On the Feasibility of Bifunctional Hydrogen Oxidation on Ni and NiCu Surfaces | Sciact - CRIS-система Института катализа

On the Feasibility of Bifunctional Hydrogen Oxidation on Ni and NiCu Surfaces Научная публикация

Журнал

Electrochimica Acta
ISSN: 0013-4686 , E-ISSN: 1873-3859

Вых. Данные

Год: 2019, Том: 305, Страницы: 452-458 Страниц : 7 DOI: 10.1016/j.electacta.2019.03.030

Ключевые слова

Hydrogen oxidation reaction, Nickel and nickel copper, Bifunctional mechanism, DFT and Monte Carlo simulations, Kinetic modeling

Авторы

Salmazo D. ^1,5 , Juarez M.F. ¹ , Oshchepkov A.G. ² , Cherstiouk O.V. ² , Bonnefont A. ³ , Shermukhamedov S.A. ⁴ , Nazmutdinov R.R. ⁴ , Schmickler W. ¹ , Savinova E.R. ⁵

Организации

1	Institute of Theoretical Chemistry, Ulm University, D-89069, Ulm, Germany
2	Boreskov Institute of Catalysis, Novosibirsk, 630090, Russia
3	Institut de Chimie de Strasbourg, UMR 7177, CNRS-University of Strasbourg, 67070, Strasbourg, France
4	Kazan National Research Technological University, 420015, Kazan, Russian Federation
5	ICPEES, UMR 7515, CNRS-University of Strasbourg, 67087, Strasbourg Cedex, France

Информация о финансировании (3)

1	Российский фонд фундаментальных исследований	17-53-150008
2	National Scientific and Technical Research Council
3	National Council for Scientific and Technological Development	248817/2013-2

Nickel is a promising alternative to noble metal catalysts for hydrogen electrocatalysis in alkaline membrane fuel cells and electrolyzers. To boost its electrocatalytic activity, it is often associated with other metals, like Cu. In this work, we combine density functional theory (DFT), Monte Carlo calculations and kinetic modeling in order to shed light on the origin of the experimentally observed activity enhancement on bimetallic NiCu nanoparticles containing ca. 5% of Cu compared to pure Ni (Topics in Catalysis, 58, (2015), 1181–1192; J. Electroanal. Chem., 783, (2016), 146–151). It is shown that the bifunctional HOR mechanism, where H ad and OH ad recombine to form water, is not viable on the monometallic Ni electrode because of the strong hydrogen adsorption and the high activation energy barrier of the recombination reaction. On bimetallic NiCu surfaces, DFT calculations predict a significant weakening of H ad adsorption energy as well as a decrease of the activation barrier of the recombination reaction for ca. 50% Cu surface coverage. Monte Carlo simulations reveal that the surface of NiCu nanoparticles is enriched in Cu atoms even for a small (ca. 5%) Cu atomic fraction in the bulk. Kinetic modeling suggests that the experimental data for NiCu nanoparticles can be well reproduced either considering fast recombination step (bifunctional mechanism) or fast (10-fold enhancement compared to pure Ni) Volmer step (Heyrovsky-Volmer mechanism). © 2019 Elsevier Ltd

Salmazo D. , Juarez M.F. , Oshchepkov A.G. , Cherstiouk O.V. , Bonnefont A. , Shermukhamedov S.A. , Nazmutdinov R.R. , Schmickler W. , Savinova E.R.
On the Feasibility of Bifunctional Hydrogen Oxidation on Ni and NiCu Surfaces
Electrochimica Acta. 2019. V.305. P.452-458. DOI: 10.1016/j.electacta.2019.03.030 WOS Scopus РИНЦ CAPlus OpenAlex

Поступила в редакцию:	31 окт. 2018 г.
Принята к публикации:	4 мар. 2019 г.
Опубликована online:	7 мар. 2019 г.
Опубликована в печати:	10 мая 2019 г.

Web of science:	WOS:000462774000049
Scopus:	2-s2.0-85063101730
РИНЦ:	38671514
Chemical Abstracts:	2019:563757
OpenAlex:	W2921909752

БД	Цитирований
Scopus	31
Web of science	30
РИНЦ	26
OpenAlex	32