AuCu双金属合金修饰共价有机框架用于高效光催化析氢
Bimetallic AuCu Alloy Decorated Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Production
杨文秀 1张金锋 2徐全龙 1杨云 1张礼杰1
作者信息
- 1. 温州大学,化学与材料工程学院,温州市先进能源存储与转化重点实验室,浙江 温州 325027
- 2. 淮北师范大学,物理与电子信息学院,污染物敏感材料与环境修复安徽省重点实验室,安徽 淮北 235000
- 折叠
摘要
共价有机框架(COFs)是一种具有π-π共轭结构和分子结构可调的晶体多孔有机材料,在光催化领域具有广阔的应用前景.然而,未改性的COFs材料具有反应动力学缓慢的缺点,因此需要引入助催化剂以降低其表面催化反应的势垒,从而加速反应过程.此工作中,采用双金属合金作为助催化剂,以提高COFs的光催化析氢性能.通过调控AuCu合金的比例,发现Au1Cu5/COF-TpPa具有最高的光催化产氢速率(8.24 mmol·g-1·h-1),甚至高于Pt修饰的COF-TpPa的产氢速率(6.51 mmol·g-1·h-1).经过系统性的表征测试和理论计算分析,Au1Cu5/COF-TpPa表现出高的载流子分离效率和低的H*生成能垒,从而具有高的光催化性能.本研究为利用双金属合金改性COF基光催化剂奠定了理论基础.
Abstract
Covalent organic frameworks(COFs)represent a kind of novel crystalline porous organic substances with extended π-conjugation framework and tunable structures,which display great promise in photocatalysis.However,unadorned COFs suffer from sluggish reaction kinetics,and a cocatalyst is essentially needed to reduce the activation barrier toward specific surface reaction and accelerate reaction kinetics.In this work,bimetallic alloys serving as co-catalysts were decorated on COFs to enhance the photocatalytic hydrogen evolution performance.By precisely-tuning the ratio of AuCu alloy,the resultant Au1Cu5/COF-TpPa displays the highest photocatalytic hydrogen generation rate(8.24 mmol·g-1·h-1),even surpassing the Pt modified COF-TpPa(6.51 mmol·h-1·g-1).According to the systematic characterizations and theoretical calculation,Au1Cu5/COF-TpPa exhibits the significantly enhanced charge carrier separation efficiency and reduced H* formation energy barrier,thus possessing high photocatalytic performance.This work affords a valuable approach to advancing COF-based photocatalysts by employing bimetallic alloy cocatalysts.
关键词
光催化/析氢/共价有机框架/双金属助催化剂Key words
Photocatalysis/H2 generation/Covalent organic framework/Bimetallic cocatalyst引用本文复制引用
基金项目
国家自然科学基金(52073263)
国家自然科学基金(52171145)
国家自然科学基金(21905209)
出版年
2024
国家科技期刊平台
NSTL
万方数据