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Title: High temperature shockwave stabilized single atoms

Abstract

The stability of single-atom catalysts is critical for their practical applications. Although a high temperature can promote the bond formation between metal atoms and the substrate with an enhanced stability, it often causes atom agglomeration and is incompatible with many temperature-sensitive substrates. Here, we report using controllable high-temperature shockwaves to synthesize and stabilize single atoms at very high temperatures (1,500-2,000 K), achieved by a periodic on-off heating that features a short on state (55 ms) and a ten-times longer off state. The high temperature provides the activation energy for atom dispersion by forming thermodynamically favourable metal-defect bonds and the off-state critically ensures the overall stability, especially for the substrate. The resultant high-temperature single atoms exhibit a superior thermal stability as durable catalysts. In conclusion, the reported shockwave method is facile, ultrafast and universal (for example, Pt, Ru and Co single atoms, and carbon, C 3N 4 and TiO 2 substrates), which opens a general route for single-atom manufacturing that is conventionally challenging.

Authors:
ORCiD logo [1];  [2];  [3];  [4]; ORCiD logo [5];  [1];  [4];  [1];  [1];  [1];  [6]; ORCiD logo [7];  [7]; ORCiD logo [6]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering
  2. Univ. of Illinois at Chicago, Chicago, IL (United States). Dept. of Mechanical and Industrial Engineering
  3. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Chemical and Biomolecular Engineering
  4. Univ. of Maryland, College Park, MD (United States). Dept. of Mechanical Engineering
  5. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Div. and Chemical Sciences and Engineering Div.
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab.
  7. Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering and Chemistry and Biochemistry
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE Advanced Research Projects Agency - Energy (ARPA-E); Petroleum Research Fund (PRF); USDOE Office of Science (SC)
OSTI Identifier:
1575071
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Nanotechnology
Additional Journal Information:
Journal Volume: 14; Journal Issue: 9; Journal ID: ISSN 1748-3387
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; high temperature catalysts; metal-carbon bonds; shockwave synthesis; single atom dispersion; thermal stability; x-ray absorption spectroscopy

Citation Formats

Yao, Yonggang, Huang, Zhennan, Xie, Pengfei, Wu, Lianping, Ma, Lu, Li, Tangyuan, Pang, Zhenqian, Jiao, Miaolun, Liang, Zhiqiang, Gao, Jinlong, He, Yang, Kline, Dylan Jacob, Zachariah, Michael R., Wang, Chongmin, Lu, Jun, Wu, Tianpin, Li, Teng, Wang, Chao, Shahbazian-Yassar, Reza, and Hu, Liangbing. High temperature shockwave stabilized single atoms. United States: N. p., 2019. Web. doi:10.1038/s41565-019-0518-7.
Yao, Yonggang, Huang, Zhennan, Xie, Pengfei, Wu, Lianping, Ma, Lu, Li, Tangyuan, Pang, Zhenqian, Jiao, Miaolun, Liang, Zhiqiang, Gao, Jinlong, He, Yang, Kline, Dylan Jacob, Zachariah, Michael R., Wang, Chongmin, Lu, Jun, Wu, Tianpin, Li, Teng, Wang, Chao, Shahbazian-Yassar, Reza, & Hu, Liangbing. High temperature shockwave stabilized single atoms. United States. doi:10.1038/s41565-019-0518-7.
Yao, Yonggang, Huang, Zhennan, Xie, Pengfei, Wu, Lianping, Ma, Lu, Li, Tangyuan, Pang, Zhenqian, Jiao, Miaolun, Liang, Zhiqiang, Gao, Jinlong, He, Yang, Kline, Dylan Jacob, Zachariah, Michael R., Wang, Chongmin, Lu, Jun, Wu, Tianpin, Li, Teng, Wang, Chao, Shahbazian-Yassar, Reza, and Hu, Liangbing. Mon . "High temperature shockwave stabilized single atoms". United States. doi:10.1038/s41565-019-0518-7.
@article{osti_1575071,
title = {High temperature shockwave stabilized single atoms},
author = {Yao, Yonggang and Huang, Zhennan and Xie, Pengfei and Wu, Lianping and Ma, Lu and Li, Tangyuan and Pang, Zhenqian and Jiao, Miaolun and Liang, Zhiqiang and Gao, Jinlong and He, Yang and Kline, Dylan Jacob and Zachariah, Michael R. and Wang, Chongmin and Lu, Jun and Wu, Tianpin and Li, Teng and Wang, Chao and Shahbazian-Yassar, Reza and Hu, Liangbing},
abstractNote = {The stability of single-atom catalysts is critical for their practical applications. Although a high temperature can promote the bond formation between metal atoms and the substrate with an enhanced stability, it often causes atom agglomeration and is incompatible with many temperature-sensitive substrates. Here, we report using controllable high-temperature shockwaves to synthesize and stabilize single atoms at very high temperatures (1,500-2,000 K), achieved by a periodic on-off heating that features a short on state (55 ms) and a ten-times longer off state. The high temperature provides the activation energy for atom dispersion by forming thermodynamically favourable metal-defect bonds and the off-state critically ensures the overall stability, especially for the substrate. The resultant high-temperature single atoms exhibit a superior thermal stability as durable catalysts. In conclusion, the reported shockwave method is facile, ultrafast and universal (for example, Pt, Ru and Co single atoms, and carbon, C3N4 and TiO2 substrates), which opens a general route for single-atom manufacturing that is conventionally challenging.},
doi = {10.1038/s41565-019-0518-7},
journal = {Nature Nanotechnology},
number = 9,
volume = 14,
place = {United States},
year = {2019},
month = {8}
}

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