原子级手性金属氧化物光催化的自旋选择。

IF 14.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES Nature Communications Pub Date : 2023-07-28 DOI:10.1038/s41467-023-40367-x
Minhua Ai, Lun Pan, Chengxiang Shi, Zhen-Feng Huang, Xiangwen Zhang, Wenbo Mi, Ji-Jun Zou
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引用次数: 1

摘要

自旋自由度是提高光催化载流子动力学和表面反应动力学的重要参数。研究表明,ZnO的手性结构可以诱导自旋选择性效应,从而提高光催化性能。以手性蛋氨酸分子为对称性破缺剂合成的ZnO晶体具有层次手性。磁圆二色性光谱和磁导探针原子力显微测量表明,手性结构在光致载流子中起自旋过滤器的作用,并诱导自旋极化。极化载流子不仅具有较长的载流子寿命,而且在反应过程中增加了三重态副产物而不是单重态副产物。因此,与非手性ZnO相比,左手性和右手性ZnO的光催化O2生成活性分别高2.0倍和1.9倍,污染物光降解活性分别高2.5倍和2.0倍。这项工作为操纵金属氧化物中电子自旋相关氧化还原催化的自旋特性提供了一种可行的策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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Spin selection in atomic-level chiral metal oxide for photocatalysis.

The spin degree of freedom is an important and intrinsic parameter in boosting carrier dynamics and surface reaction kinetics of photocatalysis. Here we show that chiral structure in ZnO can induce spin selectivity effect to promote photocatalytic performance. The ZnO crystals synthesized using chiral methionine molecules as symmetry-breaking agents show hierarchical chirality. Magnetic circular dichroism spectroscopic and magnetic conductive-probe atomic force microscopic measurements demonstrate that chiral structure acts as spin filters and induces spin polarization in photoinduced carriers. The polarized carriers not only possess the prolonged carrier lifetime, but also increase the triplet species instead of singlet byproducts during reaction. Accordingly, the left- and right-hand chiral ZnO exhibit 2.0- and 1.9-times higher activity in photocatalytic O2 production and 2.5- and 2.0-times higher activities in contaminant photodegradation, respectively, compared with achiral ZnO. This work provides a feasible strategy to manipulate the spin properties in metal oxides for electron spin-related redox catalysis.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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