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学者姓名:黄彩进
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Achieving a higher quantum yield remains an ongoing pursuit in the field of solar energy conversion. Recently, more and more studies have shown that the apparent quantum yield (AQY) of photocatalysts becomes unusually high, exceeding 90 % and even reaching 99.2 %. These studies lead us to inquire question whether the AQY of photocatalysis can break through the theoretical upper limit of 100 %. Herein, we chose the photocatalytic H2 production of Cd0.5Zn0.5S as a probe reaction and systematically investigated the effect of incident wavelength, light intensity, and reaction temperature on AQY. Our findings reveal that the AQY can exceed 100 % and even reach 247.3 % at higher temperatures when the incident light energy is greater than the bandgap of photocatalyst but less than 1.5 times. Finally, by combining experimental results and theoretical calculations, we propose a possible photo-thermal synergistic impact ionization model: Collisions of photoexcited electrons and thermal-activated electrons to produce more free electrons for catalysis.
Keyword :
AQY AQY Collision Collision High kinetic energy electron High kinetic energy electron Photocatalysis Photocatalysis Photo-thermal Photo-thermal
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GB/T 7714 | Wang, Chenyi , Ge, Baoxin , Jiang, Pengyang et al. Photocatalytic apparent quantum yield exceeding 100% achieved by photo-thermal synergistic impact ionization [J]. | APPLIED SURFACE SCIENCE , 2025 , 690 . |
MLA | Wang, Chenyi et al. "Photocatalytic apparent quantum yield exceeding 100% achieved by photo-thermal synergistic impact ionization" . | APPLIED SURFACE SCIENCE 690 (2025) . |
APA | Wang, Chenyi , Ge, Baoxin , Jiang, Pengyang , Xu, Fangjie , Cheng, Chuchu , Huang, Caijin . Photocatalytic apparent quantum yield exceeding 100% achieved by photo-thermal synergistic impact ionization . | APPLIED SURFACE SCIENCE , 2025 , 690 . |
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The imbalance between electrophilic and nucleophilic components within Mott-Schottky (M-S) electrocatalysts hinders oxygen reduction/evolution reactions (ORR/OER). We developed an innovative Co/Co3O4-NCF M-S catalyst guided by density functional theory (DFT). By precisely screening nucleophilic and electrophilic components, Co/Co3O4-NCF displays efficient catalysis activity of ORR (E 1/2 = 0.85 V) and OER (eta 10 = 320 mV). Experiments and DFT analyses revealed that strong interfacial interactions in Co/Co3O4-NCF cause harmonized integration of nucleophilic Co and electrophilic Co3O4 dual sites, which optimizes antibonding state occupancy of Co sites. Nucleophilic Co sites facilitate *OH intermediate desorption during ORR, while electrophilic Co3O4 sites accelerate *OOH intermediate dissociation in OER, achieving exceptional ORR/OER activity. Furthermore, Co/Co3O4-NCF demonstrates satisfactory cell performances as cathodes for flexible Zn-air batteries (FZABs) even under extreme conditions (-18 to 60 degrees C), promoting the application of FZABs. This work provides new insight into designing efficient M-S catalysts by integrating balanced electrophilic and nucleophilic sites.
Keyword :
Electrophilicity Electrophilicity FZABs FZABs Mott-Schottky Mott-Schottky Nucleophilicity Nucleophilicity OER OER ORR ORR
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GB/T 7714 | Jiang, Pengyang , Ge, Baoxin , Cheng, Chuchu et al. Balancing electrophilic and nucleophilic dual sites to construct efficient Mott-Schottky oxygen electrocatalysts [J]. | CHEMICAL ENGINEERING SCIENCE , 2025 , 306 . |
MLA | Jiang, Pengyang et al. "Balancing electrophilic and nucleophilic dual sites to construct efficient Mott-Schottky oxygen electrocatalysts" . | CHEMICAL ENGINEERING SCIENCE 306 (2025) . |
APA | Jiang, Pengyang , Ge, Baoxin , Cheng, Chuchu , Huang, Caijin . Balancing electrophilic and nucleophilic dual sites to construct efficient Mott-Schottky oxygen electrocatalysts . | CHEMICAL ENGINEERING SCIENCE , 2025 , 306 . |
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Random diffusion of electrons and holes aggravates rapid charge recombination and limits the efficiency of photocatalytic processes. Spin manipulation presents an efficient strategy to regulate charge carrier behavior. Herein, we successfully introduced Cu into sulfur vacancy-rich Mn0.3Cd0.7S (MCS-s), which effectively regulates electron spin polarization and enhances the internal electric field (IEF) within the semiconductor. Through coupling with phosphomolybdic acid hydrate (HPM) to construct Z-scheme heterostructure, we established an efficient pathway for charge carrier migration in the photocatalytic process. DFT calculations and experimental results indicate that sulfur vacancy-induced IEF drives electrons to migrate from the bulk phase to surfacevacancy sites, which accelerates charge carrier transport dynamics for efficient H2 evolution coupled with imine production. Remarkably, the optimized HPM/Cux-MCS-s demonstrated remarkable performance with imine production rates of 15.4 mmol/g/h, along with a high selectivity of 98.0 % towards imine, achieving over 19 times the rate of pristine MCS-s. This work provides new insight into the application of polarized electric field regulation in bifunctional photocatalysts.
