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Ultrabroadband plasmon driving selective photoreforming of methanol under ambient conditions

Nasir Uddin, Zhehao Sun, Julien Langley, Haijiao Lu, Pengfei Cao, Ary Anggara Wibowo, Xinmao Yin, Chi Sin Tang, Hieu T. Nguyen, Jack D. Evans, Xinzhe Li, Xiaoliang Zhang, Marc Heggen, Rafal E. Dunin‐Borkowski, Andrew T. S. Wee, Haitao Zhao, Nicholas J. Cox, Zongyou Yin

2023Proceedings of the National Academy of Sciences16 citationsDOIOpen Access PDF

Abstract

Liquid methanol has the potential to be the hydrogen energy carrier and storage medium for the future green economy. However, there are still many challenges before zero-emission, affordable molecular H 2 can be extracted from methanol with high performance. Here, we present noble-metal-free Cu–WC/W plasmonic nanohybrids which exhibit unsurpassed solar H 2 extraction efficiency from pure methanol of 2,176.7 µmol g −1 h −1 at room temperature and normal pressure. Macro-to-micro experiments and simulations unveil that local reaction microenvironments are generated by the coperturbation of WC/W’s lattice strain and infrared-plasmonic electric field. It enables spontaneous but selective zero-emission reaction pathways. Such microenvironments are found to be highly cooperative with solar-broadband-plasmon-excited charge carriers flowing from Cu to WC surfaces for efficient stable CH 3 OH plasmonic reforming with C 3 -dominated liquid products and 100% selective gaseous H 2 . Such high efficiency, without any CO x emission, can be sustained for over a thousand-hour operation without obvious degradation.

Topics & Concepts

PlasmonMethanolMaterials scienceExcited stateSurface plasmon resonanceHydrogenChemical physicsPhotochemistryElectric fieldCharge carrierEnergy conversion efficiencyOptoelectronicsChemical engineeringNanotechnologyChemistryAtomic physicsNanoparticleOrganic chemistryPhysicsEngineeringQuantum mechanicsCopper-based nanomaterials and applicationsCatalytic Processes in Materials ScienceZnO doping and properties
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