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学者姓名：王心晨
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Abstract ：
Photocatalysts with abundant oxygen vacancies (OVs) exhibit enhanced activity for the direct oxidation of benzene to phenol with O2, owing to their superior O2 activation and charge separation properties. However, OVs on metal oxide surfaces such as WO3 are susceptible to healing by oxygen-containing reactants or intermediates, leading to their irreversible deactivation. Herein, we demonstrate that incorporating Mo into the WO3 lattice effectively lowers the energy barrier for OV formation, promoting the dynamic formation of more abundant photoinduced OVs in situ on the surface during the photocatalytic reaction. These Mo-promoted photoinduced OVs are found to ensure the long-term sustainability of sufficient OVs under working conditions, enhancing photocatalytic performance and particularly its durability in the aerobic oxidation of benzene to phenol. These findings provide a straightforward strategy to overcome the issue of OV healing, enabling the sustainable operation of OV-rich photocatalysts for a range of emerging applications, even in O2-involved redox reactions.
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| GB/T 7714 | Yu, Zhenzhen , Yu, Dexi , Wang, Xiaoyi et al. Photoinduced Formation of Oxygen Vacancies on Mo-Incorporated WO3 for Direct Oxidation of Benzene to Phenol by Air [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (16) : 13885-13892 . |
| MLA | Yu, Zhenzhen et al. "Photoinduced Formation of Oxygen Vacancies on Mo-Incorporated WO3 for Direct Oxidation of Benzene to Phenol by Air" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 16 (2025) : 13885-13892 . |
| APA | Yu, Zhenzhen , Yu, Dexi , Wang, Xiaoyi , Huang, Meirong , Hou, Yidong , Lin, Wei et al. Photoinduced Formation of Oxygen Vacancies on Mo-Incorporated WO3 for Direct Oxidation of Benzene to Phenol by Air . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (16) , 13885-13892 . |
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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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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 nitride (PCN) photocatalysts have the potential to remove NO from ambient air. However, the catalytic performance of PCN is limited by the lack of sufficient active sites to effectively activate molecular oxygen. Herein, we report the construction of photocatalysts consisting of defective-activated-carbon and PCN via amide bond formation. This photocatalyst not only significantly enhances the chemisorption of O-2, but also accelerates the activation of molecular oxygen and oxidation of NO by creating a new electron transport pathway. This work provides a new strategy for polymer photocatalysts to promote molecular oxygen activation by constructing close-contact interfaces through amide bonding.
Keyword ：
Amide bonding Amide bonding Molecular oxygen activation Molecular oxygen activation NO oxidation NO oxidation Photocatalysis Photocatalysis Polymeric carbon nitride Polymeric carbon nitride
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| GB/T 7714 | Fang, Zixun , Zhou, Min , Lin, Zheng et al. Amide bonded polymeric carbon nitride for photocatalytic O2 activation and NO oxidation [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 353 . |
| MLA | Fang, Zixun et al. "Amide bonded polymeric carbon nitride for photocatalytic O2 activation and NO oxidation" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 353 (2024) . |
| APA | Fang, Zixun , Zhou, Min , Lin, Zheng , Yang, Can , Hou, Yidong , Yu, Jimmy C. et al. Amide bonded polymeric carbon nitride for photocatalytic O2 activation and NO oxidation . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 353 . |
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Sp(2)-carbon-conjugated covalent organic frameworks (sp(2)c-COFs) have emerged as promising platforms for phototo-chemical energy conversion due to their tailorable optoelectronic properties, in-plane pi-conjugations, and robust structures. However, the development of sp(2)c-COFs in photocatalysis is still highly hindered by their limited linkage chemistry. Herein, we report a novel thiadiazole-bridged sp(2)c-COF (sp(2)c-COF-ST) synthesized by thiadiazole-mediated aldol-type polycondensation. The resultant sp(2)c-COF-ST demonstrates high chemical stability under strong acids and bases (12 M HCl or 12 M NaOH). The electro-deficient thiadiazole together with fully conjugated and planar skeleton endows sp(2)c-COF-ST with superior photoelectrochemical performance and charge-carrier separation and migration ability. As a result, when employed as a photocathode, sp(2)c-COF-ST exhibits a significant photocurrent up to similar to 14.5 mu A cm(-2) at 0.3 V vs reversible hydrogen electrode (RHE) under visible-light irradiation (>420 nm), which is much higher than those analogous COFs with partial imine linkages (mix-COF-SNT similar to 9.5 mu A cm(-2)) and full imine linkages (imi-COF-SNNT similar to 4.9 mu A cm(-2)), emphasizing the importance of the structure-property relationships. Further temperature-dependent photoluminescence spectra and density functional theory calculations demonstrate that the sp(2)c-COF-ST has smaller exciton binding energy as well as effective mass in comparison to mix-COF-SNT and imi-COF-SNNT, which suggests that the sp(2)c-conjugated skeleton enhances the exciton dissociation and carrier migration under light irradiation. This work highlights the design and preparation of thiadiazole-bridged sp(2)c-COFs with promising photocatalytic performance.
