TY - JOUR

T1 - Liquid versus gas phase dehydrogenation of formic acid over Co@N-doped carbon materials. The role of single atomic sites

AU - Chernov, Aleksey N.

AU - Astrakova, Tatiana V.

AU - Sobolev, Vladimir I.

AU - Koltunov, Konstantin Yu

N1 - Funding Information: This work was supported by the Ministry of Science and Higher Education of the Russian Federation within the governmental order for Boreskov Institute of Catalysis (project АААА-А21-121011390008-4 ). The studies were carried out using facilities of the shared research center “National center of investigation of catalysts” at Boreskov Institute of Catalysis. Publisher Copyright: © 2021 Elsevier B.V.

PY - 2021/3

Y1 - 2021/3

N2 - N-doped carbon nanomaterials containing certain transition metals have recently attracted significant interest as the promising noble-metal-free composites for a variety of applications, including in particular catalytic generation of molecular hydrogen from formic acid (FA). This reaction is increasingly becoming essential for advanced hydrogen energy technologies in the area of energy storage and conversion devices. Here, we report a comparative study on FA decomposition over Co@N-doped carbon materials obtained by a variety of synthetic approaches. The reaction was examined under both liquid- and gas-phase conditions. Most notably, it has been shown that a technologically rather simple method for the preparation of Co@N-doped carbon, which is based on physical mixing (solid-state grinding) of cobalt(II) salts, nitrogen-containing ligands and carbon black, followed by pyrolysis, leads to the desired and highly competitive catalytic performance. The key role of single atomic catalytic sites is discussed to provide the catalytic properties of Co@N-carbon materials toward FA dehydrogenation regardless of peculiarities of their preparation method.

AB - N-doped carbon nanomaterials containing certain transition metals have recently attracted significant interest as the promising noble-metal-free composites for a variety of applications, including in particular catalytic generation of molecular hydrogen from formic acid (FA). This reaction is increasingly becoming essential for advanced hydrogen energy technologies in the area of energy storage and conversion devices. Here, we report a comparative study on FA decomposition over Co@N-doped carbon materials obtained by a variety of synthetic approaches. The reaction was examined under both liquid- and gas-phase conditions. Most notably, it has been shown that a technologically rather simple method for the preparation of Co@N-doped carbon, which is based on physical mixing (solid-state grinding) of cobalt(II) salts, nitrogen-containing ligands and carbon black, followed by pyrolysis, leads to the desired and highly competitive catalytic performance. The key role of single atomic catalytic sites is discussed to provide the catalytic properties of Co@N-carbon materials toward FA dehydrogenation regardless of peculiarities of their preparation method.

KW - Cobalt-nitrogen-carbon catalyst

KW - Dehydrogenation

KW - Energy storage

KW - Formic acid

KW - Heterogeneous catalysis

UR - http://www.scopus.com/inward/record.url?scp=85101146514&partnerID=8YFLogxK

U2 - 10.1016/j.mcat.2021.111457

DO - 10.1016/j.mcat.2021.111457

M3 - Article

AN - SCOPUS:85101146514

VL - 504

JO - Molecular Catalysis

JF - Molecular Catalysis

SN - 2468-8231

M1 - 111457

ER -