TY - JOUR
T1 - Boosting Fenton-Like Reactions via Single Atom Fe Catalysis
AU - Yin, Yu
AU - Shi, Lei
AU - Li, Wenlang
AU - Li, Xuning
AU - Wu, Hong
AU - Ao, Zhimin
AU - Tian, Wenjie
AU - Liu, Shaomin
AU - Wang, Shaobin
AU - Sun, Hongqi
N1 - Funding Information:
The author (Sun) would like to express his thanks for the support from Vice-Chancellor’s Professorial Research Fellowship. This work was also financially supported by the National Natural Science Foundation of China (No. 51602133, 21607029 and 21777033), Natural Science Foundation of Jiangsu Province (No. BK20160555), Science and Technology Program of Guangdong Province (No. 2017B020216003). The authors acknowledge the help of Martin Saunders and Alexandra Suvorova from the Centre for Microscopy, Characterization and Analysis (CMCA) of the University of Western Australia.
Funding Information:
The author (Sun) would like to express his thanks for the support from Vice-Chancellor's Professorial Research Fellowship. This work was also financially supported by the National Natural Science Foundation of China (No. 51602133, 21607029 and 21777033), Natural Science Foundation of Jiangsu Province (No. BK20160555), Science and Technology Program of Guangdong Province (No. 2017B020216003). The authors acknowledge the help of Martin Saunders and Alexandra Suvorova from the Centre for Microscopy, Characterization and Analysis (CMCA) of the University of Western Australia.
Publisher Copyright:
© 2019 American Chemical Society.
PY - 2019/10/1
Y1 - 2019/10/1
N2 - The maximization of the numbers of exposed active sites in supported metal catalysts is important to achieve high reaction activity. In this work, a simple strategy for anchoring single atom Fe on SBA-15 to expose utmost Fe active sites was proposed. Iron salts were introduced into the as-made SBA-15 containing the template and calcined for simultaneous decomposition of the iron precursor and the template, resulting in single atom Fe sites in the nanopores of SBA-15 catalysts (SAFe-SBA). X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and extended X-ray absorption fine structure (EXAFS) imply the presence of single atom Fe sites. Furthermore, EXAFS analysis suggests the structure of one Fe center with four O atoms, and density functional theory calculations (DFT) simulate this structure. The catalytic performances of SAFe-SBA were evaluated in Fenton-like catalytic oxidation of p-hydroxybenzoic acid (HBA) and phenol. It was found that the single atom SAFe-SBA catalysts displayed superior catalytic activity to aggregated iron sites (AGFe-SBA) in both HBA and phenol degradation, demonstrating the advantage of SAFe-SBA in catalysis.
AB - The maximization of the numbers of exposed active sites in supported metal catalysts is important to achieve high reaction activity. In this work, a simple strategy for anchoring single atom Fe on SBA-15 to expose utmost Fe active sites was proposed. Iron salts were introduced into the as-made SBA-15 containing the template and calcined for simultaneous decomposition of the iron precursor and the template, resulting in single atom Fe sites in the nanopores of SBA-15 catalysts (SAFe-SBA). X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and extended X-ray absorption fine structure (EXAFS) imply the presence of single atom Fe sites. Furthermore, EXAFS analysis suggests the structure of one Fe center with four O atoms, and density functional theory calculations (DFT) simulate this structure. The catalytic performances of SAFe-SBA were evaluated in Fenton-like catalytic oxidation of p-hydroxybenzoic acid (HBA) and phenol. It was found that the single atom SAFe-SBA catalysts displayed superior catalytic activity to aggregated iron sites (AGFe-SBA) in both HBA and phenol degradation, demonstrating the advantage of SAFe-SBA in catalysis.
UR - http://www.scopus.com/inward/record.url?scp=85072714123&partnerID=8YFLogxK
U2 - 10.1021/acs.est.9b03342
DO - 10.1021/acs.est.9b03342
M3 - Article
C2 - 31436973
AN - SCOPUS:85072714123
SN - 0013-936X
VL - 53
SP - 11391
EP - 11400
JO - Environmental Science and Technology
JF - Environmental Science and Technology
IS - 19
ER -