Abstract
Monitoring of interfacial electron transfer (ET) in situ is important to understand the ET mechanism and designing efficient photocatalysts. We describe herein a mass spectrometric approach to investigate the ultrafast transfer of photoelectrons that are generated by ultraviolet irradiation on surfaces of semiconductor nanoparticles or crystalline facets. The mass spectrometric approach can not only untargetedly detect various intermediates but also monitor their reactivity through associative or dissociative photoelectron capture dissociation, as well as electron detachment dissociation of adsorbed molecules. Proton-coupled electron transfer and proton-uncoupled electron transfer with radical initiated polymerization or hydroxyl radical abstraction have been unambiguously demonstrated with the mass spectrometric approach. Active crystalline facets of titanium dioxide for photocatalytic degradation of juglone and organochlorine dichlorodiphenyltrichloroethane are visualized with mass spectrometry imaging based on ion scanning and spectral reconstruction. This work provides a new technique for studying photo-electric properties of various materials.
Highlights
Monitoring of interfacial electron transfer (ET) in situ is important to understand the ET mechanism and designing efficient photocatalysts
We have reported a new ionization method based on interfacial photoelectron transfer for mass spectrometric imaging[16]
Compared with the general setup of a microscopic fluorescence imaging approach shown in Fig. 1a, by which only predicted species are detected, the mass spectrometry-based approach takes the full scan manner and all ions except radicals and neutral species are detected
Summary
Monitoring of interfacial electron transfer (ET) in situ is important to understand the ET mechanism and designing efficient photocatalysts. We describe a mass spectrometric approach to investigate the ultrafast transfer of photoelectrons that are generated by ultraviolet irradiation on surfaces of semiconductor nanoparticles or crystalline facets. The mass spectrometric approach can untargetedly detect various intermediates and monitor their reactivity through associative or dissociative photoelectron capture dissociation, as well as electron detachment dissociation of adsorbed molecules. Active crystalline facets of titanium dioxide for photocatalytic degradation of juglone and organochlorine dichlorodiphenyltrichloroethane are visualized with mass spectrometry imaging based on ion scanning and spectral reconstruction. A mass spectrometric approach was designed to untargetedly detect products along with intermediates of photocatalytic reactions and visualize active crystalline facets. The proposed mass spectrometric approach has been applied to investigate photocatalytic reactions of juglone and organochlorine 4, 40-dichlorodiphenyltrichloroethane (DDT) on surfaces of semiconductor nanoparticles. It is shown that this mass spectrometric approach should be able to provide a new way for exploring photo-electric properties of various materials
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