Full-spectrum nonmetallic plasmonic carriers for efficient isopropanol dehydration.

Lu, Changhai; You, Daotong; Li, Juan; Wen, Long; Li, Baojun; Guo, Tuan; Lou, Zaizhu

Plasmonic hot carriers have the advantage of focusing, amplifying, and manipulating optical signals via electron oscillations which offers a feasible pathway to influence catalytic reactions. However, the contribution of nonmetallic hot carriers and thermal effects on the overall reactions are still unclear, and developing methods to enhance the efficiency of the catalysis is critical. Herein, we proposed a new strategy for flexibly modulating the hot electrons using a nonmetallic plasmonic heterostructure (named W18O49-nanowires/reduced-graphene-oxides) for isopropanol dehydration where the reaction rate was 180-fold greater than the corresponding thermocatalytic pathway. The key detail to this strategy lies in the synergetic utilization of ultraviolet light and visible-near-infrared light to enhance the hot electron generation and promote electron transfer for C-O bond cleavage during isopropanol dehydration reaction. This, in turn, results in a reduced reaction activation barrier down to 0.37 eV (compared to 1.0 eV of thermocatalysis) and a significantly improved conversion efficiency of 100% propylene from isopropanol. This work provides an additional strategy to modulate hot carrier of plasmonic semiconductors and helps guide the design of better catalytic materials and chemistries. A nonmetallic plasmonic heterostructure of W18O49 nanowires on reduced-graphene oxide is reported for the efficient dehydration of isopropanol to 100% propylene. The energy barrier is found to be reduced under full-spectrum irradiation.

PLASMONICS; HOT carriers; DEHYDRATION reactions; ISOPROPYL alcohol; ACTIVATION energy; DEHYDRATION

Nature Communications, 2022, Vol 13, Issue 1, p1

2041-1723

Academic Journal

10.1038/s41467-022-34738-z