RSC_Energy Environmental Science _ cover ย Picture
01 April 2020, Issue 4,ย
Page 1041 to 1290ย
A tailored oxide interface creates dense Pt single-atom catalysts with high catalytic activity
Highly reactive dense Pt single-atoms stabilized on an oxide support can resolve a grand challenge in the economic use of Pt in catalysis. The maximized number density of reaction sites provided by dense Pt single-atoms guarantees the improved catalytic performance of Pt combined with high efficiency. By manipulating the chemical nature of multi-component interfaces, we synthesized CO-tolerant dense Pt single-atoms highly reactive for the CO oxidation reaction, which governs the key steps for chemical energy conversion and emission control. The addition of 1 wt% of Ce to TiO2 support particles creates a CeOxโTiO2 interface that stabilizes Pt single-atoms by strong electronic interactions. Dense Pt single-atoms formed on CeOx/TiO2 oxides exhibit 15.1 times greater specific mass activity toward CO oxidation at 140 ยฐC compared with a bare Pt/TiO2 catalyst. We elaborate how the CeOxโTiO2 interfaces activate the interface-mediated Marsโvan Krevelen mechanism of CO oxidation and protect Pt single-atoms from CO-poisoning. Through a comprehensive interpretation of the formation and activation of dense Pt single-atoms using operando X-ray absorption spectroscopy, density functional theory calculations, and experimental catalyst performance tests, we provide a key that enables the catalytic performance of noble metal single-atom catalysts to be optimized by atomic-scale tuning of the metalโsupport interface.
- โขMi Yoo
- Young-Sang
- ย Hyunwoo Ha
- ย Siwon Lee
- ย Jin-Seok Choi
- ย Sunyoung Oh
- ย Eunji Kang
- ย ย Hyuk Choi
- ย ย Hyesung An
- ย ย Kug-Seung Lee
- ย Jeong Young Park
- ย Richard Celestre
- ย ย Matthew A. Marcus
- ย ย Kasra Nowrouzi
- ย ย Doug Taube
- ย ย David A. Shapiro
- ย ย WooChul Jung
- ย ย Chunjoong Kim
- ย ย Hyun You Kim
https://pubs.rsc.org/en/journals/journalissues/ee#!issueid=ee013004&type=current&issnprint=1754-5692
Image created by minjeong Kim / Nanosphere
RSC_Energy Environmental Science _ cover ย Picture
01 April 2020, Issue 4,ย
Page 1041 to 1290ย
A tailored oxide interface creates dense Pt single-atom catalysts with high catalytic activity
Highly reactive dense Pt single-atoms stabilized on an oxide support can resolve a grand challenge in the economic use of Pt in catalysis. The maximized number density of reaction sites provided by dense Pt single-atoms guarantees the improved catalytic performance of Pt combined with high efficiency. By manipulating the chemical nature of multi-component interfaces, we synthesized CO-tolerant dense Pt single-atoms highly reactive for the CO oxidation reaction, which governs the key steps for chemical energy conversion and emission control. The addition of 1 wt% of Ce to TiO2 support particles creates a CeOxโTiO2 interface that stabilizes Pt single-atoms by strong electronic interactions. Dense Pt single-atoms formed on CeOx/TiO2 oxides exhibit 15.1 times greater specific mass activity toward CO oxidation at 140 ยฐC compared with a bare Pt/TiO2 catalyst. We elaborate how the CeOxโTiO2 interfaces activate the interface-mediated Marsโvan Krevelen mechanism of CO oxidation and protect Pt single-atoms from CO-poisoning. Through a comprehensive interpretation of the formation and activation of dense Pt single-atoms using operando X-ray absorption spectroscopy, density functional theory calculations, and experimental catalyst performance tests, we provide a key that enables the catalytic performance of noble metal single-atom catalysts to be optimized by atomic-scale tuning of the metalโsupport interface.
https://pubs.rsc.org/en/journals/journalissues/ee#!issueid=ee013004&type=current&issnprint=1754-5692
Image created by minjeong Kim / Nanosphere