上海科技大学章跃标等研究团队最新研究提出一种新的用于太阳光驱动制氢的基于噻唑并[5,4-d]噻唑的供体-受体共价有机框架。 相关论文于2020年12月07日发表于国际顶尖学术期刊《德国应用化学》。

二维共价有机框架（COF）可以将光活性和电活性单元组装，作为收集太阳能转换的电子或空穴传输通道，但是目前COF材料的电子转移效率较低、载流子复合效应较强，抑制了太阳能驱动光催化反应的性能。

研究人员报道了一种新的供体-受体（D-A）系统，PyTz-COF是由富含电子的芘（Py）和缺电子的噻唑[5,4-D]噻唑（Tz）构成的。PyTz-COF具有双连续异质结，在超氧阴离子自由基介导的（芳甲基）胺偶联反应中表现出优异的光电性能、光催化能力以及在太阳光驱动下的析氢反应中的光电化学活性。尤其是，与RHE相比，PyTz-COF在0.2V下的光电流高达100 mA cm-2，并且可以达到2072.4 mmol g-1h-1的析氢速率。

该工作为高效、高活性太阳能收集与转换系统的设计铺平了道路。

附：英文原文

Title: Thiazolo[5,4‐d]thiazole‐Based Donor‐Acceptor Covalent Organic Frameworks for Sunlight‐Driven Hydrogen Evolution

Author: Wenqian Li, Xiaofeng Huang, Tengwu Zeng, Yahu A. Liu, Weibo Hu, Hui Yang, Yue-Biao Zhang, Ke Wen

Issue&Volume: 07 December 2020

Abstract: 2D covalent organic frameworks (COFs) could have well‐defined arrangements of photo‐ and electro‐active units that serve as electron or hole transport channels for solar energy harvesting and conversion, but their insufficient charge transfer and rapid charge recombination impede the sunlight‐driven photocatalytic performance. We report a new donor‐acceptor (D‐A) system, PyTz‐COF that was constructed from the electron‐rich pyrene (Py) and electron‐deficient thiazolo[5,4‐d]thiazole (Tz). With its bicontinuous heterojunction, PyTz‐COF demonstrated exceptional optoelectronic properties, photocatalytic ability in superoxide anion radical‐mediated coupling of (arylmethyl)amines and photoelectrochemical activity in sunlight‐driven hydrogen evolution. Remarkably, PyTz‐COF exhibited a photocurrent up to 100 mA cm‐2 at 0.2 V vs. RHE and could reach a hydrogen evolution rate of 2072.4 mmol g‐1 h‐1. This work is paving the way for reticular design of highly efficient and highly active D‐A systems for solar energy harvesting and conversion.

DOI: 10.1002/anie.202014408

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202014408