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学者姓名:黄美榕
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The integration of photoelectrochemical (PEC) technology with persulfate-based advanced oxidation processes has emerged as a promising approach for efficient pollutant removal in environmental remediation. Herein, we developed a novel PEC system combining a Co3O4/BiVO4 (CO/BVO) photoanode with a CoFe2O4/carbon paper (CFO/CP) cathode for activating peroxymonosulfate (PMS) toward bisphenol A (BPA) removal. The enhanced photogenerated charge separation in CO/BVO and the PMS activation by CFO/CP in the PEC system enabled complete BPA degradation within 60 minutes under optimized conditions (1.0 V bias, 1.0 mM PMS). The influence of PMS concentration, applied bias, pH, and coexisting anions on BPA degradation was thoroughly investigated. Radical scavenging experiments combined with electron paramagnetic resonance analysis identified center dot SO4-, center dot OH, and photogenerated holes as dominant reactive species. The system also exhibited good stability over five consecutive cycles, with minimal metal ion leaching. This work demonstrates the potential of an efficient PEC system integrated with sulfate radical-based AOPs, offering an innovative approach for organic pollutant remediation in wastewater treatment.
Keyword :
Organic removal Organic removal Peroxymonosulfate Peroxymonosulfate Photoelectrocatalytic Photoelectrocatalytic
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GB/T 7714 | Geng, Xuanran , Zhang, Renfu , Zhang, Peiyun et al. Photoelectrochemical cell with Co3O4/BiVO4 photoanode and CoFe2O4 cathode: An efficient persulfate activation system for organic pollutants degradation [J]. | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2025 , 13 (2) . |
MLA | Geng, Xuanran et al. "Photoelectrochemical cell with Co3O4/BiVO4 photoanode and CoFe2O4 cathode: An efficient persulfate activation system for organic pollutants degradation" . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 13 . 2 (2025) . |
APA | Geng, Xuanran , Zhang, Renfu , Zhang, Peiyun , Yuan, Xiaoying , Yang, Can , Hou, Yidong et al. Photoelectrochemical cell with Co3O4/BiVO4 photoanode and CoFe2O4 cathode: An efficient persulfate activation system for organic pollutants degradation . | JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING , 2025 , 13 (2) . |
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Photocatalytic oxidation of benzene to phenol using molecular oxygen (O-2) is a promising alternative to the traditional cumene process. However, the selectivity toward phenol is often poor due to the ring-opening reaction induced by the superoxide radical (O-center dot(2)-), which is predominantly produced from the single-electron reduction of O-2. Herein, we demonstrate that introducing abundant oxygen vacancies (OVs) on the surface of titanium dioxide (TiO2) facilitates the activation of O-2 through a two-electron reduction process instead of a single-electron reduction. This effectively suppresses the generation of O-center dot(2)-, thereby reducing phenol decomposition and significantly enhancing the selectivity. In addition, these OVs can trap the electrons to promote chare separation and serve as the adsorption sites for O-2 activation. As a result, the introduction of abundant OVs on the surface of TiO2 not only enhances phenol yield but also importantly improves selectivity toward phenol. This finding enriches our understanding of how OVs influence reaction pathways and product selectivity, providing valuable insights for the design and tailoring of OV-rich photocatalysts for selective organic oxygenations.
Keyword :
benzene hydroxylation reaction benzene hydroxylation reaction O-2 activation O-2 activation oxygen vacancy oxygen vacancy photocatalysis photocatalysis selectivity selectivity
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GB/T 7714 | Zhong, Shengyang , Yu, Dexi , Ma, Yuhui et al. Oxygen Vacancy-Enhanced Selectivity in Aerobic Oxidation of Benzene to Phenol over TiO2 Photocatalysts [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (18) . |
MLA | Zhong, Shengyang et al. "Oxygen Vacancy-Enhanced Selectivity in Aerobic Oxidation of Benzene to Phenol over TiO2 Photocatalysts" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 18 (2025) . |
APA | Zhong, Shengyang , Yu, Dexi , Ma, Yuhui , Lin, Yuhong , Wang, Xiaoyi , Yu, Zhenzhen et al. Oxygen Vacancy-Enhanced Selectivity in Aerobic Oxidation of Benzene to Phenol over TiO2 Photocatalysts . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (18) . |
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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.
