Operando NMR spectroscopic analysis of proton transfer in heterogeneous photocatalytic reactions
Xue Lu Wang,
Wenqing Liu,
Yan-Yan Yu,
Yanhong Song,
Wen Qi Fang,
Daxiu Wei,
Xue-Qing Gong (),
Ye-Feng Yao () and
Hua Gui Yang ()
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Xue Lu Wang: Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology
Wenqing Liu: Shanghai Key Laboratory of Magnetic Resonance, East China Normal University
Yan-Yan Yu: Key Laboratory for Advanced Materials, Centre for Computational Chemistry, Research Institute of Industrial Catalysis, East China University of Science and Technology
Yanhong Song: Shanghai Key Laboratory of Magnetic Resonance, East China Normal University
Wen Qi Fang: Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology
Daxiu Wei: Shanghai Key Laboratory of Magnetic Resonance, East China Normal University
Xue-Qing Gong: Key Laboratory for Advanced Materials, Centre for Computational Chemistry, Research Institute of Industrial Catalysis, East China University of Science and Technology
Ye-Feng Yao: Shanghai Key Laboratory of Magnetic Resonance, East China Normal University
Hua Gui Yang: Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology
Nature Communications, 2016, vol. 7, issue 1, 1-7
Abstract:
Abstract Proton transfer (PT) processes in solid–liquid phases play central roles throughout chemistry, biology and materials science. Identification of PT routes deep into the realistic catalytic process is experimentally challenging, thus leaving a gap in our understanding. Here we demonstrate an approach using operando nuclear magnetic resonance (NMR) spectroscopy that allows to quantitatively describe the complex species dynamics of generated H2/HD gases and liquid intermediates in pmol resolution during photocatalytic hydrogen evolution reaction (HER). In this system, the effective protons for HER are mainly from H2O, and CH3OH evidently serves as an outstanding sacrificial agent reacting with holes, further supported by our density functional theory calculations. This results rule out controversy about the complicated proton sources for HER. The operando NMR method provides a direct molecular-level insight with the methodology offering exciting possibilities for the quantitative studies of mechanisms of proton-involved catalytic reactions in solid–liquid phases.
Date: 2016
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms11918
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DOI: 10.1038/ncomms11918
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