PNNL

Abstract

A research team involving Arizona State University, University of California Davis, and Washington State University/Pacific Northwest National Laboratory scientists grafted isolated and defective cerium oxide (CeOx) “nanoglue” islands onto high-surface-area silicon dioxide (SiO2). The nanoglue islands host an average of one platinum (Pt) atom each. The team found that the Pt atoms remain dispersed under both oxidizing and reducing environments at high temperatures. The dispersed activated catalyst exhibits markedly increased reactivity for carbon monoxide oxidation. The researchers attribute the improved stability under reducing conditions to the support structure and much stronger affinity of Pt atoms for CeOx than the SiO2 support. This ensures the that Pt atoms can move while remaining confined to their respective nanoglue islands. The strategy of using functional nanoglues to confine atomically dispersed metals and simultaneously enhance their reactivity is general and is anticipated to move single-atom catalysts a step closer to practical applications. This work was primarily supported by the National Science Foundation under grant no. 1955474 (CHE-1955474) and 1465057 (CHE-1465057). J.?Zeng acknowledges support by National Key Research and Development Program of China (2021YFA1500500), National Science Fund for Distinguished Young Scholars (21925204), and NSFC (U19A2015). Y.W. acknowledges support by the US Department of Energy (DOE), Office of Science (SC), Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences, Catalysis Science program (DE-AC05-RL01830, FWP-47319). Y.C., C.-Y.F., and B.C.G. acknowledge the support of DOE SC grant DE-FG02-04ER15513. X.I.P.-H. thanks Fulbright Colombia and Colciencias for financial support provided to pursue a PhD degree and acknowledges the support of DOE SC Grant DE-FG02-05ER15712 and DOE EERE/VTO. X.L. and Y.C. acknowledge funding from the China Scholarship Council (CSC) (201706340130, 201806340062). The authors thank Y.?Yu and N.?Zhang for help in the revision stage. The authors acknowledge the use of facilities within the Eyring Materials Center and the John M. Cowley Center for High Resolution Electron Microscopy at Arizona State University and thank the Stanford Synchrotron Radiation Lightsource (beamlines 4-1, 9-3) for providing beam time.