Keyword :
Benzylamine oxidation Benzylamine oxidation Internal electric field Internal electric field Photocatalytic Photocatalytic Spin polarization Spin polarization Z -scheme heterostructure Z -scheme heterostructure
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GB/T 7714 | Cheng, Chuchu , Yi, Huimin , Ge, Baoxin et al. Spin polarization modulated Z-scheme heterostructure for efficient photocatalytic H2 evolution coupled with benzylamine oxidation [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 366 . |
MLA | Cheng, Chuchu et al. "Spin polarization modulated Z-scheme heterostructure for efficient photocatalytic H2 evolution coupled with benzylamine oxidation" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 366 (2025) . |
APA | Cheng, Chuchu , Yi, Huimin , Ge, Baoxin , Jiang, Pengyang , Xu, Fangjie , Shi, Wenwen et al. Spin polarization modulated Z-scheme heterostructure for efficient photocatalytic H2 evolution coupled with benzylamine oxidation . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 366 . |
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Achieving a precise understanding and accurate design of heterogeneous catalysts based on bioinspired principles is challenging yet crucial to digging out optimal materials for artificial catalysis. Here, an ADH-mimicking dual-site photocatalyst (YCuCdS) is developed, and demonstrates the powerful effects of atomic site configuration and proton transfer environments on alcohol-amine coupling. Mechanism studies reveal that the alcohol substrate is effectively dehydrogenated at the Y sites, forming the carbonyl intermediates that rapidly experience condensation with the amine. Meanwhile, the released hydrogen species (H-ads) migrate from adjacent Cu sites to active S atoms, promoting H-2 production and hindering the over-hydrogenation of imine. As a result, a high imine yield of 92% is achieved, along with an H-2 production rate of 7400 mu mol g(-1) h(-1). This work showcases an effective strategy for the design of heterogeneous catalysts with bioinspiration.
Keyword :
alcohol-amine coupling alcohol-amine coupling bioinspired catalysis bioinspired catalysis dual sites dual sites enzyme mimicking enzyme mimicking reaction microenvironment reaction microenvironment
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GB/T 7714 | Yi, Huimin , Wang, Chenyi , Ge, Baoxin et al. Engineering Atomic Sites and Proton Transfer Microenvironments for Bioinspired Photocatalytic Alcohol-Amine Coupling [J]. | SMALL , 2025 . |
MLA | Yi, Huimin et al. "Engineering Atomic Sites and Proton Transfer Microenvironments for Bioinspired Photocatalytic Alcohol-Amine Coupling" . | SMALL (2025) . |
APA | Yi, Huimin , Wang, Chenyi , Ge, Baoxin , Xu, Fangjie , Jiang, Pengyang , Zhou, Min et al. Engineering Atomic Sites and Proton Transfer Microenvironments for Bioinspired Photocatalytic Alcohol-Amine Coupling . | SMALL , 2025 . |
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Hybrid conversion Zn-air batteries (HC-ZABs) epitomize a typical integrated energy storage and conversion device that advances green chemistry and reduces carbon emissions. However, balancing efficiency and selectivity of electrocatalytic cathodic reactions remains the bottleneck in such batteries. Herein, we address this issue by designing a high-entropy perovskite, La0.6Sr0.1Ca0.1Rb0.1Y0.1CoO3 (HE-LCO), which outperforms conventional perovskites in offering enhanced electrocatalytic activity, better selectivity, and outstanding stability for cathodic benzyl alcohol oxidation reaction (BAOR). Combined spectroscopy characterizations, operando measurements, and theoretic calculations reveal that the entropy-driven modulation of the second coordination sphere in HE-LCO balances the adsorption of nucleophile benzyl alcohol and OH-, while inhibiting competing oxygen evolution reaction (OER). Based on this rationalized HE-LCO electrocatalyst, HC-ZABs realized efficient energy storage and benzoic acid production, boasting a long lifespan of 900 cycles at 20 mA cm-2 and 6.7 mAh cm-2 per cycle. Further, practical ampere-hour-scale HC-ZABs demonstrated a 62.8% energy efficiency improvement and an average benzoic acid yield of 0.85 g per cycle, highlighting the potential of this integrated device for simultaneous sustainable energy storage and green electrochemical synthesis.
