Plasmonic nanoreactors regulating selective oxidation by energetic electrons and nanoconfined thermal fields

Chao Zhan; Qiu-Xiang Wang; Jun Yi; Liang Chen; De-Yin Wu; Ye Wang; Zhao-Xiong Xie; Martin Moskovits; Zhong-Qun Tian

doi:10.1126/sciadv.abf0962

Plasmonic nanoreactors regulating selective oxidation by energetic electrons and nanoconfined thermal fields

Sci Adv. 2021 Mar 5;7(10):eabf0962. doi: 10.1126/sciadv.abf0962. Print 2021 Mar.

Authors

Chao Zhan¹, Qiu-Xiang Wang¹, Jun Yi¹, Liang Chen¹, De-Yin Wu¹, Ye Wang¹, Zhao-Xiong Xie², Martin Moskovits^{2

3}, Zhong-Qun Tian²

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen 361005, China.
² State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen 361005, China. zqtian@xmu.edu.cn moskovits@chem.ucsb.edu zxxie@xmu.edu.cn.
³ Department of Chemistry, University of California, Santa Barbara, Santa Barbara, CA 93106, USA.

Abstract

Optimizing product selectivity and conversion efficiency are primary goals in catalysis. However, efficiency and selectivity are often mutually antagonistic, so that high selectivity is accompanied by low efficiency and vice versa. Also, just increasing the temperature is very unlikely to change the reaction pathway. Here, by constructing hierarchical plasmonic nanoreactors, we show that nanoconfined thermal fields and energetic electrons, a combination of attributes that coexist almost uniquely in plasmonic nanostructures, can overcome the antagonism by regulating selectivity and promoting conversion rate concurrently. For propylene partial oxidation, they drive chemical reactions by not only regulating parallel reaction pathways to selectively produce acrolein but also reducing consecutive process to inhibit the overoxidation to CO₂, resulting in valuable products different from thermal catalysis. This suggests a strategy to rationally use plasmonic nanostructures to optimize chemical processes, thereby achieving high yield with high selectivity at lower temperature under visible light illumination.

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