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Title: High temperature shockwave stabilized single atoms

Abstract

The stability of single atom catalysts against agglomeration is critical for their practical applications. High temperature can promote the strong binding of single atoms onto the substrate by forming metal-substrate bonds with enhanced thermal stability, but high temperature (> 1000°C) is typically against single atom dispersion and also incompatible with many temperature sensitive processes and substrates. Here we report using highly controllable, high temperature shockwaves to synthesize and stabilize single atoms (HT-SAs) at record-high temperatures (Ts=1500–2000 K), achieved by a periodic on-off heating pattern featuring a short on-state (55 ms) and a 10-times longer off-state. The high temperature on-state promotes single atom dispersion and stabilization by forming strong metal-substrate bonds; while the off-state critically ensures the overall stability by preventing overheating-induced atom aggregation and substrate deterioration. The repeated on-off shockwaves lead to a complete atom dispersion while keep the substrate stable despite high temperature exposure. We demonstrate the HT-SAs showing superior stability by in situ observation up to 1273 K as well as in practical applications as durable catalysts. The shockwave method is facile, ultrafast, and universal for synthesizing thermally-stable single atom dispersions (e.g., Pt, Ru, and Co) and on different substrates (e.g., carbon, C3N4, and TiO2), which opens amore » general route for single atom manufacturing that is conventionally challenging.« less

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]
+ Show Author Affiliations
  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 Laboratory (ANL), Argonne, IL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (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
Alternate Identifier(s):
OSTI ID: 1734877
Report Number(s):
PNNL-SA-143543
Journal ID: ISSN 1748-3387; 154489
Grant/Contract Number:  
AC02-06CH11357; AC05-76RL01830
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.
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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. https://doi.org/10.1038/s41565-019-0518-7
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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. https://doi.org/10.1038/s41565-019-0518-7. https://www.osti.gov/servlets/purl/1575071.
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@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 against agglomeration is critical for their practical applications. High temperature can promote the strong binding of single atoms onto the substrate by forming metal-substrate bonds with enhanced thermal stability, but high temperature (> 1000°C) is typically against single atom dispersion and also incompatible with many temperature sensitive processes and substrates. Here we report using highly controllable, high temperature shockwaves to synthesize and stabilize single atoms (HT-SAs) at record-high temperatures (Ts=1500–2000 K), achieved by a periodic on-off heating pattern featuring a short on-state (55 ms) and a 10-times longer off-state. The high temperature on-state promotes single atom dispersion and stabilization by forming strong metal-substrate bonds; while the off-state critically ensures the overall stability by preventing overheating-induced atom aggregation and substrate deterioration. The repeated on-off shockwaves lead to a complete atom dispersion while keep the substrate stable despite high temperature exposure. We demonstrate the HT-SAs showing superior stability by in situ observation up to 1273 K as well as in practical applications as durable catalysts. The shockwave method is facile, ultrafast, and universal for synthesizing thermally-stable single atom dispersions (e.g., Pt, Ru, and Co) and on different substrates (e.g., carbon, C3N4, and TiO2), 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 = {Mon Aug 12 00:00:00 EDT 2019},
month = {Mon Aug 12 00:00:00 EDT 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41565-019-0518-7
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Cited by: 182 works
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Figures / Tables:

Figure 1 Figure 1: In situ, high temperature shockwave synthesis of HT-SAs on defective carbon. a, Schematic diagram showing the HT-SA synthesis and dispersion process (grey: carbon atoms; cyan: metal precursor; red: metallic atoms). b, The temperature evolution during the shockwave synthesis and the detailed heating/cooling pattern. The inset shows the lightmore » emitted from the material at high temperature. c, A 10-pulse shock heating pattern, demonstrating the uniform temperature in each cycle with a high temperature on-state and a low temperature off-state. d-e, Typical HAADF images of Pt HT-SAs after 1 and 10 cycles of the thermal shock (0.01 µmol/cm2). f, EXAFS profiles (without phase correction) for Pt HT-SAs on CA-CNFs after 1 and 10 cycles of the thermal shock treatment.« less
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    Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts
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