Abstract
Atomically dispersed catalysts refer to substrate-supported heterogeneous catalysts featuring one or a few active metal atoms that are separated from one another. They represent an important class of materials ranging from single-atom catalysts (SACs) and nanoparticles (NPs).While SACs and NPs have been extensively reported, catalysts featuring a few atoms with well-defined structures are poorly studied. The difficulty in synthesizing such structures has been a critical challenge. Here we report a facile photochemical method that produces catalytic centers consisting of two Ir metal cations, bridged by O and stably bound to a support. Direct evidence unambiguously supporting the dinuclear nature of the catalysts anchored on α-Fe2O3 is obtained by aberration-corrected scanning transmission electron microscopy (AC-STEM). Experimental and computational results further reveal that the threefold hollow binding sites on the OH-terminated surface of α-Fe2O3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H2O photooxidation.
| Original language | English |
|---|---|
| Pages (from-to) | 2902-2907 |
| Number of pages | 6 |
| Journal | Proceedings of the National Academy of Sciences of the United States of America |
| Volume | 115 |
| Issue number | 12 |
| DOIs | |
| Publication status | Published - Mar 20 2018 |
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Keywords
- Catalyst
- Solar energy
- Spectroscopy
- STEM
- Water splitting
ASJC Scopus subject areas
- General
Cite this
Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation. / Zhao, Yanyan; Yang, Ke R.; Wang, Zechao; Yan, Xingxu; Cao, Sufeng; Ye, Yifan; Dong, Qi; Zhang, Xizi; Thorne, James E.; Jin, Lei; Materna, Kelly L.; Trimpalis, Antonios; Bai, Hongye; Fakra, Sirine C.; Zhong, Xiaoyan; Wang, Peng; Pan, Xiaoqing; Guo, Jinghua; Flytzani-Stephanopoulos, Maria; Brudvig, Gary W; Batista, Victor S.; Wang, Dunwei.
In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 115, No. 12, 20.03.2018, p. 2902-2907.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation
AU - Zhao, Yanyan
AU - Yang, Ke R.
AU - Wang, Zechao
AU - Yan, Xingxu
AU - Cao, Sufeng
AU - Ye, Yifan
AU - Dong, Qi
AU - Zhang, Xizi
AU - Thorne, James E.
AU - Jin, Lei
AU - Materna, Kelly L.
AU - Trimpalis, Antonios
AU - Bai, Hongye
AU - Fakra, Sirine C.
AU - Zhong, Xiaoyan
AU - Wang, Peng
AU - Pan, Xiaoqing
AU - Guo, Jinghua
AU - Flytzani-Stephanopoulos, Maria
AU - Brudvig, Gary W
AU - Batista, Victor S.
AU - Wang, Dunwei
PY - 2018/3/20
Y1 - 2018/3/20
N2 - Atomically dispersed catalysts refer to substrate-supported heterogeneous catalysts featuring one or a few active metal atoms that are separated from one another. They represent an important class of materials ranging from single-atom catalysts (SACs) and nanoparticles (NPs).While SACs and NPs have been extensively reported, catalysts featuring a few atoms with well-defined structures are poorly studied. The difficulty in synthesizing such structures has been a critical challenge. Here we report a facile photochemical method that produces catalytic centers consisting of two Ir metal cations, bridged by O and stably bound to a support. Direct evidence unambiguously supporting the dinuclear nature of the catalysts anchored on α-Fe2O3 is obtained by aberration-corrected scanning transmission electron microscopy (AC-STEM). Experimental and computational results further reveal that the threefold hollow binding sites on the OH-terminated surface of α-Fe2O3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H2O photooxidation.
AB - Atomically dispersed catalysts refer to substrate-supported heterogeneous catalysts featuring one or a few active metal atoms that are separated from one another. They represent an important class of materials ranging from single-atom catalysts (SACs) and nanoparticles (NPs).While SACs and NPs have been extensively reported, catalysts featuring a few atoms with well-defined structures are poorly studied. The difficulty in synthesizing such structures has been a critical challenge. Here we report a facile photochemical method that produces catalytic centers consisting of two Ir metal cations, bridged by O and stably bound to a support. Direct evidence unambiguously supporting the dinuclear nature of the catalysts anchored on α-Fe2O3 is obtained by aberration-corrected scanning transmission electron microscopy (AC-STEM). Experimental and computational results further reveal that the threefold hollow binding sites on the OH-terminated surface of α-Fe2O3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H2O photooxidation.
KW - Catalyst
KW - Solar energy
KW - Spectroscopy
KW - STEM
KW - Water splitting
UR - http://www.scopus.com/inward/record.url?scp=85044237676&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85044237676&partnerID=8YFLogxK
U2 - 10.1073/pnas.1722137115
DO - 10.1073/pnas.1722137115
M3 - Article
VL - 115
SP - 2902
EP - 2907
JO - Proceedings of the National Academy of Sciences of the United States of America
JF - Proceedings of the National Academy of Sciences of the United States of America
SN - 0027-8424
IS - 12
ER -