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| GB/T 7714 | Fu, Guangen , Yang, Denghui , Xu, Shunqi et al. Construction of Thiadiazole-Bridged sp2-Carbon-Conjugated Covalent Organic Frameworks with Diminished Excitation Binding Energy Toward Superior Photocatalysis [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (2) : 1318-1325 . |
| MLA | Fu, Guangen et al. "Construction of Thiadiazole-Bridged sp2-Carbon-Conjugated Covalent Organic Frameworks with Diminished Excitation Binding Energy Toward Superior Photocatalysis" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146 . 2 (2024) : 1318-1325 . |
| APA | Fu, Guangen , Yang, Denghui , Xu, Shunqi , Li, Shengxu , Zhao, Yuxiang , Yang, Haoyong et al. Construction of Thiadiazole-Bridged sp2-Carbon-Conjugated Covalent Organic Frameworks with Diminished Excitation Binding Energy Toward Superior Photocatalysis . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2024 , 146 (2) , 1318-1325 . |
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Over the past half-century, significant efforts have been dedicated to the photocatalytic H2 production from H2O under UV–visible light irradiation. These endeavors have yielded remarkable results, with efficiency levels now approaching near 100 % apparent quantum yields, notably utilizing inorganic semiconducting materials such as modified Al-doped SrTiO3 photocatalysts. Meanwhile, advancements in organic polymer semiconducting materials, exemplified by g-C3N4, have led to substantial improvements in the efficiency of photocatalytic overall water splitting for H2 evolution reaction. These improvements, achieved through chemical engineering methods and molecular-level modifications, have resulted in an apparent quantum yield of 69 % at 405 nm, accompanied by significant red-shifting of optical absorption to 1400 nm. These developments are presented in chronological order over the past half-century, underscoring the ongoing quest for innovative breakthroughs to enable large-scale practical applications of solar hydrogen production. Key considerations in this pursuit include efficiency, stability, cost-effectiveness, and the independent evolution of H2 and O2. © 2024 Chongqing University
Keyword ：
g-C3N4 g-C3N4 Inorganic semiconducting material Inorganic semiconducting material Organic polymer semiconducting material Organic polymer semiconducting material Photocatalytic hydrogen production Photocatalytic hydrogen production TiO2 TiO2 Titanate Titanate
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| GB/T 7714 | Su, J. , Zhang, J. , Chai, S. et al. Developments of photocatalytic overall water splitting to produce H2 [J]. | Nano Materials Science , 2024 . |
| MLA | Su, J. et al. "Developments of photocatalytic overall water splitting to produce H2" . | Nano Materials Science (2024) . |
| APA | Su, J. , Zhang, J. , Chai, S. , Anpo, M. , Fang, Y. , Wang, X. . Developments of photocatalytic overall water splitting to produce H2 . | Nano Materials Science , 2024 . |
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Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene produc-tion but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficient EDH by solar energy remains a giant challenge.Herein,we present that an oxygen va-cancy(Ov)-rich LaVO4(LaV04-Ov)catalyst is highly active and stable for photocatalytic EDH,through a dynamic lattice oxygen(Olatt.)and Ov co-mediated mechanism.Irradiated by simulated sunlight at mild conditions,LaVO4-Ov effectively dehydrogenates undiluted ethane to produce C2H4 and CO with a con-version of 2.3％.By loading a small amount of Pt cocatalyst,the evolution and selectivity of C2H4 are en-hanced to 275 μmol h-1 g-1 and 96.8％.Of note,LaVO4-Ov appears nearly no carbon deposition after the reaction.The isotope tracked reactions reveal that the consumed Olatt.recuperates by exposing the used catalyst with O2,thus establishing a dynamic cycle of Olatt,and achieving a facile catalyst regeneration to preserve its intrinsic activity.The refreshed LaVO4-Ov exhibits superior reusability and delivers a turnover number of about 305.The Ov promotes photo absorption,boosts ethane adsorption/activation,and accel-erates charge separation/transfer,thus improving the photocatalytic efficiency.The possible photocatalytic EDH mechanism is proposed,considering the key intermediates predicted by density functional theory(DFT)and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).
