Anion-Programmable Poly(Ionic Liquid) Nanocone Antennas for Tunable and Efficient Solar CO2 Photoconversion

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Abstract
Au/TiO2 is a promising photocatalyst for CO2 reduction, yet its performance is often limited by inefficient light utilization and insufficient local CO2 availability. Here, we present an integrated photocatalytic platform by embedding Au/TiO2 nanoparticles within imidazolium poly(ionic liquid) (PIL) nanocone arrays. The nanocone architecture provides broadband light harvesting with > 99% absorptivity, while the imidazolium PIL enriches CO2 near the catalytic sites, enabling synergistic enhancement of CO2 photoreduction. The intrinsic counter-anion exchangeability of the PIL further enables programmable regulation of the overall catalytic activity and product formation selectivity. By optimizing the counter anion and water supply, the system selectively produces CO (124.89 μmol·g–1·h–1, 94.2% selectivity) or CH4 (137.75 μmol·g–1·h–1, 100% selectivity). Metalloporphyrin counter anions additionally enable C2 product formation, while functional catalytic anions allow cascade conversion of CO2 into polymeric products. This work demonstrates an integrated strategy that couples light management, substrate enrichment, and reaction programmability for efficient and versatile solar-driven CO2 conversion.
Funding Information
  • Ministry of Science and Technology of the People's Republic of China (2013CB834502)
  • Ministry of Science and Technology of the People's Republic of China (2017YFA0204501)
  • Ministry of Science and Technology of the People's Republic of China (2022YFA1505900)

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