基于金属-有机框架同分异构体构建MOFs相结用以增强CO2光还原活性

扫码查看

原文链接

NETL
NSTL
万方数据

中文摘要：利用太阳能将CO2光转化为化学燃料是前沿研究的热点.当前,科研的重点在于开发和优化各类光催化材料的性能.异质结构不仅用于增强无机半导体催化剂的活性,而且用于金属-有机框架(MOFs)光催化剂的构建.随着异质结技术的不断进步,新的相结概念应运而生.尽管关于无机半导体中的相结研究已取得一定进展,但是MOFs相结结构的探索尚处于起步阶段.本文中,我们成功设计并构建了一种具有卓越光催化CO2还原性能的MOFs相结杂化材料.这种材料由具有高度连接性的卟啉配体(TCPP-Ni)与Zr6团簇紧密结合而成,在溶剂热反应条件下,PCN-222-Ni能够快速且均匀地成核.通过精准调控调节剂的用量,我们实现了同分异构体PCN-224-Ni在类似条件下较慢的晶体形成过程.最终制得的P@P杂化材料展现出高表面积、多孔性和卓越的结晶度.由于PCN-222-Ni和PCN-224-Ni之间的带隙匹配,光生载流子的分离和迁移得以促进,从而使P@P杂化材料展现出卓越的光还原CO2性能.这一重大突破不仅标志着MOFs相结结构研究的重大进展,还拓宽了 MOFs相结在CO2光转化领域的应用前景.

外文标题：Assembling phase-junctions based on metal-organic framework polymophism for enhanced overall CO2 photoreduction activities

外文摘要：The conversion of solar energy into chemical fuels stands at the forefront of promising applications for metal-organic frameworks(MOFs),but the rapid re-combination of photo-induced charge carriers within these frameworks poses a significant challenge to their photo-catalytic performance.Despite heterojunction construction has potential as a viable approach,its synthesis involves con-siderable complexity.Here,we present a distinct and well-defined phase junction based on polymorphic MOFs,achieved through an efficient one-pot synthesis process.This work not only paves the way for a robust platform for designing so-phisticated MOFs complexes,but also illuminates the intricate hierarchical structure-function dynamics inherent in MOFs.The fabricated PCN-222-Ni@PCN-224-Ni(P@P)hybrid ma-terial exhibits extensive surface area,a porous matrix,and superior crystallinity.The harmonious alignment of the band-gap between PCN-222-Ni and PCN-224-Ni,establishing a phase junction for type-Ⅱ carrier transfer,endows the re-sultant photocatalysts with exceptional visible-light-induced photoreduction capabilities for CO2,along with augmented stability.This significant advancement represents a significant milestone in the applications of MOFs,especially in harnes-sing solar energy for the production of sustainable chemical fuels through the process of CO2 photo-conversion.

外文关键词：

MOFs polymorphismphase-junctionsphoto-catalytic CO2 reduction

作者：

黄海波、李兰、王瑞、AR Mahammed Shaheer、刘天赋、刘海雄、曹荣

展开 >

作者单位：

School of Environmental Science and Engineering,Qingdao University,Qingdao 266071,China

State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,China

University of Chinese Academy of Sciences,Chinese Academy of Sciences,Beijing 100049,China

College of Materials and Chemistry,China Jiliang University,Hangzhou 310018,China

展开 >

关键词：

MOFs polymorphism phase-junctions photo-catalytic CO2 reduction

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaShandong Provincial Natural Science FoundationTechnology Support Program for Youth Innovation Team of Shandong Higher Education InstitutionsPostdoctoral Application Project of Qingdao

项目编号：

22201020052207124622033008ZR2023QB1732023KJ225QHBSH20230102024

出版年：

2024

DOI：

10.1007/s40843-024-2885-0

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(6)