Stable iridium dinuclear heterogeneous catalysts supported on metal-oxide substrate for solar water oxidation
Author(s) -
Yanyan Zhao,
Ke Yang,
Zechao Wang,
Xingxu Yan,
Sufeng Cao,
Yifan Ye,
Qi Dong,
Xizi Zhang,
James E. Thorne,
Lei Jin,
Kelly L. Materna,
Antonios Trimpalis,
HongYe Bai,
Sirine C. Fakra,
Xiaoyan Zhong,
Peng Wang,
Xiaoqing Pan,
Jinghua Guo,
Maria FlytzaniStephanopoulos,
Gary W. Brudvig,
Víctor S. Batista,
Dunwei Wang
Publication year - 2018
Publication title -
proceedings of the national academy of sciences
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.011
H-Index - 771
eISSN - 1091-6490
pISSN - 0027-8424
DOI - 10.1073/pnas.1722137115
Subject(s) - catalysis , iridium , heterogeneous catalysis , substrate (aquarium) , nanotechnology , oxide , materials science , chemistry , photochemistry , combinatorial chemistry , chemical engineering , organic chemistry , oceanography , engineering , geology
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-Fe 2 O 3 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-Fe 2 O 3 anchor the catalysts to provide outstanding stability against detachment or aggregation. The resulting catalysts exhibit high activities toward H 2 O photooxidation.
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