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学者姓名：张金水
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Abstract ：
Designing porous structures has proven to be an effective strategy for enhancing the photocatalytic NO oxidation activity of carbon nitride (CN). Despite significant advances in the fabrication of porous CN, a cost-effective and high-yield synthesis method for porous CN is still highly desirable. In this study, we presented a facile strategy to synthesize porous carbon nitride by V2O5-assisted thermal oxidation process. Namely, after grinding bulk CN with a small amount of NH4VO3, the mixture was subjected to thermal treatment, resulting in porous carbon nitride with a yield of 50 %. The resulting porous structure, which features an enlarged surface area and enhanced charge separation efficiency, significantly improved the photocatalytic performance for NO removal-approximately four times higher than bulk CN. Additionally, the NO removal mechanism was investigated through in-situ Fourier transform infrared spectroscopy to observe reaction intermediates and electron paramagnetic resonance trapping experiments to identify active species, providing insight into the conversion pathway. The catalytic thermal oxidation etching process effectively tuned the microstructure of g-C3N4, offering a low-cost, easy-to-implement, and time-efficient method for synthesizing porous CN, thereby providing a promising approach for developing advanced photocatalysts.
Keyword ：
NO oxidation NO oxidation O 2 activation O 2 activation Photocatalysis Photocatalysis Porous carbon nitride Porous carbon nitride
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| GB/T 7714 | Fang, Zixun , Zhou, Yao , Yang, Zhou et al. V2O5-assisted thermal oxidation strategy for synthesizing porous carbon nitride with enhanced photocatalytic NO removal performance [J]. | SURFACES AND INTERFACES , 2025 , 60 . |
| MLA | Fang, Zixun et al. "V2O5-assisted thermal oxidation strategy for synthesizing porous carbon nitride with enhanced photocatalytic NO removal performance" . | SURFACES AND INTERFACES 60 (2025) . |
| APA | Fang, Zixun , Zhou, Yao , Yang, Zhou , Yang, Can , Zhang, Jinshui , Hou, Yidong . V2O5-assisted thermal oxidation strategy for synthesizing porous carbon nitride with enhanced photocatalytic NO removal performance . | SURFACES AND INTERFACES , 2025 , 60 . |
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Abstract ：
光催化臭氧化技术作为一种新兴的高级氧化工艺,相较于传统臭氧化技术,展现出显著提升的氧化效能与环境治理潜力.光催化臭氧化技术的创新之处在于将光催化与臭氧化进行耦合,通过光生载流子(e-与h+)驱动臭氧活化,生成羟基自由基(•OH)和超氧自由基(•O2-)等高活性氧物种,形成多路径氧化网络,实现污染物的快速降解与深度矿化.相关研究表明,该技术可显著降低臭氧投加量并有效控制残留臭氧浓度,兼具经济性与环境友好性.然而,光生电子参与的臭氧还原过程涉及吸附-解离-自由基级联反应等诸多复杂步骤,其在分子层面的作用机制仍有待进一步明确,这已然成为制约该技术优化的关键科学难题. 针对光催化臭氧化反应中臭氧活化机制的复杂性,本文采用晶面工程策略,深入探究并阐明了催化剂表面结构对臭氧吸附与活化行为所起到的决定性影响.以层状Bi2O2CO3(BOC)为模型催化剂,研究发现{110}晶面与{001}晶面凭借差异化的原子排布,能够调控臭氧吸附特性与反应路径.BOC-{110}吸附臭氧能力强,可直接解离O3为表面原子氧(*O)与氧气(O2),主导表面直接氧化路径;而BOC-{001}则具有适中的O3吸附能力,有利于光生电子向O3转移,形成•O3-中间体,经质子化作用进一步生成•OH与O2,主导自由基间接氧化路径.原位光谱表征证实了这种晶面依赖的臭氧活化差异:红外光谱监测到吸附在BOC-{001}表面上臭氧(*O3)在光照条件下被迅速消耗;拉曼光谱则观察到BOC-{110}表面上*O的累积.此外,晶面工程还能调控光催化剂的内建电场,暴露{001}晶面促进激子的解离以及载流子的分离,进一步加速了光生电子活化臭氧的动力学过程,产生更多羟基自由基.因此,BOC-{001}在光催化臭氧化过程中表现出优异的苯酚矿化率(85%),明显优于BOC-{110}(53%),并保持良好的循环稳定性. 综上,晶面工程在光催化臭氧化体系中的创新性应用,为高性能催化剂的构筑提供了全新的视角.通过精准调控催化剂的暴露晶面与表面活性位点,可实现臭氧吸附强度、光生载流子迁移路径及活性自由基定向生成动力学的多维度优化.电荷分离效率与臭氧活化效率的同步提升,成功突破了光催化体系中单电子活化臭氧动力学的速率限制,进而有望实现难降解有机污染物的深度矿化.
