You Wu , Chang Cheng , Kezhen Qi , Bei Cheng , Jianjun Zhang , Jiaguo Yu , Liuyang Zhang
{"title":"ZnO/D-A共轭聚合物S-Scheme异质结高效光催化制备H2O2及电荷转移动力学研究","authors":"You Wu , Chang Cheng , Kezhen Qi , Bei Cheng , Jianjun Zhang , Jiaguo Yu , Liuyang Zhang","doi":"10.3866/PKU.WHXB202406027","DOIUrl":null,"url":null,"abstract":"<div><div>Photocatalytic technology harnesses clean, non-polluting solar energy to synthesize hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>). In this study, ZnO/PBD S-scheme heterojunction composites, featuring ZnO nanoparticles on a donor-acceptor conjugated polymer substrate (PBD), were synthesized <em>via</em> the Suzuki-Miyaura reaction and hydrothermal method. The optimal ZnO/PBD composite achieved an H<sub>2</sub>O<sub>2</sub> production efficiency of 4.07 mmol·g<sup>−1</sup>·h<sup>−1</sup>, which is 5.4 times higher than that of pristine ZnO. This significant enhancement is attributed to the formation of S-scheme heterojunctions. The successful construction of S-scheme heterojunctions was confirmed through UV-visible absorption spectroscopy and <em>in situ</em> irradiated X-ray photoelectron spectroscopy. Steady-state photoluminescence and femtosecond transient absorption (fs-TA) spectroscopies identified and verified the presence of defect states in ZnO. These defect states trap photogenerated electrons, adversely affecting the photocatalytic reaction. However, the S-scheme heterojunction effectively promotes the separation and transfer of electrons, mitigating this issue. The measured lifetimes of photogenerated electrons in these defect states, as determined by fitted fs-TA decay kinetics, provided further evidence of the carrier transfer mechanism in S-scheme heterojunctions. This work introduces a novel approach for studying organic/inorganic S-scheme heterojunctions using fs-TA spectroscopy.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (72KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"40 11","pages":"Article 2406027"},"PeriodicalIF":10.8000,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient Photocatalytic Production of H2O2 over ZnO/D-A Conjugated Polymer S-Scheme Heterojunction and Charge Transfer Dynamics Investigation\",\"authors\":\"You Wu , Chang Cheng , Kezhen Qi , Bei Cheng , Jianjun Zhang , Jiaguo Yu , Liuyang Zhang\",\"doi\":\"10.3866/PKU.WHXB202406027\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Photocatalytic technology harnesses clean, non-polluting solar energy to synthesize hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>). In this study, ZnO/PBD S-scheme heterojunction composites, featuring ZnO nanoparticles on a donor-acceptor conjugated polymer substrate (PBD), were synthesized <em>via</em> the Suzuki-Miyaura reaction and hydrothermal method. The optimal ZnO/PBD composite achieved an H<sub>2</sub>O<sub>2</sub> production efficiency of 4.07 mmol·g<sup>−1</sup>·h<sup>−1</sup>, which is 5.4 times higher than that of pristine ZnO. This significant enhancement is attributed to the formation of S-scheme heterojunctions. The successful construction of S-scheme heterojunctions was confirmed through UV-visible absorption spectroscopy and <em>in situ</em> irradiated X-ray photoelectron spectroscopy. Steady-state photoluminescence and femtosecond transient absorption (fs-TA) spectroscopies identified and verified the presence of defect states in ZnO. These defect states trap photogenerated electrons, adversely affecting the photocatalytic reaction. However, the S-scheme heterojunction effectively promotes the separation and transfer of electrons, mitigating this issue. The measured lifetimes of photogenerated electrons in these defect states, as determined by fitted fs-TA decay kinetics, provided further evidence of the carrier transfer mechanism in S-scheme heterojunctions. This work introduces a novel approach for studying organic/inorganic S-scheme heterojunctions using fs-TA spectroscopy.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (72KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>\",\"PeriodicalId\":6964,\"journal\":{\"name\":\"物理化学学报\",\"volume\":\"40 11\",\"pages\":\"Article 2406027\"},\"PeriodicalIF\":10.8000,\"publicationDate\":\"2024-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"物理化学学报\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1000681824001681\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"物理化学学报","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1000681824001681","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Efficient Photocatalytic Production of H2O2 over ZnO/D-A Conjugated Polymer S-Scheme Heterojunction and Charge Transfer Dynamics Investigation
Photocatalytic technology harnesses clean, non-polluting solar energy to synthesize hydrogen peroxide (H2O2). In this study, ZnO/PBD S-scheme heterojunction composites, featuring ZnO nanoparticles on a donor-acceptor conjugated polymer substrate (PBD), were synthesized via the Suzuki-Miyaura reaction and hydrothermal method. The optimal ZnO/PBD composite achieved an H2O2 production efficiency of 4.07 mmol·g−1·h−1, which is 5.4 times higher than that of pristine ZnO. This significant enhancement is attributed to the formation of S-scheme heterojunctions. The successful construction of S-scheme heterojunctions was confirmed through UV-visible absorption spectroscopy and in situ irradiated X-ray photoelectron spectroscopy. Steady-state photoluminescence and femtosecond transient absorption (fs-TA) spectroscopies identified and verified the presence of defect states in ZnO. These defect states trap photogenerated electrons, adversely affecting the photocatalytic reaction. However, the S-scheme heterojunction effectively promotes the separation and transfer of electrons, mitigating this issue. The measured lifetimes of photogenerated electrons in these defect states, as determined by fitted fs-TA decay kinetics, provided further evidence of the carrier transfer mechanism in S-scheme heterojunctions. This work introduces a novel approach for studying organic/inorganic S-scheme heterojunctions using fs-TA spectroscopy.
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