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GB/T 7714 | Li, Jilong , Zhao, Jiwu , Wang, Sibo 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 , 147 (17) : 14705-14714 . |
MLA | Li, Jilong et al. "Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 17 (2025) : 14705-14714 . |
APA | Li, Jilong , Zhao, Jiwu , Wang, Sibo , Peng, Kang-Shun , Su, Bo , Liu, Kunlong et al. Activating Lattice Oxygen in Perovskite Ferrite for Efficient and Stable Photothermal Dry Reforming of Methane . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (17) , 14705-14714 . |
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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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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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Photocatalytic hydroxylation of benzene in water using H2O2 as the oxidant is a green approach toward phenol synthesis. However, the immiscibility of benzene in water results in poor photocatalytic performance and a low efficiency of H2O2 utilization. To enhance drastically the affinity between the aqueous and nonaqueous phases, an amphiphilic heterojunction (Fe2O3/crystalline carbon nitride (CCN)) has been synthesized by intimately immobilizing hematite (Fe2O3) nanoparticles on a CCN surface for the photocatalytic hydroxylation of benzene to phenol. The unique amphiphilicity of Fe2O3/CCN allows the formation and stabilization of homogeneous emulsions in a benzene/water mixture to increase the effective oil/water interface area for more efficient mass transport. Moreover, the well-established type II heterojunction between Fe2O3 and CCN facilitates the fast separation and transfer of photoelectrons from CCN to Fe2O3 for the photo-Fenton activation of H2O2 with high utilization efficiency. We recorded a maximum phenol conversion of 31.6% by using a stoichiometric amount of H2O2 (10 mmol) on the photocatalytic hydroxylation of benzene. The apparent quantum yield of phenol production at lambda = 420 nm was determined to be 47.1%. This amphiphilic photocatalyst approach would be useful for realizing other advanced oxidation reactions involving immiscible components.
Keyword :
benzene hydroxylationreaction benzene hydroxylationreaction carbon nitride carbon nitride green synthesis green synthesis phenol synthesis phenol synthesis photocatalysis photocatalysis
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GB/T 7714 | Su, Ningxi , Yu, Dexi , Zhong, Shengyang et al. Emulsion of Benzene and Water Phases by an Amphiphilic Hematite/Carbon Nitride Photocatalyst for Phenol Synthesis [J]. | ACS CATALYSIS , 2025 , 15 (13) : 11911-11921 . |
MLA | Su, Ningxi et al. "Emulsion of Benzene and Water Phases by an Amphiphilic Hematite/Carbon Nitride Photocatalyst for Phenol Synthesis" . | ACS CATALYSIS 15 . 13 (2025) : 11911-11921 . |
APA | Su, Ningxi , Yu, Dexi , Zhong, Shengyang , Huang, Meirong , Hou, Yidong , Anpo, Masakazu et al. Emulsion of Benzene and Water Phases by an Amphiphilic Hematite/Carbon Nitride Photocatalyst for Phenol Synthesis . | ACS CATALYSIS , 2025 , 15 (13) , 11911-11921 . |
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The oxygen reduction reaction (ORR) can proceed through either a two- or four-electron pathway, both of which are important for a wide range of applications. The intermediate conversion of *O-2(-) + H+ -> *OOH recognized as the rate-determining step in ORR, with its efficiency strongly dependent on the nature of active sites at the surface of a catalyst. Herein, Si-supported carbon dots (Si-CDs) are introduced as cocatalysts in a photocatalytic system, where their nitrogen-carbon sites play a pivotal role in lowering the energy barrier for *OOH formation by promoting proton and electron transfers, thus enhancing the H2O2 production rate in ORR. This strategy is broadly applicable across a wide range of photocatalysts, both with and without use of sacrificial agents. The H2O2 production rate for Zn0.5Cd0.5S (30 mg) increased from 13.0 to 40.9 mu mol h(-1) when 0.6 mg of Si-CDs were added. In-situ characterizations and theoretical simulations are conducted to reveal the reaction pathway and the reduced energy requirements for the *O-2(-) + H+ -> *OOH conversion. This study provides a unique example of overcoming a key barrier in ORR using a metal-free catalyst and promotes potential applications in various fields.
