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Instruments / Technical Area	Publication Details	Published	Actions
B18-Core EXAFS E01-JEM ARM 200CF E02-JEM ARM 300CF I11-High Resolution Powder Diffraction I20-Scanning-X-ray spectroscopy (XAS/XES)	Adsorption and activation of molecular oxygen over atomic copper(I/II) site on ceria Liqun Kang , Bolun Wang , Qiming Bing , Michal Zalibera , Robert Büchel , Ruoyu Xu , Qiming Wang , Yiyun Liu , Diego Gianolio , Chiu C. Tang , Emma K. Gibson , Mohsen Danaie , Christopher Allen , Ke Wu , Sushila Marlow , Ling-Dong Sun , Qian He , Shaoliang Guan , Anton Savitsky , Juan J. Velasco-Vélez , June Callison , Christopher W. M. Kay , Sotiris E. Pratsinis , Wolfgang Lubitz , Jing-Yao Liu , Feng Ryan Wang Nature Communications 11 DOI: 10.1038/s41467-020-17852-8 Diamond Proposal Number(s): [15151, 15763, 16966, 17377, 19072, 19246, 20939, 17559, 24285, 19318, 19850] Open Access Show Abstract ▼ Abstract: Supported atomic metal sites have discrete molecular orbitals. Precise control over the energies of these sites is key to achieving novel reaction pathways with superior selectivity. Here, we achieve selective oxygen (O2) activation by utilising a framework of cerium (Ce) cations to reduce the energy of 3d orbitals of isolated copper (Cu) sites. Operando X-ray absorption spectroscopy, electron paramagnetic resonance and density-functional theory simulations are used to demonstrate that a [Cu(I)O2]3− site selectively adsorbs molecular O2, forming a rarely reported electrophilic η2-O2 species at 298 K. Assisted by neighbouring Ce(III) cations, η2-O2 is finally reduced to two O2−, that create two Cu–O–Ce oxo-bridges at 453 K. The isolated Cu(I)/(II) sites are ten times more active in CO oxidation than CuO clusters, showing a turnover frequency of 0.028 ± 0.003 s−1 at 373 K and 0.01 bar PCO. The unique electronic structure of [Cu(I)O2]3− site suggests its potential in selective oxidation.	Aug 2020

Instruments / Technical Area

Publication Details

Published

Actions

B18-Core EXAFS
E01-JEM ARM 200CF
E02-JEM ARM 300CF
I11-High Resolution Powder Diffraction
I20-Scanning-X-ray spectroscopy (XAS/XES)

Adsorption and activation of molecular oxygen over atomic copper(I/II) site on ceria