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| GB/T 7714 | Fen Wei , Weichao Xue , Zhiyang Yu et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst [J]. | 中国化学快报（英文版） , 2024 , 35 (3) : 171-176 . |
| MLA | Fen Wei et al. "Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst" . | 中国化学快报（英文版） 35 . 3 (2024) : 171-176 . |
| APA | Fen Wei , Weichao Xue , Zhiyang Yu , Xue Feng Lu , Sibo Wang , Wei Lin et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst . | 中国化学快报（英文版） , 2024 , 35 (3) , 171-176 . |
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Photocatalytic hydrogen production based on noble metal-free systems is a promising technology for the conversion of solar energy into green hydrogen, it is pivotal and challenging to tailor-make photocatalysts for achieving high photocatalytic efficiency. Herein, we reported a hollow double-shell dyad through uniformly coating covalent organic frameworks (COFs) on the surface of hollow Co9S8. The double shell architecture enhances the scattering and refraction efficiency of incident light, shortens the transmission distance of the photogenerated charge carriers, and exposes more active sites for photocatalytic conversion. The hydrogen evolution rate is as high as 23.15 mmol g-1 h-1, which is significantly enhanced when compared with that of their physical mixture (0.30 mmol g-1 h-1) and Pt-based counterpart (11.84 mmol g-1 h-1). This work provides a rational approach to the construction of noble-metal-free photocatalytic systems based on COFs to enhance hydrogen evolution performance. Hollow double-shell dyads have been constructed using covalent organic frameworks and transition metal sulfides, the double-shell architecture broadens light absorption, improves hydrogen evolution kinetics and reduces the photogenerated electron transfer resistance, resulting in high performance in photocatalytic hydrogen evolution reaction. image
Keyword ：
Covalent organic frameworks Covalent organic frameworks Dyad Dyad Hollow structure Hollow structure Hydrogen generation Hydrogen generation Photocatalysis Photocatalysis
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| GB/T 7714 | Wang, Meiying , Lv, Haowei , Dong, Beibei et al. Photoelectron Migration Boosted by Hollow Double-Shell Dyads Based on Covalent Organic Frameworks for Highly Efficient Photocatalytic Hydrogen Generation [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (17) . |
| MLA | Wang, Meiying et al. "Photoelectron Migration Boosted by Hollow Double-Shell Dyads Based on Covalent Organic Frameworks for Highly Efficient Photocatalytic Hydrogen Generation" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 17 (2024) . |
| APA | Wang, Meiying , Lv, Haowei , Dong, Beibei , He, Wenhao , Yuan, Daqiang , Wang, Xinchen et al. Photoelectron Migration Boosted by Hollow Double-Shell Dyads Based on Covalent Organic Frameworks for Highly Efficient Photocatalytic Hydrogen Generation . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (17) . |
