揭示二维共价有机框架光催化的结构-活性关系: 从分子工程到高性能优化

doi:10.1016/S1872-2067(26)65021-8

摘要/Abstract

摘要： 面对全球的化石能源枯竭和日益恶化的环境污染问题, 急需开发可再生能源以应对这一挑战. 太阳能作为绿色环保的能源选择, 可被转化为可储存的二次能源. 光催化剂是太阳能转换二次能源过程中的关键材料, 而二维共价有机框架(2D-COF)作为一类由强共价键精确连接、具有原子级规整孔道和高度可定制性骨架的新兴晶态多孔聚合物, 已经从最初的结构设计奇迹, 迅速发展成为光催化领域不可或缺的关键材料平台.
本综述系统性地梳理了2D-COF从核心结构特性(如原子级精确的可设计孔道、极高的比表面积、卓越的物理化学稳定性以及可调控的光电性质)到光催化功能实现之间的内在逻辑链条. 本文重点阐释了上述特性的协同作用机制, 使其在光催化水分解、二氧化碳还原、有机合成及环境污染物降解等多个前沿领域取得一系列突破性进展成为可能, 充分彰显了其相较于传统无机材料与非晶态材料的独特性能优势. 本文不仅是对已有研究成果的汇编, 更是构建了一个从“分子结构设计”到“宏观光催化性能”的系统性认知框架. 深入剖析了如何通过前体单体连接方式的理性选择、官能团的精准植入以及堆叠方式的调控, 来定向优化2D-COF的光吸收范围、激子分离效率、电荷迁移速率以及表面反应活性, 从而建立了清晰的“结构-性能”构效关系. 本研究的核心理论贡献在于: 突破了传统“试错法”的研究范式, 为相关领域的研究者提供了系统化的理性设计指引, 实现了针对特定光催化反应的COF材料精准定制; 同时也为多孔材料领域提供了可移植的通用设计思路, 助力光催化材料研究由经验式探索向理性化设计转型升级.
尽管2D-COF材料展现出巨大的应用前景, 但其实际应用仍面临若干关键挑战: 一是在合成方法上, 发展绿色、温和、可放大的制备策略; 二是在性能优化上, 通过理论计算与先进表征相结合, 深入揭示微观机制, 指导材料能带结构与界面性质的精准调控; 三是在材料体系创新上, 探索2D-COF与无机半导体、金属配合物或分子催化剂的复合策略, 构建高效Z型或异质结光催化系统; 四是在应用拓展上, 推进COF基光催化材料在集成化器件中的实际应用, 并探索其在人工光合作用、氮气还原等新兴领域的应用潜力. 展望未来, 随着合成方法学、先进表征技术与理论模拟的深度融合, 2D-COF材料有望超越基础研究的范畴, 成为应对能源危机、环境污染及实现“双碳”目标等全球性挑战的核心材料解决方案之一.

关键词: 光催化剂, 二维多孔材料, 共价有机框架, 构性关系, 反应机理

Abstract: Faced with national fossil energy depletion and worsening environmental pollution, the shift to renewable energy is urgent. Solar energy, as a green and eco-friendly option, is converted into storable secondary energy to achieve carbon neutrality. Photocatalysts are key for this solar-to-secondary energy conversion, and two-dimensional covalent organic frameworks (2-D COFs) are highly promising candidates due to their large specific surface area, excellent stability, and flexible structural design. This paper comprehensively reviews the structural design of 2-D COFs, photocatalytic mechanisms, and the structure-function relationship. It also explores their applications in six fields: carbon dioxide reduction for carbon mitigation, uranium extraction from seawater for resource security, hydrogen peroxide synthesis as an eco-friendly alternative, organic transformation with high selectivity, and pollutant degradation for environmental improvement and hydrogen synthesis as a renewable energy. However, 2-D COFs face challenges in the photocatalytic field, including a limited light absorption range and relatively low charge separation efficiency. These issues hinder their full-scale application and performance optimization. Despite these obstacles, this study provides key insights and future directions for advancing 2-D COFs, aiming to inspire further research to overcome current limitations and unlock their full potential.

Key words: Photocatalyst, Two-dimensional porous materials, Covalent organic frameworks, Structure-activity relationship, Reaction mechanism

刘家英, 方煜. 揭示二维共价有机框架光催化的结构-活性关系: 从分子工程到高性能优化[J]. 催化学报, DOI: 10.1016/S1872-2067(26)65021-8.

Jiaying Liu, Yu Fang. Unraveling structure-activity relationships in 2-D covalent organic frameworks for photocatalysis: From molecular engineering to high-performance optimization[J]. Chinese Journal of Catalysis, DOI: 10.1016/S1872-2067(26)65021-8.

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