中国科学院大连化学物理研究所吴凯丰课题组实现了使用无铅纳米晶体的近红外光子上转换和太阳能合成。这一研究成果于2023年2月6日发表在国际顶尖学术期刊《自然—光子学》上。
该研究团队报道了锌掺杂CuInSe2纳米晶体作为一种低成本和无铅的替代品，实现了近红外到黄色的上转换，外部量子效率达到16.7%。当直接与光氧化还原催化结合时，该系统可以实现高效的近红外驱动的有机合成和聚合，从而解决了纳米晶体敏化上转化的重吸收损失问题。
此外，这些纳米晶体的宽带光捕获可以在室内阳光下进行非常快速的反应。将“太阳合成”的范围扩大到近红外，可能会实现一个世纪以来利用阳光进行高附加值化学转化的梦想。
研究人员表示，近红外到可见光的光子上转换具有广泛的应用前景。目前用于该光谱窗口的三态氟离子上转换的光敏剂通常含有贵金属或有毒元素，效率相对较低。虽然胶体纳米晶体已经成为多功能光敏剂，但唯一发现用于近红外上转换的纳米晶体家族是剧毒的硫族铅。
附：英文原文
Title: Near-infrared photon upconversion and solar synthesis using lead-free nanocrystals
Author: Liang, Wenfei, Nie, Chengming, Du, Jun, Han, Yaoyao, Zhao, Guohui, Yang, Fan, Liang, Guijie, Wu, Kaifeng
Issue&Volume: 2023-02-06
Abstract: Near-infrared-to-visible photon upconversion holds great promise for a diverse range of applications. Current photosensitizers for triplet-fusion upconversion across this spectral window often contain either precious or toxic elements and have relatively low efficiencies. Although colloidal nanocrystals have emerged as versatile photosensitizers, the only family of nanocrystals discovered for near-infrared upconversion is the highly toxic lead chalcogenides. Here we report zinc-doped CuInSe2 nanocrystals as a low-cost and lead-free alternate, enabling near-infrared-to-yellow upconversion with an external quantum efficiency reaching 16.7%. When directly merged with photoredox catalysis, this system enables efficient near-infrared-driven organic synthesis and polymerization, which in turn solves the issue of reabsorption loss for nanocrystal-sensitized upconversion. Moreover, the broadband light capture of these nanocrystals enables very rapid reactions under indoor sunlight. Extending the reach of ‘solar synthesis’ into the near-infrared may realize the century-long dream of conducting high-added-value chemical transformations using sunlight.
DOI: 10.1038/s41566-023-01156-6
Source: https://www.nature.com/articles/s41566-023-01156-6