Promoted surface charge density from interlayer Zn-N4 configuration in carbon nitride for enhanced CO2 photoreduction

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外文摘要：The solar-driven reduction of CO2 into valuable products is a promising method to alleviate global environmental problems and energy crises.However,the low surface charge density limits the photocatalytic conversion performance of CO2.Herein,a polymeric carbon nitride(PCN)photocatalyst with Zn single atoms(Zn1/CN)was designed and synthesized for CO2 photoreduction.The results of the CO2 photoreduction studies show that the CO and CH4 yields of Zn1/CN increased fivefold,reaching 76.9 and 22.9 pmol/(g·h),respectively,in contrast to the unmodified PCN.Ar+plasma-etched X-ray photoelectron spectroscopy and synchrotron radiation-based X-ray absorption fine structure results reveal that Zn single atom is mainly present in the interlayer space of PCN in the Zn-N4 configuration.Photoelectrochemical characterizations indicate that the interlayer Zn-N4 configuration can amplify light absorption and establish an interlayer charge transfer channel.Light-assisted Kelvin probe force microscopy confirms that more photogenerated electrons are delivered to the catalyst surface through interlayer Zn-N4 configuration,which increases its surface charge density.Further,in-situ infrared spectroscopy combined with density functional theory calculation reveals that promoted surface charge density accelerates key intermediates(*COOH)conversion,thus achieving efficient CO2 conversion.This work elucidates the role of internal single atoms in catalytic surface reactions,which provides important implications for the design of single-atom catalysts.

外文关键词：

single-atom catalystsphotocatalytic CO2 reductioninterlayer modificationcharge transfer dynamicssurface charge density

作者：

Xianjin Shi、Yu Huang、Gangqiang Zhu、Wei Peng、Meijuan Chen

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作者单位：

State Key Laboratory of Loess and Quaternary Geology(SKLLQG),Key Laboratory of Aerosol Chemistry and Physics,Institute of Earth Environment,Chinese Academy of Sciences,Xi'an 710061,China

Center of Excellence in Quaternary Science and Global Change,Chinese Academy of Sciences,Xi'an 710061,China

University of Chinese Academy of Sciences,Beijing 100049,China

School of Physics and Information Technology,Shaanxi Normal University,Xi'an 710062,China

School of Human Settlements and Civil Engineering,Xi'an Jiaotong University,Xi'an 710049,China

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基金：

Strategic Priority Research Program of the Chinese Academy of Sciences,ChinaStrategic Priority Research Program of the Chinese Academy of Sciences,ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaCAS Youth Interdisciplinary Team

项目编号：

XDA23010300XDA230100005187864441573138

出版年：

2024

DOI：

10.1007/s12274-023-6079-y

纳米研究(英文版)

CSTPCD

ISSN：

年,卷(期)：2024.17(4)

参考文献量51