Boosted Charge Transfer for Highly Efficient Photosynthesis of H2O2 over Z-Scheme I−/K+ Co-Doped g-C3N4/Metal–Organic-Frameworks in Pure Water under Visible Light
{"title":"Boosted Charge Transfer for Highly Efficient Photosynthesis of H2O2 over Z-Scheme I−/K+ Co-Doped g-C3N4/Metal–Organic-Frameworks in Pure Water under Visible Light","authors":"Xize Lu, Zongwei Chen, Zhuofeng Hu, Fuyu Liu, Zhihong Zuo, Zixiang Gao, Haiguang Zhang, Youcai Zhu, Runzeng Liu, Yongguang Yin, Yong Cai, Dongling Ma, Qingzhe Zhang","doi":"10.1002/aenm.202401873","DOIUrl":null,"url":null,"abstract":"Photocatalytic oxygen reduction reaction (ORR) is an environmentally friendly and cost-effective approach for H<sub>2</sub>O<sub>2</sub> synthesis. However, the current photosynthesis system suffers from sluggish kinetics, rapid recombination of photoexcited charge carriers, and weak redox potentials, resulting in unsatisfactory solar-to-chemical conversion efficiency. Herein, a Z-scheme heterojunction (UiO/IKCN) is constructed through coupling I<sup>−</sup>/K<sup>+</sup> co-doped g-C<sub>3</sub>N<sub>4</sub> (IKCN) with NH<sub>2</sub>-UiO-66, a typical metal-organic framework material. Under visible light irradiation, the optimal UiO/IKCN exhibits exceptional H<sub>2</sub>O<sub>2</sub> production rates in pure water (13.3 mM g<sup>−1</sup> h<sup>−1</sup>) and in isopropanol solution (72.6 mM g<sup>−1</sup> h<sup>−1</sup>), that is 48.4 times higher than pristine CN in isopropanol (1.5 mM g<sup>−1</sup> h<sup>−1</sup>). A high apparent quantum yield of 10.28% at 420 nm is achieved by UiO/IKCN, surpassing most previously reported values. The dominating role of two-electron ORR in H<sub>2</sub>O<sub>2</sub> photosynthesis is elucidated in detail. The significantly enhanced photocatalytic activity can be attributed to the facilitated charge separation and Z-scheme charge transfer, which are unambiguously verified by stable-state surface photovoltage, transient photoluminescence, femtosecond transient absorption spectroscopy, in-situ irradiated X-ray photoelectron spectroscopy, and density functional theory calculations. This study represents the first exploration of H<sub>2</sub>O<sub>2</sub> production using NH<sub>2</sub>-UiO-66 and provides insights into the rational design of Z-scheme heterojunction for highly efficient photosynthesis.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4000,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/aenm.202401873","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Photocatalytic oxygen reduction reaction (ORR) is an environmentally friendly and cost-effective approach for H2O2 synthesis. However, the current photosynthesis system suffers from sluggish kinetics, rapid recombination of photoexcited charge carriers, and weak redox potentials, resulting in unsatisfactory solar-to-chemical conversion efficiency. Herein, a Z-scheme heterojunction (UiO/IKCN) is constructed through coupling I−/K+ co-doped g-C3N4 (IKCN) with NH2-UiO-66, a typical metal-organic framework material. Under visible light irradiation, the optimal UiO/IKCN exhibits exceptional H2O2 production rates in pure water (13.3 mM g−1 h−1) and in isopropanol solution (72.6 mM g−1 h−1), that is 48.4 times higher than pristine CN in isopropanol (1.5 mM g−1 h−1). A high apparent quantum yield of 10.28% at 420 nm is achieved by UiO/IKCN, surpassing most previously reported values. The dominating role of two-electron ORR in H2O2 photosynthesis is elucidated in detail. The significantly enhanced photocatalytic activity can be attributed to the facilitated charge separation and Z-scheme charge transfer, which are unambiguously verified by stable-state surface photovoltage, transient photoluminescence, femtosecond transient absorption spectroscopy, in-situ irradiated X-ray photoelectron spectroscopy, and density functional theory calculations. This study represents the first exploration of H2O2 production using NH2-UiO-66 and provides insights into the rational design of Z-scheme heterojunction for highly efficient photosynthesis.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.