Keyword :
Active site Active site Carbon dots Carbon dots H2O2 H2O2 *OOH *OOH Photocatalytic oxygen reduction Photocatalytic oxygen reduction
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GB/T 7714 | Wang, Yankun , Zhang, Mingxian , Wu, Haihua et al. Si/Carbon-dots with Surface N-C Sites Promoting Proton and Electron Transfers in Oxygen Reduction Reaction [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
MLA | Wang, Yankun et al. "Si/Carbon-dots with Surface N-C Sites Promoting Proton and Electron Transfers in Oxygen Reduction Reaction" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025) . |
APA | Wang, Yankun , Zhang, Mingxian , Wu, Haihua , Huang, Meirong , Fang, Yuanxing , Anpo, Masakazu et al. Si/Carbon-dots with Surface N-C Sites Promoting Proton and Electron Transfers in Oxygen Reduction Reaction . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
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Phenolic resins, with a unique it-conjugated semiconductor band structure, have attracted numerous attentions in solar energy conversion. However, their metal-free nature often results in a lack of sufficient active sites on their surface to interact with substrate molecules. Herein, we demonstrate that abundant active sites can be created in situ on the surface of phenolic resins through direct condensation of triphenylborate (TPB) with 3-aminophenol (3-AP) by using a molecular design approach. The electron-deficient central B atoms in the TPB motifs and the electron-rich N atoms in the 3-AP motifs are uniformly distributed on the phenolic resin surfaces at spatially appropriate distances, serving as synergistic Lewis acid and base sites for the adsorption and activation of substrate molecules. Moreover, the polarized electric field induced by these Lewis acid-base sites facilitates exciton dissociation and rapid charge separation. The modified phenolic resin was found to be highly effective for the selective oxidation of methyl phenyl sulfide (MPS) with O2. This study presents a novel strategy for the molecular design of phenolic resins with synergistic active sites to enhance photocatalytic organic transformations.
Keyword :
Aerobic oxidation reaction Aerobic oxidation reaction Cooperative Lewis acid-base pair Cooperative Lewis acid-base pair Phenolic resin Phenolic resin Photocatalysis Photocatalysis Synergy effect Synergy effect
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GB/T 7714 | Li, Meng , Zhang, Jingyi , Liang, Linfang et al. In-situ generation of synergistic Lewis acid-base sites on phenolic resins for enhanced photocatalytic aerobic oxidation reactions [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 372 . |
MLA | Li, Meng et al. "In-situ generation of synergistic Lewis acid-base sites on phenolic resins for enhanced photocatalytic aerobic oxidation reactions" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 372 (2025) . |
APA | Li, Meng , Zhang, Jingyi , Liang, Linfang , Huang, Meirong , Hou, Yidong , Anpo, Masakazu et al. In-situ generation of synergistic Lewis acid-base sites on phenolic resins for enhanced photocatalytic aerobic oxidation reactions . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 372 . |
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A promising strategy to enhance exciton dissociation and charge separation in phenolic-polymer-based photocatalysts is the generation and utilization of benzenoid-quinoid donor-acceptor (D-A) couples inside the phenolic resin frameworks. However, there are often more donors than acceptors in phenolic resin due to the sluggish kinetics of in situ oxidation of phenols to quinoid methides, leading to a mismatched D/A ratio. Herein, we report a well-cross-linked phenolic resin with a unity D/A ratio synthesized by using phloroglucinol as a building block for condensation with formaldehyde. The higher electron density on the aromatic ring not only facilitates the in situ oxidation of phloroglucinols to quinoid methides, forming equivalent D-A couples, but also lowers the energy barrier for the condensation reaction, resulting in a highly cross-linked framework with a well-developed pi-conjugated electronic structure. The phloroglucinol-formaldehyde resin product demonstrates significantly improved photocatalytic performance in the selective oxidation of methyl phenyl sulfide and the oxidative coupling of benzylamine. Our approach shows the potential of photocatalytic phenolic resins for solar-induced chemical conversion.
Keyword :
aerobic oxidation reactions aerobic oxidation reactions electron donor-acceptor architecture electron donor-acceptor architecture phenolic resin phenolic resin photocatalysis photocatalysis pi-conjugatedpolymer pi-conjugatedpolymer
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GB/T 7714 | Li, Meng , Huang, Meirong , Lin, Zheng et al. Phenolic Resin with an Optimized Donor-Acceptor Architecture for Photocatalytic Aerobic Oxidation [J]. | ACS CATALYSIS , 2024 , 14 (23) : 17622-17632 . |
MLA | Li, Meng et al. "Phenolic Resin with an Optimized Donor-Acceptor Architecture for Photocatalytic Aerobic Oxidation" . | ACS CATALYSIS 14 . 23 (2024) : 17622-17632 . |
APA | Li, Meng , Huang, Meirong , Lin, Zheng , Hou, Yidong , Anpo, Masakazu , Yu, Jimmy C. et al. Phenolic Resin with an Optimized Donor-Acceptor Architecture for Photocatalytic Aerobic Oxidation . | ACS CATALYSIS , 2024 , 14 (23) , 17622-17632 . |
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