羧基表面修饰与钾离子层间调控双重优化的氮化碳用于增强CO2光还原性能
Dual-facet engineering of surface carboxyl functionalization and interlayer potassium ions regulation in carbon nitride for enhanced CO2 photoreduction
关晨 1廖宇龙 1向全军1
作者信息
- 1. State Key Laboratory of Electronic Thin Film and Integrated Devices,School of Electronic Science and Engineering,University of Electronic Science and Technology of China,Chengdu 610054,China
- 折叠
摘要
对石墨相氮化碳(g-C3N4)的表面和层间结构进行同时优化,可以显著提高其光生载流子分离效率.然而,将具有特定优势的改性策略有效整合,从而构建由体相到表面的电荷传输通道仍存在巨大挑战.在此,我们提出了一种利用羧基和钾离子共修饰g-C3N4的新方法,用于引导其动态电荷转移过程.具体而言,我们将羧基官能团修饰在表面,通过其吸电子效应产生的驱动力改善表面的载流子动力学.同时,我们将钾离子插入g-C3N4层间,通过连接相邻层间促进载流子的跨层传输.该双功能光催化剂在无需助催化剂或牺牲剂的气固体系中实现了高达17.93 μmol g-1 h-1的CO产出速率,比未改性的g-C3N4高出8.68倍.这项工作有望进一步加深我们对光催化剂材料体相和层间区域载流子定向迁移机制的理解.
Abstract
Simultaneous optimization of surface and in-terlayer characteristics of graphite-phase carbon nitride(g-C3N4)is crucial for enhanced photogenerated-carrier se-paration efficiency.Integration of distinct strategies with specific merits for constructing efficacious charge carrier transport pathways from bulk to surface faces challenges.Herein,we proposed a novel carboxyl functional group and potassium(K)ions co-modified g-C3N4 for steering dynamic charge transfer processes.Specifically,carboxyl functional groups were grafted to the surface to substantially improve charge carrier dynamics through the driving force induced by its electron-withdrawing effects.Concurrently,K ions were inserted into the interlayers of g-C3N4 to facilitate interlayer carrier transport by bridging adjacent layers.Such a bi-func-tional photocatalyst achieves 8.68-fold increase in CO yield compared wtih the pristine g-C3N4 without any cocatalyst or sacrificial agent.This work provides a profound discernment into the directional transport of charge carriers within the surface and interlayers,and presents a promising approach for rational design of photocatalysts with remarkably efficient solar energy conversion.
关键词
surface carboxyl functionalization/interlayer po-tassium ions regulation/charge carrier dynamics/carbon nitride/CO2 photoreductionKey words
surface carboxyl functionalization/interlayer po-tassium ions regulation/charge carrier dynamics/carbon nitride/CO2 photoreduction引用本文复制引用
基金项目
National Natural Science Foundation of China(22272019)
Sichuan Science and Technology Program(2022ZYD0039)
Sichuan Science and Technology Program(2022NSFSC1213)
Sichuan Science and Technology Program(2023NSFSC1069)
出版年
2024
NETL
NSTL
万方数据