Keyword ：
Bi2O2CO3 Bi2O2CO3 光催化臭氧化 光催化臭氧化 吸附构型 吸附构型 晶面工程 晶面工程 臭氧活化 臭氧活化
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| GB/T 7714 | 杨洋 , 杨洲 , 赖志明 et al. Bi2O2CO3纳米片晶面工程增强光催化臭氧化:揭示臭氧吸附与电子转移机制 [J]. | 催化学报 , 2025 , 72 (5) : 143-153 . |
| MLA | 杨洋 et al. "Bi2O2CO3纳米片晶面工程增强光催化臭氧化:揭示臭氧吸附与电子转移机制" . | 催化学报 72 . 5 (2025) : 143-153 . |
| APA | 杨洋 , 杨洲 , 赖志明 , 阳灿 , 侯乙东 , 陶慧琳 et al. Bi2O2CO3纳米片晶面工程增强光催化臭氧化:揭示臭氧吸附与电子转移机制 . | 催化学报 , 2025 , 72 (5) , 143-153 . |
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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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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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Photocatalytic ozonation holds promise for advanced water purification, yet its development has been hindered by a limited understanding of ozone activation mechanisms and its related photogenerated electron transfer dynamics. Herein, we employed in-situ DRIFTS and Raman spectroscopy to elucidate the distinct adsorption and activation behaviors of ozone (O3) on the {001} and {110} crystal facets of Bi2O2CO3 (BOC) nanosheets. BOC-{001} demonstrates superior photocatalytic ozonation performance, with 85% phenol mineralization and excellent durability, significantly outperforming the 53% mineralization rate of BOC-{110}. This enhanced activity is attributed to non-dissociative ozone adsorption and favorable adsorption energy over {001} facet, which facilitate the one-electron O3 reduction pathway. Furthermore, crystal facet engineering strengthens the built-in electric field, promoting exciton dissociation and the generation of localized charge carriers. The synergistic effects of optimized electron availability and ozone adsorption significantly boost the production of reactive oxygen species. These findings provide a deeper understanding of the critical roles of O3 adsorption and electron transfer in radical generation, which could provide some guidance for the strategic development of highly effective photocatalytic ozonation catalysts. © 2025 Dalian Institute of Chemical Physics, the Chinese Academy of Sciences
Keyword ：
Air cleaners Air cleaners Boron compounds Boron compounds Nanosheets Nanosheets Ozonization Ozonization Photocatalysis Photocatalysis Selenium compounds Selenium compounds
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| GB/T 7714 | Yang, Yang , Yang, Zhou , Lai, Zhiming et al. Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism [J]. | Chinese Journal of Catalysis , 2025 , 72 : 143-153 . |
| MLA | Yang, Yang et al. "Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism" . | Chinese Journal of Catalysis 72 (2025) : 143-153 . |
| APA | Yang, Yang , Yang, Zhou , Lai, Zhiming , Yang, Can , Hou, Yidong , Tao, Huilin et al. Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism . | Chinese Journal of Catalysis , 2025 , 72 , 143-153 . |
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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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The development of durable and highly efficient visible-light-driven photocatalysts is essential for the photo- catalytic ozonation process towards degrading organic pollutants. This study presents CN-MA, a novel photo- catalyst synthesized by grafting carbon nitride (CN) with single-atom Mn and 2-hydroxy-4,6-dimethylpyrimidine (HDMP) via one-step thermal polymerization. Experimental characterization and theoretical calculation results reveal that incorporating single-atom Mn and HDMP into CN alters the charge density distribution on the heptazine rings. This modification enhances the absorption of visible light and reduces exciton binding energy, leading to improved separation and migration of photogenerated charge carriers. Moreover, the single-atom Mn provides abundant active sites for O3 adsorption and activation, which increases the utilization of photo- generated electrons to produce highly reactive oxidative species. Consequently, CN-MA exhibits superior photocatalytic ozonation activity, achieving 94% mineralization of phenol within 60 min and maintaining excellent stability over multiple cycles. The research also proposes a plausible reaction mechanism based on free-radical trapping experiments and steady-state concentration experiments using molecular probes. This strategy advances the development of molecular-engineered catalysts co-modified with single metal atoms, thereby enhancing the photocatalytic ozonation process for the degradation of organic pollutants.
