等离子体子
甲醇
材料科学
激发态
表面等离子共振
氢
光化学
电场
载流子
化学物理
能量转换效率
化学工程
纳米颗粒
纳米技术
光电子学
化学
原子物理学
有机化学
工程类
物理
量子力学
作者
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
标识
DOI:10.1073/pnas.2212075120
摘要
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 H2 can be extracted from methanol with high performance. Here, we present noble-metal-free Cu-WC/W plasmonic nanohybrids which exhibit unsurpassed solar H2 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 CH3OH plasmonic reforming with C3-dominated liquid products and 100% selective gaseous H2. Such high efficiency, without any COx emission, can be sustained for over a thousand-hour operation without obvious degradation.
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