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学者姓名：方元行
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Abstract ：
Photocatalytic water oxidation half-reaction is a critical bottleneck in achieving efficient overall water splitting using polymeric photocatalysts, primarily due to the lack of efficient water oxidation sites and sluggish reaction kinetics. To address these challenges, a doping engineering strategy is proposed to activate inert carbon atoms as efficient water oxidation sites in poly(heptazine imide) (PHI). Computational analysis revealed that Rb+ dopants can induce in-plane structural distortions in PHI, thereby modulating the electronic structure of carbon atoms. This modulation enhanced the adsorption of *OH intermediates on carbon atoms and significantly reduced the reaction barrier for water oxidation. Furthermore, charge carriers dynamics uncovered that the incorporation of the Rb+ ions into the PHI framework can promote the photoexcited exciton dissociation and induce the holes to migrate to the water oxidation sites. As a result, the Rb-doped PHI achieved an excellent apparent quantum efficiency value of up to 20.4% at 400 nm for water oxidation. This finding offers a new channel for researchers to develop highly efficient polymeric photocatalysts for photocatalytic water oxidation reactions.
Keyword ：
carbon nitride carbon nitride doping engineering doping engineering photocatalytic water oxidation photocatalytic water oxidation polymeric photocatalysts polymeric photocatalysts
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| GB/T 7714 | Pan, Zhiming , Zhu, Xingdian , Zhang, Xirui et al. Activating Inert Carbon Atoms in Poly(Heptazine Imide) via Doping Engineering for High-Efficiency Photocatalytic Water Oxidation [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Pan, Zhiming et al. "Activating Inert Carbon Atoms in Poly(Heptazine Imide) via Doping Engineering for High-Efficiency Photocatalytic Water Oxidation" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Pan, Zhiming , Zhu, Xingdian , Zhang, Xirui , Qie, Mingyang , Zhang, Guigang , Fang, Yuanxing . Activating Inert Carbon Atoms in Poly(Heptazine Imide) via Doping Engineering for High-Efficiency Photocatalytic Water Oxidation . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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H2 and O2 evolutions occur simultaneously for conventional particulate photocatalytic overall water splitting (PPOWS), leading to a significant backward reaction and the formation of an explosive H2/O2 gas mixture. This is an issue that must be addressed prior to industrialization of PPOWS. Here, a convenient, cost-effective, and scalable concept is introduced to uncouple hydrogen and oxygen production for PPOWS. Based on this idea, a three-component photocatalyst, Co(5 %)-HPCN/(rGO/Pt), is constructed, consisting of a photoresponsive chip (HPCN), a H2 evolution cocatalyst (rGO/Pt), and a cobalt complex capable of reversibly binding O2 (Co), to achieve the decoupling of PPOWS under alternating UV and visible light irradiations. The asynchronous O2 and H2 evolution strategy have considerable flexibility regarding the photocatalyst structure and light sources suitable for PPOWS.
Keyword ：
carbon nitride chips carbon nitride chips overall water splitting overall water splitting photocatalytic photocatalytic PPOWS decoupling PPOWS decoupling reaction mechanism reaction mechanism
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| GB/T 7714 | Liu, Dan , Xu, Huihui , Shen, Jinni et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
| MLA | Liu, Dan et al. "Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 9 (2025) . |
| APA | Liu, Dan , Xu, Huihui , Shen, Jinni , Wang, Xun , Qiu, Chengwei , Lin, Huaxiang et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
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Poly(heptazine imide) (PHI) is a promising photocatalyst for hydrogen peroxide (H2O2) production; however, enhancing its specific surface area to expose internal active sites and understanding their roles in key mechanistic steps for the H2O2 synthesis remain challenging. Here, we utilized organic cations to exfoliate bulk PHI and fabricate PHI nanosheets for producing H2O2 at a rate of 27.35 mmol g-1 h-1 under simulated solar light irradiation, outperforming most of the reported carbon nitride-based catalysts. Importantly, after 36 h of cyclic accumulation reactions in a self-created spiral flow reactor, the H2O2 concentration stabilized at 2.7 wt.%, close to medical sterilization levels. In situ spectroscopic characterizations and density functional theory calculations revealed that the exfoliation results in molecular reconfiguration of the PHI basal planes, forming the active sites to promote charge separation and electron localization. This new structure also creates midgap states, enabling direct H2O2 production via a one-step, two-electron pathway, bypassing the superoxide radical pathway. Theoretical calculations suggest that the localized electronic structure created by the active sites favors the protonation of adsorbed O2 and stabilizes the *OOH species, which converts to H2O2. This study elucidates and underscores the importance of active-site reconfiguration for efficient photocatalytic oxygen reduction reaction (ORR) pathways.