Keyword ：
Carbon nitride Carbon nitride Molecular engineering Molecular engineering Photocatalytic ozonation Photocatalytic ozonation Single-atom Single-atom
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| GB/T 7714 | Lai, Zhiming , Yang, Yang , Yang, Zhou et al. Carbon nitride grafted with single-atom manganese and 2-hydroxy-4,6-di-methylpyrimidine: A visible-light-driven photocatalyst for enhanced ozonation of organic pollutants [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 683 : 1106-1118 . |
| MLA | Lai, Zhiming et al. "Carbon nitride grafted with single-atom manganese and 2-hydroxy-4,6-di-methylpyrimidine: A visible-light-driven photocatalyst for enhanced ozonation of organic pollutants" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 683 (2025) : 1106-1118 . |
| APA | Lai, Zhiming , Yang, Yang , Yang, Zhou , Ruan, Wenqi , Yang, Can , Chen, Qiang et al. Carbon nitride grafted with single-atom manganese and 2-hydroxy-4,6-di-methylpyrimidine: A visible-light-driven photocatalyst for enhanced ozonation of organic pollutants . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 683 , 1106-1118 . |
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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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Persulfate-based advanced oxidation technology, due to its high efficiency, controllability, and safety, shows great potential for the deep removal of organic pollution, yet its mineralization efficiency is hindered by the lack of synergy between radical and nonradical pathways. Herein, we present defective carbon nitride (DCN) as a highly efficient peroxymonosulfate (PMS) activation catalyst that couples nonradical aggregation with radical mineralization. The tailored electronic structure of the DCN framework enhances visible-light absorption, photogenerated charge separation, and electron transfer ability due to a built-in electric field. DCN effectively interacts with PMS to rapidly accumulate pollutants from the bulk solution onto the catalyst surface via an electron-transfer pathway. Simultaneously, the accumulated pollutants undergo in-situ decomposition by center dot SO4- radicals formed on the catalyst surface under visible light irradiation, achieving a remarkable 98 % mineralization ratio. The mixed-pathway process demonstrates excellent cyclic stability and environmental robustness. This study introduces a novel strategy to enhance the catalytic oxidation performance of metal-free catalysts by controlling persulfate activation pathways for water decontamination.
Keyword ：
Carbon nitride Carbon nitride Peroxymonosulfate Peroxymonosulfate Photocatalysis Photocatalysis Pollutant mineralization Pollutant mineralization Synergistic Synergistic
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| GB/T 7714 | Ming, Hongbo , Ruan, Wenqi , Yuan, Xiaoying et al. Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 360 . |
| MLA | Ming, Hongbo et al. "Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization" . | SEPARATION AND PURIFICATION TECHNOLOGY 360 (2025) . |
| APA | Ming, Hongbo , Ruan, Wenqi , Yuan, Xiaoying , Cheng, Jiajia , Yang, Can , Hou, Yidong et al. Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 360 . |
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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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