TY - JOUR
T1 - Environment of Metal-O-Fe Bonds Enabling High Activity in CO2Reduction on Single Metal Atoms and on Supported Nanoparticles
AU - Zhu, Yifeng
AU - Yuk, Simuck F.
AU - Zheng, Jian
AU - Nguyen, Manh Thuong
AU - Lee, Mal Soon
AU - Szanyi, Janos
AU - Kovarik, Libor
AU - Zhu, Zihua
AU - Balasubramanian, Mahalingam
AU - Glezakou, Vassiliki Alexandra
AU - Fulton, John L.
AU - Lercher, Johannes A.
AU - Rousseau, Roger
AU - Gutiérrez, Oliver Y.
N1 - Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/4/14
Y1 - 2021/4/14
N2 - Single-atom catalysts are often reported to have catalytic properties that surpass those of nanoparticles, while a direct comparison of sites common and different for both is lacking. Here we show that single atoms of Pt-group metals embedded into the surface of Fe3O4 have a greatly enhanced interaction strength with CO2 compared with the Fe3O4 surface. The strong CO2 adsorption on single Rh atoms and corresponding low activation energies lead to 2 orders of magnitude higher conversion rates of CO2 compared to Rh nanoparticles. This high activity of single atoms stems from the partially oxidic state imposed by their coordination to the support. Fe3O4-supported Rh nanoparticles follow the behavior of single atoms for CO2 interaction and reduction, which is attributed to the dominating role of partially oxidic sites at the Fe3O4-Rh interface. Thus, we show a likely common catalytic chemistry for two kinds of materials thought to be different, and we show that single atoms of Pt-group metals on Fe3O4 are especially successful materials for catalyzed reactions that depend primarily upon sites with the metal-O-Fe environment.
AB - Single-atom catalysts are often reported to have catalytic properties that surpass those of nanoparticles, while a direct comparison of sites common and different for both is lacking. Here we show that single atoms of Pt-group metals embedded into the surface of Fe3O4 have a greatly enhanced interaction strength with CO2 compared with the Fe3O4 surface. The strong CO2 adsorption on single Rh atoms and corresponding low activation energies lead to 2 orders of magnitude higher conversion rates of CO2 compared to Rh nanoparticles. This high activity of single atoms stems from the partially oxidic state imposed by their coordination to the support. Fe3O4-supported Rh nanoparticles follow the behavior of single atoms for CO2 interaction and reduction, which is attributed to the dominating role of partially oxidic sites at the Fe3O4-Rh interface. Thus, we show a likely common catalytic chemistry for two kinds of materials thought to be different, and we show that single atoms of Pt-group metals on Fe3O4 are especially successful materials for catalyzed reactions that depend primarily upon sites with the metal-O-Fe environment.
UR - http://www.scopus.com/inward/record.url?scp=85104275731&partnerID=8YFLogxK
U2 - 10.1021/jacs.1c02276
DO - 10.1021/jacs.1c02276
M3 - Article
C2 - 33819019
AN - SCOPUS:85104275731
SN - 0002-7863
VL - 143
SP - 5540
EP - 5549
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 14
ER -