Electronic structure modification of platinum on titanium nitride resulting in enhanced catalytic activity and durability for oxygen reduction and formic acid oxidation

Sungeun Yang; Dong Young Chung; Young Joo Tak; Jiwhan Kim; Haksu Han; Jong Sung Yu; Aloysius Soon; Yung Eun Sung; Hyunjoo Lee

doi:10.1016/j.apcatb.2015.02.033

Electronic structure modification of platinum on titanium nitride resulting in enhanced catalytic activity and durability for oxygen reduction and formic acid oxidation

Sungeun Yang, Dong Young Chung, Young Joo Tak, Jiwhan Kim, Haksu Han, Jong Sung Yu, Aloysius Soon, Yung Eun Sung, Hyunjoo Lee

Research output: Contribution to journal › Article › peer-review

56 Citations (Scopus)

Abstract

It is very important to improve the mass activity and durability of platinum (Pt) catalysts for oxygen reduction and the oxidation of small organic molecules for fuel cell applications. A strong interaction between Pt and the support materials can change the electronic structures of platinum, enhancing catalytic activity and durability. Here, we deposited various amounts of Pt on TiN supports and characterized these catalysts using electron microscopy, H₂ uptake, XANES, XPS, and valence-band XPS. The Pt nanoparticles had very small sizes (<2nm) with a narrow size distribution. Compared to a commercial Pt/C catalyst, the Pt surface in Pt/TiN catalysts was in a higher reduction state, and the Pt d-band center was downshifted. The results of DFT calculations confirmed that Pt could be stabilized on the TiN surface and that the Pt d-band center is downshifted relative to bulk Pt. The activity and durability of the Pt/TiN catalysts was enhanced for the oxygen reduction reaction and formic acid oxidation over that of the Pt/C catalyst. For the oxygen reduction reaction at 0.9V (vs. RHE), the mass activity was 0.29A/mg_Pt for the 10wt% Pt/TiN catalyst and 0.17A/mg_Pt for the Pt/C catalyst. After 5000 cycles of an accelerated durability test, the Pt/TiN exhibited a mass activity of 0.24A/mg_Pt, whereas the Pt/C catalyst exhibited a mass activity of 0.12A/mg_Pt. The Pt/TiN catalyst followed a direct pathway with fewer surface-poisoning intermediates for formic acid oxidation, which enhanced the activity of the Pt/TiN catalyst over that of the Pt/C catalyst. The modification of the electronic structure of Pt catalysts by interaction with TiN supports can significantly enhance the activity and durability of the catalyst.

Original language	English
Pages (from-to)	35-42
Number of pages	8
Journal	Applied Catalysis B: Environmental
Volume	174-175
DOIs	https://doi.org/10.1016/j.apcatb.2015.02.033
Publication status	Published - 2015 Sept 1

Bibliographical note

Funding Information:
This work was supported by the Global Frontier R&D Program on Center for Multiscale Energy System (2011-0031575) through National Research Foundation of Korea funded by the Ministry of Education, Science and Technology. The experiments at PLS were supported in part by MSIP and POSTECH.

Publisher Copyright:
© 2015 Elsevier B.V.

All Science Journal Classification (ASJC) codes

Catalysis
Environmental Science(all)
Process Chemistry and Technology

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10.1016/j.apcatb.2015.02.033

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Yang, S., Chung, D. Y., Tak, Y. J., Kim, J., Han, H., Yu, J. S., Soon, A., Sung, Y. E., & Lee, H. (2015). Electronic structure modification of platinum on titanium nitride resulting in enhanced catalytic activity and durability for oxygen reduction and formic acid oxidation. Applied Catalysis B: Environmental, 174-175, 35-42. https://doi.org/10.1016/j.apcatb.2015.02.033

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title = "Electronic structure modification of platinum on titanium nitride resulting in enhanced catalytic activity and durability for oxygen reduction and formic acid oxidation",

abstract = "It is very important to improve the mass activity and durability of platinum (Pt) catalysts for oxygen reduction and the oxidation of small organic molecules for fuel cell applications. A strong interaction between Pt and the support materials can change the electronic structures of platinum, enhancing catalytic activity and durability. Here, we deposited various amounts of Pt on TiN supports and characterized these catalysts using electron microscopy, H2 uptake, XANES, XPS, and valence-band XPS. The Pt nanoparticles had very small sizes (<2nm) with a narrow size distribution. Compared to a commercial Pt/C catalyst, the Pt surface in Pt/TiN catalysts was in a higher reduction state, and the Pt d-band center was downshifted. The results of DFT calculations confirmed that Pt could be stabilized on the TiN surface and that the Pt d-band center is downshifted relative to bulk Pt. The activity and durability of the Pt/TiN catalysts was enhanced for the oxygen reduction reaction and formic acid oxidation over that of the Pt/C catalyst. For the oxygen reduction reaction at 0.9V (vs. RHE), the mass activity was 0.29A/mgPt for the 10wt% Pt/TiN catalyst and 0.17A/mgPt for the Pt/C catalyst. After 5000 cycles of an accelerated durability test, the Pt/TiN exhibited a mass activity of 0.24A/mgPt, whereas the Pt/C catalyst exhibited a mass activity of 0.12A/mgPt. The Pt/TiN catalyst followed a direct pathway with fewer surface-poisoning intermediates for formic acid oxidation, which enhanced the activity of the Pt/TiN catalyst over that of the Pt/C catalyst. The modification of the electronic structure of Pt catalysts by interaction with TiN supports can significantly enhance the activity and durability of the catalyst.",

author = "Sungeun Yang and Chung, {Dong Young} and Tak, {Young Joo} and Jiwhan Kim and Haksu Han and Yu, {Jong Sung} and Aloysius Soon and Sung, {Yung Eun} and Hyunjoo Lee",

note = "Funding Information: This work was supported by the Global Frontier R&D Program on Center for Multiscale Energy System (2011-0031575) through National Research Foundation of Korea funded by the Ministry of Education, Science and Technology. The experiments at PLS were supported in part by MSIP and POSTECH. Publisher Copyright: {\textcopyright} 2015 Elsevier B.V.",