Keyword :
Competitive adsorption Competitive adsorption High-entropy High-entropy Hybrid conversion batteries Hybrid conversion batteries Perovskite electrocatalyst Perovskite electrocatalyst
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GB/T 7714 | Jiang, Pengyang , Xu, Yan , Gong, Zhe et al. Entropy-Driven Competitive Adsorption Sites Tailoring Unlocks Efficient Hybrid Conversion Zn-Air Batteries [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
MLA | Jiang, Pengyang et al. "Entropy-Driven Competitive Adsorption Sites Tailoring Unlocks Efficient Hybrid Conversion Zn-Air Batteries" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025) . |
APA | Jiang, Pengyang , Xu, Yan , Gong, Zhe , Ge, Baoxin , Ding, Luyao , Huang, Caijin et al. Entropy-Driven Competitive Adsorption Sites Tailoring Unlocks Efficient Hybrid Conversion Zn-Air Batteries . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
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The synergetic combination of hydrogen (H2) generation with benzylamine (BA) dehydrogenation shows promise in terms of avoiding sacrificial agents and emitting pollutants without using up unlimited solar energy. However, the rational design of the electron transfer bridge and active sites of photocatalysts remains constrained, reducing the effectiveness of the target selective photocatalytic BA dehydrogenation coupling (PBDC) system. Herein, a bimetallic CuCo nanoparticles used as an efficient cocatalyst is coated on the Mn0.3Cd0.7S (MCS) nanorods (CuCo/MCS) that endows an optimal electronic structure, a directional electron transport tunnel, and suitable reactive sites for the PBDC reaction. Theoretical and experimental studies reveal that the synergistic effect of Cu and Co nanoparticles lowers the overall energy barrier of BA, facilitating the N-benzy-lidenebenzylamine (NBBA) and H-2 generation. The incorporation of CuCo nanoparticles as cocatalysts into MCS not only reduces the overpotential of proton reduction but also weakens the adsorption of imine, thus producing H2 at a rate of 14.10 mmol g(-1) h(-1), with a BA conversion of 94.43 % and selectivity of 99 %. This work will offer a profound understanding of bimetal-anchored photocatalysts in electron transfer for synergetic renewable fuels and valuable chemical production.
Keyword :
CuCo cocatalysts CuCo cocatalysts H2 evolution H2 evolution Mn0.3Cd0.7S Mn0.3Cd0.7S Photocatalysis Photocatalysis Selective imines synthesis Selective imines synthesis
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GB/T 7714 | Lu, Mei , Ge, Baoxin , Xu, Fangjie et al. Encapsulating bimetallic nanoparticles on Mn0.3Cd0.7S solid solution for boosted photocatalytic selective imines synthesis [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 692 . |
MLA | Lu, Mei et al. "Encapsulating bimetallic nanoparticles on Mn0.3Cd0.7S solid solution for boosted photocatalytic selective imines synthesis" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 692 (2025) . |
APA | Lu, Mei , Ge, Baoxin , Xu, Fangjie , Zhou, Min , Xing, Fangsu , Huang, Caijin . Encapsulating bimetallic nanoparticles on Mn0.3Cd0.7S solid solution for boosted photocatalytic selective imines synthesis . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 692 . |
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Sluggish hole transfer and the resulting pronounced charge recombination hinder the efficiency of photocatalytic overall water splitting. Herein, we present Si quantum dots (SiQDs) as hole transporter to construct SiQDs/Cu-doped ZnIn2S4 heterojunction photocatalysts (Cu0.48SZ) for overall water splitting. Under visible light illumination, Cu0.48SZ exhibits highly stable overall water-splitting activity of 210 μmol g−1 h−1 H2 and 97 μmol g−1 h−1 O2 with an apparent quantum yield (AQY) of 2.57 % at 420 nm. Results demonstrate that the synergy of SiQDs and Cu doping enhances carrier-separation efficiency and reduce surface kinetic barriers, leading to high photocatalytic performance. The presence of SiQDs effectively accelerates the transfer of photoexcited holes and avoids the self-oxidation of ZnIn2S4, favoring water oxidation. The Cu doping increases the electron density around the S atoms of ZnIn2S4 and thus promotes water reduction. This work extends the application of SiQDS as efficient hole transporter for photocatalytic overall water splitting. © 2024 Elsevier B.V.
