CO$_2$ Conversion in Cu-Pd based Disordered Network Metamaterials with Ultra-Small Mode Volume

TL;DR

This paper introduces Cu-Pd disordered network metamaterials with ultra-small mode volumes that enhance plasmonic light localization, enabling efficient CO$_2$ conversion and tunable reaction selectivity.

Contribution

It presents a scalable Cu-Pd plasmonic network platform with ultra-small mode volumes for plasmon-assisted catalysis, demonstrating tunable CO$_2$ conversion and selectivity.

Findings

Achieved light localization with mode volumes less than 8×10^{-24} m^3.

Observed CO$_2$ conversion rates up to 430 mmol g^{-1} h^{-1}.

Demonstrated tunable reaction selectivity by modifying network composition.

Abstract

Plasmons can drive chemical reactions by directly exciting intramolecular transitions. However, strong coupling of plasmons to single molecules remains a challenge as ultra-small mode volumes are required. In the presented work, we propose Cu-Pd plasmonic network metamaterials as a scalable platform for plasmon-assisted catalysis. Due to the absence of translational symmetry, these networks provide a unique plasmonic environment featuring a large local density of optical states and an unparalleled density of hotspots that effectively localizes light in mode volumes $V<8\cdot10^{-24}$ m$^3$. Catalytic performance tests during CO$_2$ conversion reveal production rates of up to 4.3$\cdot$10$^2$ mmol g$^{-1}$h$^{-1}$ and altered reaction selectivity under light illumination. Importantly, we show that the selectivity of the catalytic process can be tuned by modifying the network's chemical composition, offering a versatile approach to optimize reaction pathways.