Ultrabroadband plasmon driving selective photoreforming of methanol under ambient conditions.

Autor:	Uddin N; Research School of Chemistry, Australian National University, Canberra ACT 2601, Australia., Sun Z; Research School of Chemistry, Australian National University, Canberra ACT 2601, Australia.; Materials Interfaces Center, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, Guangdong 518055, P.R. China., Langley J; Research School of Chemistry, Australian National University, Canberra ACT 2601, Australia., Lu H; Research School of Chemistry, Australian National University, Canberra ACT 2601, Australia., Cao P; Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungzentrum Jülich GmbH 52428, Jülich, Germany., Wibowo A; Research School of Electrical, Energy and Materials Engineering, Australian National University, Canberra ACT 2601, Australia., Yin X; Physics Department, Shanghai Key Laboratory of High Temperature Superconductors, Shanghai University, Shanghai 200444, P.R. China.; Department of Physics, Faculty of Science, National University of Singapore, Singapore 117542, Singapore., Tang CS; Singapore Synchrotron Light Source, National University of Singapore, Singapore 117603, Singapore., Nguyen HT; Research School of Electrical, Energy and Materials Engineering, Australian National University, Canberra ACT 2601, Australia., Evans JD; Centre for Advanced Nanomaterials and Department of Chemistry, Adelaide, The University of Adelaide, Adelaide SA 5000, Australia., Li X; State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, P.R. China., Zhang X; Key Laboratory of Ocean Energy Utilization and Energy Conservation of Ministry of Education, School of Energy and Power Engineering, Dalian University of Technology, Dalian 116024, P.R. China., Heggen M; Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungzentrum Jülich GmbH 52428, Jülich, Germany., Dunin-Borkowski RE; Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungzentrum Jülich GmbH 52428, Jülich, Germany., Wee ATS; Department of Physics, Faculty of Science, National University of Singapore, Singapore 117542, Singapore., Zhao H; Materials Interfaces Center, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, Guangdong 518055, P.R. China., Cox N; Research School of Chemistry, Australian National University, Canberra ACT 2601, Australia., Yin Z; Research School of Chemistry, Australian National University, Canberra ACT 2601, Australia.
Jazyk:	angličtina
Zdroj:	Proceedings of the National Academy of Sciences of the United States of America [Proc Natl Acad Sci U S A] 2023 Jan 17; Vol. 120 (3), pp. e2212075120. Date of Electronic Publication: 2023 Jan 12.
DOI:	10.1073/pnas.2212075120
Abstrakt:	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.
Databáze:	MEDLINE
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