Keyword :
Copper Copper Efficiency Efficiency Heterojunctions Heterojunctions Indium compounds Indium compounds Photocatalytic activity Photocatalytic activity Semiconductor quantum dots Semiconductor quantum dots Silicon Silicon Silicon compounds Silicon compounds Zinc compounds Zinc compounds
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GB/T 7714 | Shi, Wenwen , Ge, Baoxin , Jiang, Pengyang et al. SiQDs-mediated highly efficient hole transfer for photocatalytic overall water splitting over Cu-doped ZnIn2S4 [J]. | Applied Catalysis B: Environmental , 2024 , 354 . |
MLA | Shi, Wenwen et al. "SiQDs-mediated highly efficient hole transfer for photocatalytic overall water splitting over Cu-doped ZnIn2S4" . | Applied Catalysis B: Environmental 354 (2024) . |
APA | Shi, Wenwen , Ge, Baoxin , Jiang, Pengyang , Wang, Qiaoyun , He, Lifeng , Huang, Caijin . SiQDs-mediated highly efficient hole transfer for photocatalytic overall water splitting over Cu-doped ZnIn2S4 . | Applied Catalysis B: Environmental , 2024 , 354 . |
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Interfacial charge-transfer efficiency determines the photoelectrochemical (PEC) performance of Fe2O3-based heterojunction photoanodes. Herein, we present Fe2O3 nanoarrays coated by CoFe bimetal organic framework (CoFe-MOF) nanolayers (CoFe-MOF/F) via in-situ solvothermal method. The resulting CoFe-MOF/F photoanode has a current density of 2.2 mA cm- 2 at 1.23 V vs. RHE, which is about 2.2 times that of pristine Fe2O3. Moreover, the CoFe-MOF/F photoanode shows a negative shift of onset potential, and excellent long-term PEC stability. The in-situ synthesized CoFe-MOF on the photoanode surface enhances the interaction force between the photoanode and the photoanode and strengthen the interface binding, therefore, the interface defects are reduced and the transfer efficiency of interfacial carriers increases, wich effectively improve the performance of the photoanode. This work provides an in- situ strategy for enhancing the binding force between the cocatalyst and the photoanode to improve the PEC performance of the photoelectrode. This approach is not only effective but also scalable, offering the prospect of optimizing the performance of a wide range of photoanode materials.
Keyword :
Hematite Hematite Heterojunction Heterojunction Interfacial binding Interfacial binding
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GB/T 7714 | Li, Zhijie , Yi, Huimin , Jiang, Pengyang et al. Interfacial binding-enhanced charge transport for CoFe-MOF/Fe2O3 photoanodes with excellent PEC performance [J]. | APPLIED SURFACE SCIENCE , 2024 , 681 . |
MLA | Li, Zhijie et al. "Interfacial binding-enhanced charge transport for CoFe-MOF/Fe2O3 photoanodes with excellent PEC performance" . | APPLIED SURFACE SCIENCE 681 (2024) . |
APA | Li, Zhijie , Yi, Huimin , Jiang, Pengyang , Ge, Baoxin , Huang, Caijin . Interfacial binding-enhanced charge transport for CoFe-MOF/Fe2O3 photoanodes with excellent PEC performance . | APPLIED SURFACE SCIENCE , 2024 , 681 . |
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Sluggish hole transfer and the resulting pronounced charge recombination hinder the efficiency of photocatalytic overall water splitting. Herein, we present Si quantum dots (SiQDs) as hole transporter to construct SiQDs/Cu-doped ZnIn2S4 heterojunction photocatalysts (Cu(0.48)SZ) for overall water splitting. Under visible light illumination, Cu0.48SZ exhibits highly stable overall water-splitting activity of 210 mu mol g(-1) h(-1) H-2 and 97 mu mol g(-1) h(-1) O-2 with an apparent quantum yield (AQY) of 2.57 % at 420 nm. Results demonstrate that the synergy of SiQDs and Cu doping enhances carrier-separation efficiency and reduce surface kinetic barriers, leading to high photocatalytic performance. The presence of SiQDs effectively accelerates the transfer of photoexcited holes and avoids the self-oxidation of ZnIn2S4, favoring water oxidation. The Cu doping increases the electron density around the S atoms of ZnIn2S4 and thus promotes water reduction. This work extends the application of SiQDS as efficient hole transporter for photocatalytic overall water splitting.
