中国科学技术大学张晓东团队报道了用于高效CO₂化学固定的超薄面内异质结构。相关研究成果发表在2021年11月15日出版的国际知名学术期刊《德国应用化学》。

将二氧化碳（CO₂）化学固定为高附加值有机物被认为是大规模工业生产中具有竞争力和可行的方法，在该过程中需要具有促进CO₂活化能力的催化剂。

该文中，研究人员提出了一种平面内异质结构策略来构建Lewis酸碱位点，以高效激活CO₂。以超薄面内Cu₂O/Cu异质结构为原型，研究人员发现异质界面上的Lewis酸碱位点可以促进表面C和O的混合配位，其不仅加强了CO₂的吸附，而且有效地激活了惰性分子。原位漫反射红外傅里叶变换光谱（DRIFTS）和准原位X射线光电子能谱（XPS）表明，Lewis酸碱位点可以很容易地将CO₂活化为CO₂物种，这是CO₂固定的关键中间自由基。因此，丰富的Lewis酸碱位赋予Cu₂O/Cu纳米片以优异的碳酸二甲酯生成性能，在温和条件下，转化率高达28%，选择性接近100%。

该研究为CO₂固定反应提供了一个模型结构。

附：英文原文

Title: Ultrathin in-plane heterostructures for efficient CO2 chemical fixation

Author: Sen Jin, Wei Shao, Shichuan Chen, Lei Li, Shu Shang, Yan Zhao, Xiaodong Zhang, Yi Xie

Issue&Volume: 2021-11-15

Abstract: Chemical fixation of carbon dioxide (CO  2  ) into value-added organics is regarded as a competitive and viable method in large scale industrial production, during which the catalysts with promoting CO  2  activation ability are needed. Herein, we proposed an in-plane heterostructure strategy to construct Lewis acid–base sites for efficient CO  2  activation. By taking ultrathin in-plane Cu  2  O/Cu heterostructures as a prototype, we show that Lewis acid-base sites on heterointerface can facilitate a mixed C and O dual coordination on surface, which not only strengthen CO  2  adsorption, but also effectively activate the inert molecules. As revealed by  in-situ  diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and quasi  in-situ  X-ray photoelectron spectroscopy (XPS), Lewis acid-base sites could readily activate CO  2  to CO  2  –  species, which is the key intermediate radical for CO  2  fixation. As a result, abundant Lewis acid–base sites endow Cu  2  O/Cu nanosheets with excellent performances for dimethyl carbonate generation, a high conversion yield of 28% with nearly 100% selectivity under mild conditions. This study provides a model structure for CO  2  fixation reactions.

DOI: 10.1002/anie.202113411

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202113411