TY - JOUR
T1 - Functional CeO x nanoglues for robust atomically dispersed catalysts
AU - Li, Xu
AU - Pereira-Hernández, Xavier Isidro
AU - Chen, Yizhen
AU - Xu, Jia
AU - Zhao, Jiankang
AU - Pao, Chih Wen
AU - Fang, Chia Yu
AU - Zeng, Jie
AU - Wang, Yong
AU - Gates, Bruce C.
AU - Liu, Jingyue
N1 - Funding Information:
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.
Funding Information:
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.
Publisher Copyright:
© 2022, The Author(s), under exclusive licence to Springer Nature Limited.
PY - 2022/11/10
Y1 - 2022/11/10
N2 - Single-atom catalysts1 make exceptionally efficient use of expensive noble metals and can bring out unique properties1–3. However, applications are usually compromised by limited catalyst stability, which is due to sintering3,4. Although sintering can be suppressed by anchoring the metal atoms to oxide supports1,5,6, strong metal–oxygen interactions often leave too few metal sites available for reactant binding and catalysis6,7, and when exposed to reducing conditions at sufficiently high temperatures, even oxide-anchored single-atom catalysts eventually sinter4,8,9. Here we show that the beneficial effects of anchoring can be enhanced by confining the atomically dispersed metal atoms on oxide nanoclusters or ‘nanoglues’, which themselves are dispersed and immobilized on a robust, high-surface-area support. We demonstrate the strategy by grafting isolated and defective CeOx nanoglue islands onto high-surface-area SiO2; the nanoglue islands then each host on average one Pt atom. We find that the Pt atoms remain dispersed under both oxidizing and reducing environments at high temperatures, and that the activated catalyst exhibits markedly increased activity for CO oxidation. We attribute the improved stability under reducing conditions to the support structure and the much stronger affinity of Pt atoms for CeOx than for SiO2, which ensures the Pt atoms can move but remain 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 we anticipate that it will take single-atom catalysts a step closer to practical applications.
AB - Single-atom catalysts1 make exceptionally efficient use of expensive noble metals and can bring out unique properties1–3. However, applications are usually compromised by limited catalyst stability, which is due to sintering3,4. Although sintering can be suppressed by anchoring the metal atoms to oxide supports1,5,6, strong metal–oxygen interactions often leave too few metal sites available for reactant binding and catalysis6,7, and when exposed to reducing conditions at sufficiently high temperatures, even oxide-anchored single-atom catalysts eventually sinter4,8,9. Here we show that the beneficial effects of anchoring can be enhanced by confining the atomically dispersed metal atoms on oxide nanoclusters or ‘nanoglues’, which themselves are dispersed and immobilized on a robust, high-surface-area support. We demonstrate the strategy by grafting isolated and defective CeOx nanoglue islands onto high-surface-area SiO2; the nanoglue islands then each host on average one Pt atom. We find that the Pt atoms remain dispersed under both oxidizing and reducing environments at high temperatures, and that the activated catalyst exhibits markedly increased activity for CO oxidation. We attribute the improved stability under reducing conditions to the support structure and the much stronger affinity of Pt atoms for CeOx than for SiO2, which ensures the Pt atoms can move but remain 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 we anticipate that it will take single-atom catalysts a step closer to practical applications.
UR - http://www.scopus.com/inward/record.url?scp=85140591537&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85140591537&partnerID=8YFLogxK
U2 - 10.1038/s41586-022-05251-6
DO - 10.1038/s41586-022-05251-6
M3 - Article
C2 - 36289341
AN - SCOPUS:85140591537
VL - 611
SP - 284
EP - 288
JO - Nature
JF - Nature
SN - 0028-0836
IS - 7935
ER -