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doi = "10.1016/j.apcatb.2015.02.033",

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Electronic structure modification of platinum on titanium nitride resulting in enhanced catalytic activity and durability for oxygen reduction and formic acid oxidation. / Yang, Sungeun; Chung, Dong Young; Tak, Young Joo et al.

In: Applied Catalysis B: Environmental, Vol. 174-175, 01.09.2015, p. 35-42.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - Electronic structure modification of platinum on titanium nitride resulting in enhanced catalytic activity and durability for oxygen reduction and formic acid oxidation

AU - Yang, Sungeun

AU - Chung, Dong Young

AU - Tak, Young Joo

AU - Kim, Jiwhan

AU - Han, Haksu

AU - Yu, Jong Sung

AU - Soon, Aloysius

AU - Sung, Yung Eun

AU - Lee, Hyunjoo

N1 - Funding Information: This work was supported by the Global Frontier R&D Program on Center for Multiscale Energy System (2011-0031575) through National Research Foundation of Korea funded by the Ministry of Education, Science and Technology. The experiments at PLS were supported in part by MSIP and POSTECH. Publisher Copyright: © 2015 Elsevier B.V.

PY - 2015/9/1

Y1 - 2015/9/1

N2 - It is very important to improve the mass activity and durability of platinum (Pt) catalysts for oxygen reduction and the oxidation of small organic molecules for fuel cell applications. A strong interaction between Pt and the support materials can change the electronic structures of platinum, enhancing catalytic activity and durability. Here, we deposited various amounts of Pt on TiN supports and characterized these catalysts using electron microscopy, H2 uptake, XANES, XPS, and valence-band XPS. The Pt nanoparticles had very small sizes (<2nm) with a narrow size distribution. Compared to a commercial Pt/C catalyst, the Pt surface in Pt/TiN catalysts was in a higher reduction state, and the Pt d-band center was downshifted. The results of DFT calculations confirmed that Pt could be stabilized on the TiN surface and that the Pt d-band center is downshifted relative to bulk Pt. The activity and durability of the Pt/TiN catalysts was enhanced for the oxygen reduction reaction and formic acid oxidation over that of the Pt/C catalyst. For the oxygen reduction reaction at 0.9V (vs. RHE), the mass activity was 0.29A/mgPt for the 10wt% Pt/TiN catalyst and 0.17A/mgPt for the Pt/C catalyst. After 5000 cycles of an accelerated durability test, the Pt/TiN exhibited a mass activity of 0.24A/mgPt, whereas the Pt/C catalyst exhibited a mass activity of 0.12A/mgPt. The Pt/TiN catalyst followed a direct pathway with fewer surface-poisoning intermediates for formic acid oxidation, which enhanced the activity of the Pt/TiN catalyst over that of the Pt/C catalyst. The modification of the electronic structure of Pt catalysts by interaction with TiN supports can significantly enhance the activity and durability of the catalyst.

AB - It is very important to improve the mass activity and durability of platinum (Pt) catalysts for oxygen reduction and the oxidation of small organic molecules for fuel cell applications. A strong interaction between Pt and the support materials can change the electronic structures of platinum, enhancing catalytic activity and durability. Here, we deposited various amounts of Pt on TiN supports and characterized these catalysts using electron microscopy, H2 uptake, XANES, XPS, and valence-band XPS. The Pt nanoparticles had very small sizes (<2nm) with a narrow size distribution. Compared to a commercial Pt/C catalyst, the Pt surface in Pt/TiN catalysts was in a higher reduction state, and the Pt d-band center was downshifted. The results of DFT calculations confirmed that Pt could be stabilized on the TiN surface and that the Pt d-band center is downshifted relative to bulk Pt. The activity and durability of the Pt/TiN catalysts was enhanced for the oxygen reduction reaction and formic acid oxidation over that of the Pt/C catalyst. For the oxygen reduction reaction at 0.9V (vs. RHE), the mass activity was 0.29A/mgPt for the 10wt% Pt/TiN catalyst and 0.17A/mgPt for the Pt/C catalyst. After 5000 cycles of an accelerated durability test, the Pt/TiN exhibited a mass activity of 0.24A/mgPt, whereas the Pt/C catalyst exhibited a mass activity of 0.12A/mgPt. The Pt/TiN catalyst followed a direct pathway with fewer surface-poisoning intermediates for formic acid oxidation, which enhanced the activity of the Pt/TiN catalyst over that of the Pt/C catalyst. The modification of the electronic structure of Pt catalysts by interaction with TiN supports can significantly enhance the activity and durability of the catalyst.

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Electronic structure modification of platinum on titanium nitride resulting in enhanced catalytic activity and durability for oxygen reduction and formic acid oxidation

Abstract

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