Keyword ：
Electron transport Electron transport Hydrogen peroxide synthesis Hydrogen peroxide synthesis Ion exchange Ion exchange Photocatalysis Photocatalysis Poly(heptazine imide) nanosheets Poly(heptazine imide) nanosheets
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| GB/T 7714 | Luo, Laiyu , Wu, Qinglong , Wang, Siyu et al. Defective Poly(heptazine imide) Nanosheets for Efficient One-Step Two-Electron Photocatalytic O2 Reduction to Medical-Like H2O2 [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (29) . |
| MLA | Luo, Laiyu et al. "Defective Poly(heptazine imide) Nanosheets for Efficient One-Step Two-Electron Photocatalytic O2 Reduction to Medical-Like H2O2" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 29 (2025) . |
| APA | Luo, Laiyu , Wu, Qinglong , Wang, Siyu , Song, Haojie , Li, Jiaqi , Zhang, Liping et al. Defective Poly(heptazine imide) Nanosheets for Efficient One-Step Two-Electron Photocatalytic O2 Reduction to Medical-Like H2O2 . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (29) . |
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Photo-/electro-catalytic CO2 reduction with H2O to produce fuels and chemicals offers a dual solution to address both environmental and energy challenges. For a long time, catalyst design in this reaction system has primarily focused on optimizing reduction sites to improve the efficiency or guide the reaction pathway of the CO2 reduction half-reaction. However, less attention has been paid to designing activation sites for H2O to modulate the H2O dissociation half-reaction. Impressively, the rate-determining step in overall CO2 reduction is the latter, and it influences the evolution direction and formation energy of carbon-containing intermediates through the proton-coupled electron transfer process. Herein, we summarize the mechanism of the H2O dissociation half-reaction in modulating CO2 reduction performance based on cutting-edge research. These analyses aim to uncover the potential regulatory mechanisms by which H2O activation influences CO2 reduction pathways and conversion efficiency, and to establish a mechanism-structure-performance relationship that can guide the design and development of high-efficiency catalytic materials. A summary of advanced characterization techniques for investigating the dissociation mechanism of H2O is presented. We also discuss the challenges and offer perspectives on the future design of activation sites to improve the performance of photo-/electro-catalytic CO2 reduction.
Keyword ：
H2O oxidation/activation H2O oxidation/activation Proton/electron-feeding Proton/electron-feeding Rate-determining step Rate-determining step Reduction of CO2 Reduction of CO2 Reverse reaction Reverse reaction Water hydrogen bond network Water hydrogen bond network
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| GB/T 7714 | Ma, Minzhi , Fang, Yuanxing , Huang, Zeai et al. Mechanistic Insights Into H2O Dissociation in Overall Photo-/Electro-Catalytic CO2 Reduction [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (19) . |
| MLA | Ma, Minzhi et al. "Mechanistic Insights Into H2O Dissociation in Overall Photo-/Electro-Catalytic CO2 Reduction" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 19 (2025) . |
| APA | Ma, Minzhi , Fang, Yuanxing , Huang, Zeai , Wu, Sixin , He, Weiwei , Ge, Suxiang et al. Mechanistic Insights Into H2O Dissociation in Overall Photo-/Electro-Catalytic CO2 Reduction . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (19) . |
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Abstract ：
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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This study presents a systematic theoretical and experimental investigation aimed at optimizing the photocatalytic oxygen evolution reaction (OER) performance of poly(heptazine imides) containing metal cations (PHI-Ms). Deploying advanced density functional theory (DFT) and time-dependent DFT calculations, time-resolved spectroscopy, and photocatalytic OER measurements, we established key design principles for enhancing the OER activity: (i) favoring Co and Fe cations in the +III oxidation state to improve light-harvesting and reduce the Gibbs free changes; (ii) minimizing the content of K+ co-cations, which negatively affect catalytic performance by increasing the desorption Gibbs free energy of O2 and promoting charge localization; (iii) avoiding high concentrations of metal cation to limit agglomeration and mitigate charge recombination; and (iv) exploring oxygen doping of the PHI layer by substituting N atoms located away from the metal active sites, thereby enhancing charge separation and promoting hole generation. These insights offer valuable design guidelines for the development of PHI-M systems with improved photocatalytic performance, advancing the potential of earth-abundant catalysts for practical water-splitting applications.
