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Title: Efficient Hydrogen Production from Methanol Using a Single-Site Pt1/CeO2 Catalyst

Abstract

Hydrogen is regarded as an attractive alternative energy carrier due to its high gravimetric energy density and only water production upon combustion. However, due to its low volumetric energy density, there are still some challenges in practical hydrogen storage and transportation. In the last decade, using chemical bonds of liquid organic molecules as hydrogen carriers to generate hydrogen in situ provided a feasible method to potentially solve this problem. Research efforts on liquid organic hydrogen carriers (LOHCs) seek practical carrier systems and advanced catalytic materials that have the potential to reduce costs, increase reaction rate, and provide a more efficient catalytic hydrogen genera-tion/storage process. In this work, we used methanol as a hydrogen carrier to release hydrogen in situ with the single-site Pt1/CeO2 catalyst. Moreover, in this reaction, compared with traditional nanoparticle catalysts, the single site catalyst displays excellent hydrogen generation efficiency, 40 times higher than that of a 2.5 nm Pt/CeO2 sample, and 800 times higher compared to a 7.0 nm Pt/CeO2 sample. Our in-depth study highlights the benefits of single-site catalysts and paves the way for further rational design of highly efficient catalysts for sustainable energy storage applications.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [4]; ORCiD logo [4];  [5];  [6];  [6];  [4];  [7];  [8];  [8];  [9];  [10]; ORCiD logo [10]; ORCiD logo [10]; ORCiD logo [3];  [11];  [12] more »; ORCiD logo [2] « less
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Xiamen Univ. (China). College of Chemistry and Chemical Engineering, Collaborative Innovation Center for Chemistry for Energy Materials, Dept. of Chemistry, and State Key Lab. of Physical Chemistry of Solid Surfaces
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  5. Xiamen Univ. (China). College of Chemistry and Chemical Engineering, Collaborative Innovation Center for Chemistry for Energy Materials, Dept. of Chemistry, and State Key Lab. of Physical Chemistry of Solid Surfaces
  6. Science-Based Industrial Park, Hsinchu (Taiwan). National Synchrotron Radiation Research Center
  7. Chinese Academy of Sciences (CAS), Xiamen (China). Inst. of Urban Environment
  8. Univ. of Central Florida, Orlando, FL (United States). Dept. of Civil, Environmental and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), and Nano-Science Technology Center (NSTC)
  9. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Material Science Division, Molecular Foundry
  10. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
  11. State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
  12. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Material Science Division, Molecular Foundry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1572860
Grant/Contract Number:  
AC02-05CH11231; NA-0003525
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 45; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Lu-Ning, Hou, Kai-Peng, Liu, Yi-Sheng, Qi, Zhi-Yuan, Zheng, Qi, Lu, Yi-Hsien, Chen, Jia-Yu, Chen, Jeng-Lung, Pao, Chih-Wen, Wang, Shuo-Bo, Li, Yao-Bin, Xie, Shao-Hua, Liu, Fu-Dong, Prendergast, David, Klebanoff, Leonard E., Stavila, Vitalie, Allendorf, Mark D., Guo, Jinghua, Zheng, Lan-Sun, Su, Ji, and Somorjai, Gabor A. Efficient Hydrogen Production from Methanol Using a Single-Site Pt1/CeO2 Catalyst. United States: N. p., 2019. Web. doi:10.1021/jacs.9b09431.
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Chen, Lu-Ning, Hou, Kai-Peng, Liu, Yi-Sheng, Qi, Zhi-Yuan, Zheng, Qi, Lu, Yi-Hsien, Chen, Jia-Yu, Chen, Jeng-Lung, Pao, Chih-Wen, Wang, Shuo-Bo, Li, Yao-Bin, Xie, Shao-Hua, Liu, Fu-Dong, Prendergast, David, Klebanoff, Leonard E., Stavila, Vitalie, Allendorf, Mark D., Guo, Jinghua, Zheng, Lan-Sun, Su, Ji, & Somorjai, Gabor A. Efficient Hydrogen Production from Methanol Using a Single-Site Pt1/CeO2 Catalyst. United States. https://doi.org/10.1021/jacs.9b09431
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Chen, Lu-Ning, Hou, Kai-Peng, Liu, Yi-Sheng, Qi, Zhi-Yuan, Zheng, Qi, Lu, Yi-Hsien, Chen, Jia-Yu, Chen, Jeng-Lung, Pao, Chih-Wen, Wang, Shuo-Bo, Li, Yao-Bin, Xie, Shao-Hua, Liu, Fu-Dong, Prendergast, David, Klebanoff, Leonard E., Stavila, Vitalie, Allendorf, Mark D., Guo, Jinghua, Zheng, Lan-Sun, Su, Ji, and Somorjai, Gabor A. Thu . "Efficient Hydrogen Production from Methanol Using a Single-Site Pt1/CeO2 Catalyst". United States. https://doi.org/10.1021/jacs.9b09431. https://www.osti.gov/servlets/purl/1572860.
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@article{osti_1572860,
title = {Efficient Hydrogen Production from Methanol Using a Single-Site Pt1/CeO2 Catalyst},
author = {Chen, Lu-Ning and Hou, Kai-Peng and Liu, Yi-Sheng and Qi, Zhi-Yuan and Zheng, Qi and Lu, Yi-Hsien and Chen, Jia-Yu and Chen, Jeng-Lung and Pao, Chih-Wen and Wang, Shuo-Bo and Li, Yao-Bin and Xie, Shao-Hua and Liu, Fu-Dong and Prendergast, David and Klebanoff, Leonard E. and Stavila, Vitalie and Allendorf, Mark D. and Guo, Jinghua and Zheng, Lan-Sun and Su, Ji and Somorjai, Gabor A.},
abstractNote = {Hydrogen is regarded as an attractive alternative energy carrier due to its high gravimetric energy density and only water production upon combustion. However, due to its low volumetric energy density, there are still some challenges in practical hydrogen storage and transportation. In the last decade, using chemical bonds of liquid organic molecules as hydrogen carriers to generate hydrogen in situ provided a feasible method to potentially solve this problem. Research efforts on liquid organic hydrogen carriers (LOHCs) seek practical carrier systems and advanced catalytic materials that have the potential to reduce costs, increase reaction rate, and provide a more efficient catalytic hydrogen genera-tion/storage process. In this work, we used methanol as a hydrogen carrier to release hydrogen in situ with the single-site Pt1/CeO2 catalyst. Moreover, in this reaction, compared with traditional nanoparticle catalysts, the single site catalyst displays excellent hydrogen generation efficiency, 40 times higher than that of a 2.5 nm Pt/CeO2 sample, and 800 times higher compared to a 7.0 nm Pt/CeO2 sample. Our in-depth study highlights the benefits of single-site catalysts and paves the way for further rational design of highly efficient catalysts for sustainable energy storage applications.},
doi = {10.1021/jacs.9b09431},
journal = {Journal of the American Chemical Society},
number = 45,
volume = 141,
place = {United States},
year = {2019},
month = {10}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/jacs.9b09431
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Cited by: 6 works
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Figures / Tables:

Figure 1 Figure 1: (a) Cs-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images of Pt1/CeO2 catalyst, the brighter dots cycled are Pt single sites, (b) HAADF-STEM and corresponding elemental mappings images of Pt1/CeO2 catalyst.
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