ｇ－Ｃ３Ｎ４／半導体複合材料の構築と表界面制御による二酸化炭素光還元の高機能化

g-C3N4/半导体复合材料的构建及通过表面和界面控制增强二氧化碳光还原

• 批准号: 15F15070
• 负责人: 葉 金花
• 金额: $ 1.47万
• 依托单位: National Institute for Materials Science
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for JSPS Fellows
• 财政年份: 2015
• 资助国家: 日本
• 起止时间: 2015-07-29 至 2017-03-31
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-15F15070/
• 关键词: Photocatalysis; Carbon nitride; H2 evolution; CO2 reduction

The project is mainly focused on exploring highly efficient photocatalysts for chemical fuel production based on visible-light responsive organic semiconductor, i.e. carbon nitride. We have been devoted to enhance the charge carrier separation and transport through the following two pathways and have obtained significant progress:1) Constructing an imine-linked antenna-reaction center complex composed of low-molecular-weight carbon nitride and Co porphyrin, where the photo-generated electron-hole is separated more efficiently since electrons could be easily trapped by Co(II) to form Co(I) species and the active site immobilized on the C-N framework facilitated the redox photocatalytic reaction;2) Designing carbon nitride with enhanced in-planar ordering by controlling the self-assembly of heptazine precursors and calcination of the assembled precursors, where the intraplanar transport of the photo-generated charge carriers can be largely enhanced. It was found that the sub-micro rod-like morphology of the assembled heptazine precursor was well maintained during the poly-condensation without volumetric shrinkage in spite of different temperature-rise rates in the calcination process. The enhanced ordering within the graphitic planar and the induced excellent charge separation contributed to a tremendously improved H2 evolution rate of 420 umol/h under visible light (λ > 420 nm) with an apparent quantum efficiency of 8.9% at 420 nm, which is among the highest value for C3N4-related photocatalyst in the literature.

该项目主要致力于探索基于可见光响应有机半导体（即氮化碳）的用于化学燃料生产的高效光催化剂。我们致力于通过以下两条途径增强载流子的分离和传输，并取得了重大进展：1）构建了由低分子量氮化碳和钴卟啉组成的亚胺连接的天线反应中心复合物，其中电子很容易被Co（II）捕获形成Co（I）物质并固定活性位点，从而更有效地分离光生电子 - 空穴。 C-N骨架上的C-N骨架促进了氧化还原光催化反应；2）通过控制七嗪前驱体的自组装和组装前驱体的煅烧，设计具有增强面内有序性的氮化碳，其中光生载流子的面内传输可以大大增强。研究发现，尽管煅烧过程中的升温速率不同，但组装的七嗪前体在缩聚过程中仍能很好地保持亚微米棒状形态，而没有体积收缩。石墨平面内增强的有序性和诱导的优异的电荷分离使得可见光（λ > 420 nm）下的H2析出速率大大提高为420 umol/h，420 nm处的表观量子效率为8.9%，这是文献中C3N4相关光催化剂的最高值之​​一。

项目成果

New Function of Nanometals in Solar-to-Chemical Energy Conversion

纳米金属在太阳能到化学能转换中的新功能

• 发表时间: 2016
• 作者: Guixia Zhao;Hong Pang;Guigao Liu;Peng Li;Huimin Liu;Huabin Zhang;Li Shi;Jinhua Ye;Jinhua Ye
• 通讯作者: Jinhua Ye

Design and Construction of Nanomaterials System for Solar Fuel Production

太阳能燃料生产纳米材料系统的设计与构建

• 发表时间: 2016
• 作者: Huabin Zhang;Huimin Liu;Xianguang Meng;Thang Duy Dao;Tadaaki Nagao;and Jinhua Ye;Jinhua Ye
• 通讯作者: Jinhua Ye

In Situ Bond Modulation of Graphitic Carbon Nitride to Construct p-n Homojunctions for Enhanced Photocatalytic Hydrogen Production

• DOI: 10.1002/adfm.201602779
• 发表时间: 2016-10-04
• 期刊: ADVANCED FUNCTIONAL MATERIALS
• 影响因子: 19
• 作者: Liu, Guigao;Zhao, Guixia;Ye, Jinhua
• 通讯作者: Ye, Jinhua

Surface-plasmon-assisted photo-driven CO2 reduction catalyzed by nanometals

纳米金属催化的表面等离子体辅助光驱动二氧化碳还原

• 发表时间: 2016
• 作者: Huabin Zhang;Huimin Liu;Xianguang Meng;Thang Duy Dao;Tadaaki Nagao;and Jinhua Ye
• 通讯作者: and Jinhua Ye

New Materials and Strategy for Light Capture and Catalysis

光捕获和催化的新材料和策略

• 发表时间: 2016
• 作者: Huabin Zhang;Huimin Liu;Xianguang Meng;Thang Duy Dao;Tadaaki Nagao;and Jinhua Ye;Jinhua Ye;葉 金花
• 通讯作者: 葉 金花