Keyword :
Hole transfer Hole transfer Photocatalytic overall water splitting Photocatalytic overall water splitting SiQDs SiQDs ZnIn2S4 ZnIn2S4
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GB/T 7714 | Shi, Wenwen , Ge, Baoxin , Jiang, Pengyang et al. SiQDs-mediated highly efficient hole transfer for photocatalytic overall water splitting over Cu-doped ZnIn2S4 [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 354 . |
MLA | Shi, Wenwen et al. "SiQDs-mediated highly efficient hole transfer for photocatalytic overall water splitting over Cu-doped ZnIn2S4" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 354 (2024) . |
APA | Shi, Wenwen , Ge, Baoxin , Jiang, Pengyang , Wang, Qiaoyun , He, Lifeng , Huang, Caijin . SiQDs-mediated highly efficient hole transfer for photocatalytic overall water splitting over Cu-doped ZnIn2S4 . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 354 . |
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The orbital hybridization between metal and oxygen of perovskite catalysts can lower the overpotential and enhance the oxygen evolution reaction (OER) activity. This study combines density functional theory with experiments to clarify how Sr/Fe codoping modulates orbital hybridization and enhances OER catalytic activity of LaCoO3. The as-prepared La0.50Sr0.50Co0.75Fe0.25O3 shows remarkable performance with a low overpotential of 310 mV at 10 mA cm(-2) current density and a 107.03 mV dec(-1) Tafel slope, outperforming most state-of-the-art perovskite-based OER electrocatalysts. The experimental results confirm that Sr/Fe codoping enhances the expansion of Co-O-Co bond angles and strengthens the covalency of the Co-O bond in LaCoO3, leading to enhanced electrocatalytic activity. Moreover, increasing Sr doping reduces the distance between the Co 3d/O 2p center and the Fermi level, decreasing the energy difference between them and enhancing the degree of orbital hybridization between Co 3d and O 2p. As the degree of Co 3d/O 2p orbital hybridization increases, a higher charge transfer was found between the active center and intermediate product, OOH, reducing the energy barrier of the rate-determining step while lowering the overpotential. This study provides thorough insight into the rational design of OER catalysts based on orbital hybridization.
Keyword :
Co 3d/O 2p orbital hybridization Co 3d/O 2p orbital hybridization Co-O-Cobond angle Co-O-Cobond angle DFT prediction DFT prediction LaCoO3 LaCoO3 oxygenevolution reaction oxygenevolution reaction Zn-air batteries Zn-air batteries
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GB/T 7714 | Ge, Baoxin , Jiang, Pengyang , Chen, Biyi et al. Controlling Co 3d/O 2p Orbital Hybridization in LaCoO3 by Modulating the Co-O-Co Bond Angle for Enhanced Oxygen Evolution Reaction Catalysis [J]. | ACS CATALYSIS , 2024 , 15 (1) : 477-486 . |
MLA | Ge, Baoxin et al. "Controlling Co 3d/O 2p Orbital Hybridization in LaCoO3 by Modulating the Co-O-Co Bond Angle for Enhanced Oxygen Evolution Reaction Catalysis" . | ACS CATALYSIS 15 . 1 (2024) : 477-486 . |
APA | Ge, Baoxin , Jiang, Pengyang , Chen, Biyi , Huang, Caijin . Controlling Co 3d/O 2p Orbital Hybridization in LaCoO3 by Modulating the Co-O-Co Bond Angle for Enhanced Oxygen Evolution Reaction Catalysis . | ACS CATALYSIS , 2024 , 15 (1) , 477-486 . |
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