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Title: Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts

Authors:
; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division; National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1429858
DOE Contract Number:
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nature (London); Journal Volume: 544; Journal Issue: 7648
Country of Publication:
United States
Language:
English

Citation Formats

Lin, Lili, Zhou, Wu, Gao, Rui, Yao, Siyu, Zhang, Xiao, Xu, Wenqian, Zheng, Shijian, Jiang, Zheng, Yu, Qiaolin, Li, Yong-Wang, Shi, Chuan, Wen, Xiao-Dong, and Ma, Ding. Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts. United States: N. p., 2017. Web. doi:10.1038/nature21672.
Lin, Lili, Zhou, Wu, Gao, Rui, Yao, Siyu, Zhang, Xiao, Xu, Wenqian, Zheng, Shijian, Jiang, Zheng, Yu, Qiaolin, Li, Yong-Wang, Shi, Chuan, Wen, Xiao-Dong, & Ma, Ding. Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts. United States. doi:10.1038/nature21672.
Lin, Lili, Zhou, Wu, Gao, Rui, Yao, Siyu, Zhang, Xiao, Xu, Wenqian, Zheng, Shijian, Jiang, Zheng, Yu, Qiaolin, Li, Yong-Wang, Shi, Chuan, Wen, Xiao-Dong, and Ma, Ding. Wed . "Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts". United States. doi:10.1038/nature21672.
@article{osti_1429858,
title = {Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts},
author = {Lin, Lili and Zhou, Wu and Gao, Rui and Yao, Siyu and Zhang, Xiao and Xu, Wenqian and Zheng, Shijian and Jiang, Zheng and Yu, Qiaolin and Li, Yong-Wang and Shi, Chuan and Wen, Xiao-Dong and Ma, Ding},
abstractNote = {},
doi = {10.1038/nature21672},
journal = {Nature (London)},
number = 7648,
volume = 544,
place = {United States},
year = {Wed Mar 22 00:00:00 EDT 2017},
month = {Wed Mar 22 00:00:00 EDT 2017}
}
  • Here, the water-gas shift (WGS) reaction (where carbon monoxide plus water yields dihydrogen and carbon dioxide) is an essential process for hydrogen generation and carbon monoxide removal in various energy-related chemical operations. This equilibrium-limited reaction is favored at a low working temperature. Potential application in fuel cells also requires a WGS catalyst to be highly active, stable, and energy-efficient and to match the working temperature of on-site hydrogen generation and consumption units. We synthesized layered gold (Au) clusters on a molybdenum carbide (α-MoC) substrate to create an interfacial catalyst system for the ultralow-temperature WGS reaction. Water was activated over α-MoCmore » at 303 kelvin, whereas carbon monoxide adsorbed on adjacent Au sites was apt to react with surface hydroxyl groups formed from water splitting, leading to a high WGS activity at low temperatures.« less
    Cited by 9
  • Here, the water-gas shift (WGS) reaction (where carbon monoxide plus water yields dihydrogen and carbon dioxide) is an essential process for hydrogen generation and carbon monoxide removal in various energy-related chemical operations. This equilibrium-limited reaction is favored at a low working temperature. Potential application in fuel cells also requires a WGS catalyst to be highly active, stable, and energy-efficient and to match the working temperature of on-site hydrogen generation and consumption units. We synthesized layered gold (Au) clusters on a molybdenum carbide (α-MoC) substrate to create an interfacial catalyst system for the ultralow-temperature WGS reaction. Water was activated over α-MoCmore » at 303 kelvin, whereas carbon monoxide adsorbed on adjacent Au sites was apt to react with surface hydroxyl groups formed from water splitting, leading to a high WGS activity at low temperatures.« less
    Cited by 9
  • We present that Pt/MoC and Pt/TiC(001) are excellent catalysts for the low-temperature water-gas shift (WGS, CO + H 2O → H 2 + CO 2) reaction. They exhibit high-activity, stability and selectivity. The highest catalytic activities are seen for small coverages of Pt on the carbide substrates. Synergistic effects at the metal-carbide interface produce an enhancement in chemical activity with respect to pure Pt, MoC and TiC. A clear correlation is found between the ability of the Pt/MoC and Pt/TiC(001) surfaces to partially dissociate water and their catalytic activity for the WGS reaction. Finally, an overall comparison of the resultsmore » for Pt/MoC and Pt/Mo 2C(001) indicates that the metal/carbon ratio in the carbide support can have a strong influence in the stability and selectivity of WGS catalysts and is a parameter that must be taken into consideration when designing these systems.« less
  • In this paper, the water gas shift (WGS) reaction catalyzed by orthorhombic β-Mo 2C and cubic δ-MoC surfaces with and without Au clusters supported thereon has been studied by means of a combination of sophisticated experiments and state-of-the-art computational modeling. Experiments evidence the importance of the metal/carbon ratio on the performance of these systems, where Au/δ-MoC is presented as a suitable catalyst for WGS at low temperatures owing to its high activity, selectivity (only CO 2 and H 2 are detected), and stability (oxycarbides are not observed). Periodic density functional theory-based calculations show that the supported Au clusters and themore » Au/δ-MoC interface do not take part directly in water dissociation but their presence is crucial to switch the reaction mechanism, drastically decreasing the effect of the reverse WGS reaction and favoring the WGS products desorption, thus leading to an increase in CO 2 and H 2 production. Finally, the present results clearly display the importance of the Mo/C ratio and the synergy with the admetal clusters in tuning the activity and selectivity of the carbide substrate.« less