coupling mechanism over the Au/Zn2Ti3O8 hybrid is also proposed.
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| GB/T 7714 | Huang, Qiuying , Cai, Junjian , Wei, Fen et al. Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (32) : 21334-21340 . |
| MLA | Huang, Qiuying et al. "Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions" . | JOURNAL OF MATERIALS CHEMISTRY A 12 . 32 (2024) : 21334-21340 . |
| APA | Huang, Qiuying , Cai, Junjian , Wei, Fen , Fan, Yaming , Liang, Zheng , Liu, Kunlong et al. Selective oxidative coupling of methane to ethane with oxygen using an Au/Zn2Ti3O8 photocatalyst under mild conditions . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (32) , 21334-21340 . |
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The catalytic conversion of methane into value-added products under mild reaction conditions presents a key challenge in heterogeneous catalysis. In this study, we investigate the conversion of methane to acetic acid (CH3COOH) and other methyl oxygenates by using molecule CO as the promoter on Ir/ZSM-5 catalyst. An optimum space-time yield of 7.4 mmol center dot gcat- 1 center dot h- 1 to acetic acid was achieved under mild conditions (2.5 MPa CH4, 2.5 MPa CO, 80 degrees C). The influence of CO on methane conversion was investigated across various transition metals. Ir, Fe, Rh, and Pd showed promotion towards oxygenated compound formation, while Cu and Cr exhibited inhibition. Sequential charging of CH4 and CO experiments reveal the critical role of CO in acetic acid production. Furthermore, the role of CO was further investigated by in situ Raman, in-situ FTIR and EPR. This work shows the role of CO in mild conversion of CH4 to CH3COOH on Ir catalyst.
Keyword ：
Acetic acid Acetic acid Carbon monoxide Carbon monoxide C-H bond C-H bond Iridium Iridium Methane Methane Zeolite Zeolite
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| GB/T 7714 | Liu, Bo , Xiang, Chunyan , Yang, Junye et al. The promoting role of carbon monoxide in mild conversion of methane to acetic acid on atomically dispersed Ir catalyst anchored in ZSM-5 [J]. | JOURNAL OF CATALYSIS , 2024 , 438 . |
| MLA | Liu, Bo et al. "The promoting role of carbon monoxide in mild conversion of methane to acetic acid on atomically dispersed Ir catalyst anchored in ZSM-5" . | JOURNAL OF CATALYSIS 438 (2024) . |
| APA | Liu, Bo , Xiang, Chunyan , Yang, Junye , Sun, Ping , Yang, Yaxin , Xu, Yuanjie et al. The promoting role of carbon monoxide in mild conversion of methane to acetic acid on atomically dispersed Ir catalyst anchored in ZSM-5 . | JOURNAL OF CATALYSIS , 2024 , 438 . |
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