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The integration of heterogeneous photocatalysts with nickel catalysis is garnering considerable interest for their capacity to enable distinct metal-photoredox processes for organic synthesis. However, the challenge about robustness and recyclability of the photocatalyst persists. Herein, a crystalline carbon nitride (MCN-B) photocatalyst with intentionally introduced defects and a dedicated designed active site has been presented. Results reveal by incorporating the deprotonated cyano-group (N--CN) sites, this host material could provide stable binding sites for Ni (II) ions through the Hard-Soft Acid-Base (HSAB) effect, thereby facilitating charge transmission between semiconductor and metal centers. Consequently, the integrated carbon nitride nickel (Ni/MCNB) heterogeneous photocatalyst demonstrates high effectiveness in diverse photocatalytic C-N coupling reactions (21 examples, up to 93% yield) under conditions free from organic ligands and additives, which shows competent performance to the homogeneous catalysts. Moreover, the Ni/MCN-B catalyst demonstrates remarkable recyclability, maintaining its photoredox efficiency after 10 cycles with minimal loss of activity and a diminished metal leaching rate, which signifies a substantial advancement in the field of photocatalytic system design.
Keyword ：
Carbon nitride Carbon nitride Cross-coupling Cross-coupling Crystalline polymer Crystalline polymer Photocatalysis Photocatalysis
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| GB/T 7714 | Zhang, Huali , Chen, Xiaoxiao , Cheng, Jiajia et al. Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst [J]. | JOURNAL OF CATALYSIS , 2024 , 433 . |
| MLA | Zhang, Huali et al. "Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst" . | JOURNAL OF CATALYSIS 433 (2024) . |
| APA | Zhang, Huali , Chen, Xiaoxiao , Cheng, Jiajia , Yang, Xintuo , Lin, Wei , Hou, Yidong et al. Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst . | JOURNAL OF CATALYSIS , 2024 , 433 . |
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Photocatalytic synthesis of H2O2 is an advantageous and ecologically sustainable alternative to the conventional anthraquinone process. However, achieving high conversion efficiency without sacrificial agents remains a challenge. In this study, two covalent organic frameworks (COF-O and COF-C) were prepared with identical skeletal structures but with their pore walls anchored to different alkyl chains. They were used to investigate the effect of the chemical microenvironment of pores on photocatalytic H2O2 production. Experimental results reveal a change of hydrophilicity in COF-O, leading to suppressed charge recombination, diminished charge transfer resistance, and accelerated interfacial electron transfer. An apparent quantum yield as high as 10.3 % (lambda=420 nm) can be achieved with H2O and O-2 through oxygen reduction reaction. This is among the highest ever reported for polymer photocatalysts. This study may provide a novel avenue for optimizing photocatalytic activity and selectivity in H2O2 generation.
Keyword ：
Hydrazone-lined covalent organic frameworks Hydrazone-lined covalent organic frameworks Microenvironment modulation Microenvironment modulation Photocatalytic H2O2 production Photocatalytic H2O2 production Selectivity Selectivity
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| GB/T 7714 | Xie, Zhipeng , Chen, Xiong , Wang, Wenbin et al. Variation of Chemical Microenvironment of Pores in Hydrazone-Linked Covalent Organic Frameworks for Photosynthesis of H2O2 [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (39) . |
| MLA | Xie, Zhipeng et al. "Variation of Chemical Microenvironment of Pores in Hydrazone-Linked Covalent Organic Frameworks for Photosynthesis of H2O2" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 39 (2024) . |
| APA | Xie, Zhipeng , Chen, Xiong , Wang, Wenbin , Ke, Xiating , Zhang, Xirui , Wang, Sibo et al. Variation of Chemical Microenvironment of Pores in Hydrazone-Linked Covalent Organic Frameworks for Photosynthesis of H2O2 . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (39) . |
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