Yifeng Xu, Xipeng Xin, Hexige Wuliji, Kai Ye, Qingdong Liu, Yiqiu Zhu, Kunpeng Zhao, Yang Ren, Xuefeng Song, Lian Gao
{"title":"通过低温熔盐辅助镁热还原实现全太阳光谱响应氮化碳","authors":"Yifeng Xu, Xipeng Xin, Hexige Wuliji, Kai Ye, Qingdong Liu, Yiqiu Zhu, Kunpeng Zhao, Yang Ren, Xuefeng Song, Lian Gao","doi":"10.1111/jace.20525","DOIUrl":null,"url":null,"abstract":"<p>The solar energy conversion efficiency of graphitic carbon nitride (GCN)-based photocatalysts is significantly hindered by the limited intrinsic absorption range and low carrier mobility of GCN. Herein, a novel carbon nitride (SC-CN) with exquisitely designed electronic band structure is proposed by continual stoichiometric manipulation, introducing wide dispersed midgap states for stepwise electron excitation. Importantly, the modulation of electronic structure paves the way for multilevel electron transitions, resulting in the full solar spectrum absorption covering a range of 250–2500 nm. Moreover, these defect levels markedly enhance the nonradiative relaxation in SC-CN, leading to a distinct photothermal effect where its temperature can be raised to 80°C under 100 mW cm<sup>−2</sup> near-infrared (NIR) light. Ultimately, a full solar conversion improvement for microcystin photoredox degradation is realized due to the synergetic interaction of photothermal effect and interfacial charge transfer in an SC-CN@GCN heterojunction.</p>","PeriodicalId":200,"journal":{"name":"Journal of the American Ceramic Society","volume":"108 7","pages":""},"PeriodicalIF":3.5000,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Full solar spectrum responsive carbon nitride enabled by low-temperature molten-salt-assisted magnesiothermic reduction\",\"authors\":\"Yifeng Xu, Xipeng Xin, Hexige Wuliji, Kai Ye, Qingdong Liu, Yiqiu Zhu, Kunpeng Zhao, Yang Ren, Xuefeng Song, Lian Gao\",\"doi\":\"10.1111/jace.20525\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The solar energy conversion efficiency of graphitic carbon nitride (GCN)-based photocatalysts is significantly hindered by the limited intrinsic absorption range and low carrier mobility of GCN. Herein, a novel carbon nitride (SC-CN) with exquisitely designed electronic band structure is proposed by continual stoichiometric manipulation, introducing wide dispersed midgap states for stepwise electron excitation. Importantly, the modulation of electronic structure paves the way for multilevel electron transitions, resulting in the full solar spectrum absorption covering a range of 250–2500 nm. Moreover, these defect levels markedly enhance the nonradiative relaxation in SC-CN, leading to a distinct photothermal effect where its temperature can be raised to 80°C under 100 mW cm<sup>−2</sup> near-infrared (NIR) light. Ultimately, a full solar conversion improvement for microcystin photoredox degradation is realized due to the synergetic interaction of photothermal effect and interfacial charge transfer in an SC-CN@GCN heterojunction.</p>\",\"PeriodicalId\":200,\"journal\":{\"name\":\"Journal of the American Ceramic Society\",\"volume\":\"108 7\",\"pages\":\"\"},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2025-03-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Ceramic Society\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1111/jace.20525\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, CERAMICS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Ceramic Society","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1111/jace.20525","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, CERAMICS","Score":null,"Total":0}
引用次数: 0
摘要
氮化石墨碳(GCN)基光催化剂的固有吸收范围有限,载流子迁移率低,严重阻碍了其太阳能转换效率的提高。本文通过连续化学计量操作,提出了一种具有精心设计的电子能带结构的新型氮化碳(SC-CN),引入了广泛分散的中隙态,用于逐步电子激发。重要的是,电子结构的调制为多层电子跃迁铺平了道路,从而实现了覆盖250 - 2500nm范围的全太阳光谱吸收。此外,这些缺陷水平显著增强了SC-CN的非辐射弛豫,导致了明显的光热效应,在100 mW cm - 2近红外(NIR)光下,SC-CN的温度可以提高到80°C。最终,由于在SC-CN@GCN异质结中光热效应和界面电荷转移的协同作用,实现了微囊藻毒素光氧化还原降解的完全太阳能转换改进。
Full solar spectrum responsive carbon nitride enabled by low-temperature molten-salt-assisted magnesiothermic reduction
The solar energy conversion efficiency of graphitic carbon nitride (GCN)-based photocatalysts is significantly hindered by the limited intrinsic absorption range and low carrier mobility of GCN. Herein, a novel carbon nitride (SC-CN) with exquisitely designed electronic band structure is proposed by continual stoichiometric manipulation, introducing wide dispersed midgap states for stepwise electron excitation. Importantly, the modulation of electronic structure paves the way for multilevel electron transitions, resulting in the full solar spectrum absorption covering a range of 250–2500 nm. Moreover, these defect levels markedly enhance the nonradiative relaxation in SC-CN, leading to a distinct photothermal effect where its temperature can be raised to 80°C under 100 mW cm−2 near-infrared (NIR) light. Ultimately, a full solar conversion improvement for microcystin photoredox degradation is realized due to the synergetic interaction of photothermal effect and interfacial charge transfer in an SC-CN@GCN heterojunction.
期刊介绍:
The Journal of the American Ceramic Society contains records of original research that provide insight into or describe the science of ceramic and glass materials and composites based on ceramics and glasses. These papers include reports on discovery, characterization, and analysis of new inorganic, non-metallic materials; synthesis methods; phase relationships; processing approaches; microstructure-property relationships; and functionalities. Of great interest are works that support understanding founded on fundamental principles using experimental, theoretical, or computational methods or combinations of those approaches. All the published papers must be of enduring value and relevant to the science of ceramics and glasses or composites based on those materials.
Papers on fundamental ceramic and glass science are welcome including those in the following areas:
Enabling materials for grand challenges[...]
Materials design, selection, synthesis and processing methods[...]
Characterization of compositions, structures, defects, and properties along with new methods [...]
Mechanisms, Theory, Modeling, and Simulation[...]
JACerS accepts submissions of full-length Articles reporting original research, in-depth Feature Articles, Reviews of the state-of-the-art with compelling analysis, and Rapid Communications which are short papers with sufficient novelty or impact to justify swift publication.