Hui-Qin Zheng, Jun Wang, Ming-Cai Yin, Yao-Ting Fan
{"title":"利用 Ru(II)-Phenantroline 衍生物提高纳米二氧化钛制氢的光催化活性","authors":"Hui-Qin Zheng, Jun Wang, Ming-Cai Yin, Yao-Ting Fan","doi":"10.1134/S0023158424600044","DOIUrl":null,"url":null,"abstract":"<p>Two novel Ru(II)-phenanthroline derivatives complexes, Ru-1 and Ru-2, were synthesized and characterized. The key distinction between Ru-1 and Ru-2 lies in their ligands: L1 (2-hydroxy-5-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl) benzoic acid) and L2 (2-hydroxy-3-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl)benzoic acid). In L1, the –OH group is located in the <i>para</i>-position, while in L2, it resides in the <i>ortho-</i>position. Subsequently, Pt/TiO<sub>2</sub> and Ru-1/Pt/TiO<sub>2</sub> (and Ru-2/Pt/TiO<sub>2</sub>) composites were prepared using photo-deposition and impregnation methods, respectively. The Ru-1/Pt/TiO<sub>2</sub> and Ru-2/Pt/TiO<sub>2</sub> composites were thoroughly characterized using various techniques, including ultraviolet-visible spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), fluorescence spectroscopy (FL), cyclic voltammetry (CV) experiments, and other relevant techniques. Photocatalytic hydrogen production systems were established by employing Ru-1/Pt-TiO<sub>2</sub> and Ru-2/Pt-TiO<sub>2</sub> as photocatalysts and ascorbic acid (H<sub>2</sub>A) as a sacrificial reagent. The results demonstrated that the maximum hydrogen production reached 1461 μmol (Ru-1/Pt/TiO<sub>2</sub>) and 843 μmol (Ru-2/Pt/TiO<sub>2</sub>) under optimized conditions with 20 mg of composite photocatalyst, 0.3 mol L<sup>–1</sup> of H<sub>2</sub>A, and pH 4, within 4 h of irradiation (λ > 420 nm). Correspondingly, the photocatalytic hydrogen production rates were 18 267 and 10 523 μmol g<sup>–1</sup> h<sup>–1</sup>, respectively. Mechanism studies revealed that electrons flow from the highest occupied molecular orbital (HOMO) of Ru-1 to the conduction band (CB) of TiO<sub>2</sub>, subsequently combining with H<sup>+</sup> on the surface of the Pt metal nanoparticles to generate hydrogen gas. The holes on the lowest unoccupied molecular orbital (LUMO) of the photosensitizer are oxidized by H<sub>2</sub>A, thereby regenerating the activity of the composite catalyst by restoring the photosensitizer.</p>","PeriodicalId":682,"journal":{"name":"Kinetics and Catalysis","volume":"65 4","pages":"366 - 377"},"PeriodicalIF":1.3000,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancement of Photocatalytic Activity for Hydrogen Production of Nano-TiO2 Using Ru(II)-Phenantroline Derivatives\",\"authors\":\"Hui-Qin Zheng, Jun Wang, Ming-Cai Yin, Yao-Ting Fan\",\"doi\":\"10.1134/S0023158424600044\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Two novel Ru(II)-phenanthroline derivatives complexes, Ru-1 and Ru-2, were synthesized and characterized. The key distinction between Ru-1 and Ru-2 lies in their ligands: L1 (2-hydroxy-5-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl) benzoic acid) and L2 (2-hydroxy-3-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl)benzoic acid). In L1, the –OH group is located in the <i>para</i>-position, while in L2, it resides in the <i>ortho-</i>position. Subsequently, Pt/TiO<sub>2</sub> and Ru-1/Pt/TiO<sub>2</sub> (and Ru-2/Pt/TiO<sub>2</sub>) composites were prepared using photo-deposition and impregnation methods, respectively. The Ru-1/Pt/TiO<sub>2</sub> and Ru-2/Pt/TiO<sub>2</sub> composites were thoroughly characterized using various techniques, including ultraviolet-visible spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), fluorescence spectroscopy (FL), cyclic voltammetry (CV) experiments, and other relevant techniques. Photocatalytic hydrogen production