Keyword ：
catalytic tests catalytic tests density functional theory (DFT) density functional theory (DFT) metal cation incorporation metal cation incorporation metal oxidation state metal oxidation state oxygen doping oxygen doping oxygen evolution reaction (OER) oxygen evolution reaction (OER) poly(heptazine imides)(PHI) poly(heptazine imides)(PHI)
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| GB/T 7714 | Liu, Shanping , Diez-Cabanes, Valentin , Tong, Haijian et al. Tunability of Carbon Nitrides for Enhanced Photocatalytic Oxygen Evolution Reaction [J]. | ACS CATALYSIS , 2025 , 15 (16) : 13860-13871 . |
| MLA | Liu, Shanping et al. "Tunability of Carbon Nitrides for Enhanced Photocatalytic Oxygen Evolution Reaction" . | ACS CATALYSIS 15 . 16 (2025) : 13860-13871 . |
| APA | Liu, Shanping , Diez-Cabanes, Valentin , Tong, Haijian , Fang, Yuanxing , Antonietti, Markus , Pelicano, Christian Mark et al. Tunability of Carbon Nitrides for Enhanced Photocatalytic Oxygen Evolution Reaction . | ACS CATALYSIS , 2025 , 15 (16) , 13860-13871 . |
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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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Heterogeneous photoelectrocatalysis systems have recently seen significant growth in organic transformations, but are limited by the inherent physicochemical properties of electrode materials. To enhance selectivity in these processes, we propose an innovative advancement in the rational design of photoanodes. Specifically, we incorporated cobalt porphyrin co-catalysts with confined Co sites onto bismuth vanadate films as a photoanode. This photoanode significantly enhances the efficacy of styrene epoxidation, achieving selectivity and conversion rates of 90 % and 99 %, respectively. Notably, the reaction utilizes water as the sole oxygen source, operates at room temperature, and is easily scalable for gram-scale synthesis. The developed photoanode demonstrates robust performance across various alkene substrates. Operando characterizations reveal that during the epoxidation reaction, the confined Co sites within the porphyrin structure catalyze the oxidation of H2O to form Co-O*, serving as critical intermediates that facilitate cyclization reactions via one-electron processes. This study introduces an innovative heterogeneous photoelectrocatalysis strategy with customizable active sites tailored for selective catalytic organic transformations.
Keyword ：
Epoxidation Epoxidation Heterogeneous Heterogeneous Photoelectrocatalysis Photoelectrocatalysis Selectivity Selectivity
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| GB/T 7714 | Wu, Haisu , Wang, Yankun , Huang, Meirong et al. Alkene Epoxidation with Water by Confined Active Co Sites on BiVO4 Photoanodes under Visible Light [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (7) . |
| MLA | Wu, Haisu et al. "Alkene Epoxidation with Water by Confined Active Co Sites on BiVO4 Photoanodes under Visible Light" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 7 (2025) . |
| APA | Wu, Haisu , Wang, Yankun , Huang, Meirong , Cheng, Jiajia , Sa, Baisheng , Fang, Yuanxing et al. Alkene Epoxidation with Water by Confined Active Co Sites on BiVO4 Photoanodes under Visible Light . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (7) . |
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Mesoporous bioactive glasses (MBGs) are gaining recognition in bone tissue engineering for their osteoblast differentiation-inducing properties and customizable structures. However, the challenge of peri-implantitis has hindered their broader application. To address this, double transition metal TiNbCTx MXene acted as near-infrared (NIR) photothermal agent, has been integrated with MBG nanospheres to develop novel multifunctional TiNbCTx/MBG (TNC/MBG) nanocomposites in this work. The results demonstrate that the TNC/MBG composites feature uniform mesoporous spherical MBG nanoparticles on TiNbCTx nanosheets, boasting a significantly enhanced specific surface area of up to 444.74 m(2) g(-1) and a more negative zeta potential than pristine MBG. Importantly, the TNC/MBG nanocomposites can effectively promote apatite formation, as well as the proliferation and viability of MC3T3-E1 cells. Moreover, it is highlighted that the TNC/MBG nanocomposites display remarkable photothermal conversion efficiency and stability, leading to over 95% antibacterial inhibition rates against both S. aureus and E. coli under NIR irradiation. These findings offer an appealing strategy to develop multifunctional TNC/MBG nanocomposites with enhanced biological activity and robust antibacterial properties, which shows great potential for various biomedical applications.
Keyword ：
antibacterial property antibacterial property biological behavior biological behavior mesoporous bioactive glass mesoporous bioactive glass photothermal conversion performance photothermal conversion performance TiNbCTx MXene TiNbCTx MXene
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| GB/T 7714 | Yan, Siqing , Ma, Qian , Wen, Cuilian et al. Enhanced Biological Behavior and Photothermal Antibacterial Performance of TiNbCTx MXene Modified Mesoporous Bioactive Glass Nanocomposites [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (24) . |
| MLA | Yan, Siqing et al. "Enhanced Biological Behavior and Photothermal Antibacterial Performance of TiNbCTx MXene Modified Mesoporous Bioactive Glass Nanocomposites" . | ADVANCED FUNCTIONAL MATERIALS 35 . 24 (2025) . |
| APA | Yan, Siqing , Ma, Qian , Wen, Cuilian , Luo, Lijin , Jin, Junhao , Li, Xiong et al. Enhanced Biological Behavior and Photothermal Antibacterial Performance of TiNbCTx MXene Modified Mesoporous Bioactive Glass Nanocomposites . | ADVANCED FUNCTIONAL MATERIALS , 2025 , 35 (24) . |
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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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