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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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Abstract ：
Photocatalytic oxidation of benzene to phenol using molecular O2 is one of the most promising sustainable approaches for the green synthesis of phenol. Introducing oxygen vacancies (OVs) on semiconductor surfaces by defect engineering is a promising strategy to enhance the efficiency of benzene oxidation to produce phenol due to the unique functions of OVs in facilitating the charge separation and activation of molecular O2. Herein, a vacuum-sealed annealing strategy has been well developed to generate abundant surface OVs on semiconductors, such as WO3. The well-sealed quartz vial creates a well-controlled low-pressure condition for the formation of OVs without the need for external energy for maintaining the vacuum state. Moreover, the gaseous species generated during the thermal annealing process help mitigate stress-induced defects, particularly bulk defects. The vacuum-sealed annealed WO3 with sufficient OVs and reduced bulk defects shows a better photocatalytic performance in the one-step oxidation of benzene to phenol with O2, compared to the WO3 synthesized through thermal annealing in Ar and H2 atmospheres. The present vacuum-sealed annealing strategy is found to be further applicable to engineer a wide range of semiconducting photocatalysts with abundant OVs to optimize their properties for efficient photocatalysis and other OV-promoted systems.
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| GB/T 7714 | Yu, Dexi , Lin, Yuhong , Zhou, Wenhui et al. Photocatalytic Oxidation of Benzene to Phenol with O2 over WO3 Treated by Vacuum-Sealed Annealing [J]. | LANGMUIR , 2025 , 41 (6) : 4287-4295 . |
| MLA | Yu, Dexi et al. "Photocatalytic Oxidation of Benzene to Phenol with O2 over WO3 Treated by Vacuum-Sealed Annealing" . | LANGMUIR 41 . 6 (2025) : 4287-4295 . |
| APA | Yu, Dexi , Lin, Yuhong , Zhou, Wenhui , Wang, Xiaoyi , Yu, Zhenzhen , Hou, Yidong et al. Photocatalytic Oxidation of Benzene to Phenol with O2 over WO3 Treated by Vacuum-Sealed Annealing . | LANGMUIR , 2025 , 41 (6) , 4287-4295 . |
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Oxygen vacancies (OVs) spatially confined on the surface of metal oxide semiconductors are advantageous for photocatalysis, in particular, for O2-involved redox reactions. However, the thermal annealing process used to generate surface OVs often results in undesired bulk OVs within the metal oxides. Herein, a high pressure-assisted thermal annealing strategy has been developed for selectively confining desirable amounts of OVs on the surface of metal oxides, such as tungsten oxide (WO3). Applying a pressure of 1.2 gigapascal (GPa) on WO3 induces significant lattice compression, which would strengthen the W-O bonds and increase the diffusion activation energy for the migration of the O migration. This pressure-induced compression effectively inhibits the formation of bulk OVs, resulting in a high density of surface-confined OVs on WO3. These well-defined surface OVs significantly enhance the photocatalytic activation of O2, facilitating H2O2 production and aerobic oxidative coupling of amines. This strategy holds promise for the defect engineering of other metal oxides, enabling abundant surface OVs for a range of emerged applications.
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| GB/T 7714 | Wang, Xiaoyi , Xue, Sikang , Huang, Meirong et al. Pressure-Induced Engineering of Surface Oxygen Vacancies on Metal Oxides for Heterogeneous Photocatalysis [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (6) : 4945-4951 . |
| MLA | Wang, Xiaoyi et al. "Pressure-Induced Engineering of Surface Oxygen Vacancies on Metal Oxides for Heterogeneous Photocatalysis" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 6 (2025) : 4945-4951 . |
| APA | Wang, Xiaoyi , Xue, Sikang , Huang, Meirong , Lin, Wei , Hou, Yidong , Yu, Zhiyang et al. Pressure-Induced Engineering of Surface Oxygen Vacancies on Metal Oxides for Heterogeneous Photocatalysis . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (6) , 4945-4951 . |
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Photocatalytic chemical transformations for green organic synthesis has attracted much interest. However, their development is greatly hampered by the lack of sufficient reactive sites on the photocatalyst surface for the adsorption and activation of substrate molecules. Herein, we demonstrate that the introduction of well-defined Lewis and Br & oslash;nsted acid sites coexisting on the surface of TiO2 (SO42-/N-TiO2) creates abundant active adsorption sites for photoredox reactions. The electron-deficient Lewis acid sites supply coordinatively unsaturated surface sites to adsorb molecular oxygen, and the Br & oslash;nsted acid sites are liable to donate protons to form hydrogen bonds with the OH groups of alcohols like benzyl alcohol (BA). These coexistent acid sites result in a strong synergistic effect in photocatalytic aerobic oxidation of BA. For example, the conversion of BA to benzaldehyde was found to be 88.6 %, being much higher than those of pristine TiO2 (14.7 %), N-doped TiO2 (N-TiO2, 24.6 %), sulfated TiO2 (SO42-/ TiO2, 35.4 %), and even their sum. The apparent quantum efficiency (AQE) was determined to be 58.1 % at 365 nm and 12.9 % at 420 nm over SO42-/N-TiO2. This strategy to create effective synergistic Lewis and Br & oslash;nsted acids on the catalyst surfaces enables us to apply it to other semiconducting photocatalytic organic transformations.
Keyword ：
br & oslash;nsted acids br & oslash;nsted acids heterogeneous catalysis heterogeneous catalysis lewis acids lewis acids oxidation oxidation photocatalysis photocatalysis
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| GB/T 7714 | Yu, Dexi , Zou, Junhua , Zeng, Lingdong et al. Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (15) . |
| MLA | Yu, Dexi et al. "Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 15 (2025) . |
| APA | Yu, Dexi , Zou, Junhua , Zeng, Lingdong , Hou, Yidong , Lin, Wei , Wu, Ling et al. Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (15) . |
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核磁共振技术（NMR）是迄今为止研究最完全、应用范围最广的波谱技术之一，遍及生物、医药、矿物勘探、化学等领域，多位杰出科学家因为NMR研究而获得诺贝尔奖，其中虞福春和他的同事普洛科特（W.G.Proctor）发现了核所处的化学环境会影响核的化学位移这一现象，也被称呼为Proctor-Yu（虞）效应。紧接着虞福春又在KSbF
Keyword ：
Proctor-Yu(虞)效应 Proctor-Yu(虞)效应 化学位移 化学位移 核磁共振 核磁共振 虞福春 虞福春
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| GB/T 7714 | 丁业皓 , 张雅惠 , 陈佳义 et al. 核磁共振技术中的Proctor-Yu(虞)效应 [J]. | 化学教育(中英文) , 2025 , 46 (08) : 127-129 . |
| MLA | 丁业皓 et al. "核磁共振技术中的Proctor-Yu(虞)效应" . | 化学教育(中英文) 46 . 08 (2025) : 127-129 . |
| APA | 丁业皓 , 张雅惠 , 陈佳义 , 王心晨 , 袁耀锋 . 核磁共振技术中的Proctor-Yu(虞)效应 . | 化学教育(中英文) , 2025 , 46 (08) , 127-129 . |
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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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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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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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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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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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