systems were established by employing Ru-1/Pt-TiO<sub>2</sub> and Ru-2/Pt-TiO<sub>2</sub> as photocatalysts and ascorbic acid (H<sub>2</sub>A) as a sacrificial reagent. The results demonstrated that the maximum hydrogen production reached 1461 μmol (Ru-1/Pt/TiO<sub>2</sub>) and 843 μmol (Ru-2/Pt/TiO<sub>2</sub>) under optimized conditions with 20 mg of composite photocatalyst, 0.3 mol L<sup>–1</sup> of H<sub>2</sub>A, and pH 4, within 4 h of irradiation (λ > 420 nm). Correspondingly, the photocatalytic hydrogen production rates were 18 267 and 10 523 μmol g<sup>–1</sup> h<sup>–1</sup>, respectively. Mechanism studies revealed that electrons flow from the highest occupied molecular orbital (HOMO) of Ru-1 to the conduction band (CB) of TiO<sub>2</sub>, subsequently combining with H<sup>+</sup> on the surface of the Pt metal nanoparticles to generate hydrogen gas. The holes on the lowest unoccupied molecular orbital (LUMO) of the photosensitizer are oxidized by H<sub>2</sub>A, thereby regenerating the activity of the composite catalyst by restoring the photosensitizer.</p>\",\"PeriodicalId\":682,\"journal\":{\"name\":\"Kinetics and Catalysis\",\"volume\":\"65 4\",\"pages\":\"366 - 377\"},\"PeriodicalIF\":1.3000,\"publicationDate\":\"2024-07-31\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Kinetics and Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1134/S0023158424600044\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Kinetics and Catalysis","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1134/S0023158424600044","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Enhancement of Photocatalytic Activity for Hydrogen Production of Nano-TiO2 Using Ru(II)-Phenantroline Derivatives
Two novel Ru(II)-phenanthroline derivatives complexes, Ru-1 and Ru-2, were synthesized and characterized. The key distinction between Ru-1 and Ru-2 lies in their ligands: L1 (2-hydroxy-5-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl) benzoic acid) and L2 (2-hydroxy-3-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl)benzoic acid). In L1, the –OH group is located in the para-position, while in L2, it resides in the ortho-position. Subsequently, Pt/TiO2 and Ru-1/Pt/TiO2 (and Ru-2/Pt/TiO2) composites were prepared using photo-deposition and impregnation methods, respectively. The Ru-1/Pt/TiO2 and Ru-2/Pt/TiO2 composites were thoroughly characterized using various techniques, including ultraviolet-visible spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), fluorescence spectroscopy (FL), cyclic voltammetry (CV) experiments, and other relevant techniques. Photocatalytic hydrogen production systems were established by employing Ru-1/Pt-TiO2 and Ru-2/Pt-TiO2 as photocatalysts and ascorbic acid (H2A) as a sacrificial reagent. The results demonstrated that the maximum hydrogen production reached 1461 μmol (Ru-1/Pt/TiO2) and 843 μmol (Ru-2/Pt/TiO2) under optimized conditions with 20 mg of composite photocatalyst, 0.3 mol L–1 of H2A, and pH 4, within 4 h of irradiation (λ > 420 nm). Correspondingly, the photocatalytic hydrogen production rates were 18 267 and 10 523 μmol g–1 h–1, respectively. Mechanism studies revealed that electrons flow from the highest occupied molecular orbital (HOMO) of Ru-1 to the conduction band (CB) of TiO2, subsequently combining with H+ on the surface of the Pt metal nanoparticles to generate hydrogen gas. The holes on the lowest unoccupied molecular orbital (LUMO) of the photosensitizer are oxidized by H2A, thereby regenerating the activity of the composite catalyst by restoring the photosensitizer.
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Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.
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