| Autre titre | Optical control of selectivity of high rate CO2 photoreduction via interband- or hot electron Z-scheme reaction pathways in Au-TiO2 plasmonic photonic crystal photocatalyst |
|---|
| DOI | Trouver le DOI : https://doi.org/10.1016/j.apcatb.2020.118644 |
|---|
| Auteur | Rechercher : Zeng, Sheng; Rechercher : Vahidzadeh, Ehsan; Rechercher : Vanessen, Collin G.; Rechercher : Kar, PiyushIdentifiant ORCID : https://orcid.org/0000-0001-9238-1418; Rechercher : Kisslinger, RyanIdentifiant ORCID : https://orcid.org/0000-0003-2456-396X; Rechercher : Goswami, Ankur; Rechercher : Zhang, Yun; Rechercher : Mahdi, Najia; Rechercher : Riddell, SaralynIdentifiant ORCID : https://orcid.org/0000-0002-5107-6086; Rechercher : Kobryn, Alexander E.1; Rechercher : Gusarov, Sergey1; Rechercher : Kumar, PawanIdentifiant ORCID : https://orcid.org/0000-0003-2804-9298; Rechercher : Shankar, KarthikIdentifiant ORCID : https://orcid.org/0000-0001-7347-3333 |
|---|
| Affiliation | - Conseil national de recherches du Canada. Nanotechnologie
|
|---|
| Format | Texte, Article |
|---|
| Sujet | heterogeneous catalysis; light trapping; plasmonic photocatalysis; density functional theory; FDTD simulations |
|---|
| Résumé | Photonic crystals consisting of TiO₂ nanotube arrays (PMTiNTs) with periodically modulated diameters were fabricated using a precise charge-controlled pulsed anodization technique. The PMTiNTs were decorated with gold nanoparticles (Au NPs) to form plasmonic photonic crystal photocatalysts (Au-PMTiNTs). A systematic study of CO₂ photoreduction performance on as-prepared samples was conducted using different wavelengths and illumination sequences. A remarkable selectivity of the mechanism of CO₂ photoreduction could be engineered by merely varying the spectral composition of the illumination sequence. Under AM1.5 G simulated sunlight (pathway#1), the Au-PMTiNTs produced methane (302 μmol gcat.⁻¹ h⁻¹) from CO2 with high selectivity (89.3 %). When also illuminated by a UV-poor white lamp (pathway#2), the Au-PMTiNTs produced formaldehyde (420 μmol gcat.⁻¹ h⁻¹) and carbon monoxide (323 μmol gcat.⁻¹ h⁻¹) with almost no methane evolved. We confirmed the photoreduction results by 13C isotope labeling experiments using GC[sbnd]MS. These results point to optical control of the selectivity of high-rate CO2 photoreduction through selection of one of two different mechanistic pathways. Pathway#1 implicates electron-hole pairs generated through interband transitions in TiO₂ and Au as the primary active species responsible for reducing CO₂ to methane. Pathway#2 involves excitation of both TiO₂ and surface plasmons in Au. Hot electrons produced by plasmon damping and photogenerated holes in TiO₂ proceed to reduce CO₂ to HCHO and CO through a plasmonic Z-scheme. |
|---|
| Date de publication | 2020-01-15 |
|---|
| Maison d’édition | Elsevier |
|---|
| Dans | |
|---|
| Langue | anglais |
|---|
| Publications évaluées par des pairs | Oui |
|---|
| Identificateur | S092633732030059X |
|---|
| Exporter la notice | Exporter en format RIS |
|---|
| Signaler une correction | Signaler une correction (s'ouvre dans un nouvel onglet) |
|---|
| Identificateur de l’enregistrement | 605e383c-5925-4edf-8814-2764938ff200 |
|---|
| Enregistrement créé | 2020-06-29 |
|---|
| Enregistrement modifié | 2020-06-29 |
|---|
