TY - JOUR
T1 - Phase and sulfur vacancy engineering in cadmium sulfide for boosting hydrogen production from catalytic plastic waste photoconversion
AU - Nguyen, Thanh Tam
AU - Hidalgo-Jiménez, Jacqueline
AU - Sauvage, Xavier
AU - Saito, Katsuhiko
AU - Guo, Qixin
AU - Edalati, Kaveh
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2025/1/15
Y1 - 2025/1/15
N2 - Cadmium sulfide (CdS) is a well-known low-bandgap photocatalyst, but its efficiency is often hindered by rapid photo-generated carrier recombination and a limited number of active catalytic sites. To overcome these challenges, this study introduces an efficient CdS photocatalyst through a novel strategy combining metastable-to-stable phase transformation and sulfur vacancy generation. This strategy integrates hydrothermal treatment and a high-pressure process to create sulfur vacancies, which serve as active catalytic sites, within a thermodynamically stable wurtzite (hexagonal) phase known for its superior photocatalytic properties. The resulting CdS photocatalyst demonstrates exceptional performance in photoreforming for hydrogen production and the conversion of polyethylene terephthalate (PET) plastic into valuable materials. Compared to commercial CdS catalysts, this new material shows a 23-fold increase in both hydrogen production and plastic degradation without the need for co-catalysts. Quenching experiments reveal that holes and hydroxyl radicals play crucial roles in the photoreforming process of this vacancy-rich CdS. First-principles calculations via density functional theory (DFT) indicate that the hexagonal phase possesses a lower bandgap and it exhibits further bandgap narrowing with the introduction of sulfur vacancies. These findings not only present an innovative approach to CdS processing but also highlight the critical role of sulfur vacancies as effective defects for the catalytic photoreforming of microplastics.
AB - Cadmium sulfide (CdS) is a well-known low-bandgap photocatalyst, but its efficiency is often hindered by rapid photo-generated carrier recombination and a limited number of active catalytic sites. To overcome these challenges, this study introduces an efficient CdS photocatalyst through a novel strategy combining metastable-to-stable phase transformation and sulfur vacancy generation. This strategy integrates hydrothermal treatment and a high-pressure process to create sulfur vacancies, which serve as active catalytic sites, within a thermodynamically stable wurtzite (hexagonal) phase known for its superior photocatalytic properties. The resulting CdS photocatalyst demonstrates exceptional performance in photoreforming for hydrogen production and the conversion of polyethylene terephthalate (PET) plastic into valuable materials. Compared to commercial CdS catalysts, this new material shows a 23-fold increase in both hydrogen production and plastic degradation without the need for co-catalysts. Quenching experiments reveal that holes and hydroxyl radicals play crucial roles in the photoreforming process of this vacancy-rich CdS. First-principles calculations via density functional theory (DFT) indicate that the hexagonal phase possesses a lower bandgap and it exhibits further bandgap narrowing with the introduction of sulfur vacancies. These findings not only present an innovative approach to CdS processing but also highlight the critical role of sulfur vacancies as effective defects for the catalytic photoreforming of microplastics.
KW - Cadmium sulfide (CdS)
KW - Microplastics
KW - Phase transformation
KW - Photocatalysis
KW - Plastic waste degradation
KW - Sulfur vacancy
UR - http://www.scopus.com/inward/record.url?scp=85212548423&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85212548423&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2024.158730
DO - 10.1016/j.cej.2024.158730
M3 - Article
AN - SCOPUS:85212548423
SN - 1385-8947
VL - 504
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 158730
ER -