TY - JOUR

T1 - Effects of the carbon support doping with nitrogen for the hydrogen production from formic acid over Ni catalysts

AU - Nishchakova, Alina D.

AU - Bulushev, Dmitri A.

AU - Stonkus, Olga A.

AU - Asanov, Igor P.

AU - Ishchenko, Arcady V.

AU - Okotrub, Alexander V.

AU - Bulusheva, Lyubov G.

PY - 2019/11

Y1 - 2019/11

N2 - Porous nitrogen-doped and nitrogen-free carbon materials possessing high specific surface areas (400-1000 m2 g-1) were used for deposition of Ni by impregnation with nickel acetate followed by reduction. The nitrogen-doped materials synthesized by decomposition of acetonitrile at 973, 1073, and 1173 K did not differ much in the total content of incorporated nitrogen (4-5 at%), but differed in the ratio of the chemical forms of nitrogen. An X-ray photoelectron spectroscopy study showed that the rise in the synthesis temperature led to a strong growth of the content of graphitic nitrogen on the support accompanied by a reduction of the content of pyrrolic nitrogen. The content of pyridinic nitrogen did not change significantly. The prepared nickel catalysts supported on nitrogen-doped carbons showed by a factor of up to two higher conversion of formic acid as compared to that of the nickel catalyst supported on the nitrogen-free carbon. This was related to stabilization of Ni in the state of single Ni2+ cations or a few atoms clusters by the pyridinic nitrogen sites. The nitrogen-doped nickel catalysts possessed a high stability in the reaction at least within 5 h and a high selectivity to hydrogen (97%). 2019 by the authors.

AB - Porous nitrogen-doped and nitrogen-free carbon materials possessing high specific surface areas (400-1000 m2 g-1) were used for deposition of Ni by impregnation with nickel acetate followed by reduction. The nitrogen-doped materials synthesized by decomposition of acetonitrile at 973, 1073, and 1173 K did not differ much in the total content of incorporated nitrogen (4-5 at%), but differed in the ratio of the chemical forms of nitrogen. An X-ray photoelectron spectroscopy study showed that the rise in the synthesis temperature led to a strong growth of the content of graphitic nitrogen on the support accompanied by a reduction of the content of pyrrolic nitrogen. The content of pyridinic nitrogen did not change significantly. The prepared nickel catalysts supported on nitrogen-doped carbons showed by a factor of up to two higher conversion of formic acid as compared to that of the nickel catalyst supported on the nitrogen-free carbon. This was related to stabilization of Ni in the state of single Ni2+ cations or a few atoms clusters by the pyridinic nitrogen sites. The nitrogen-doped nickel catalysts possessed a high stability in the reaction at least within 5 h and a high selectivity to hydrogen (97%). 2019 by the authors.

KW - Formic acid decomposition

KW - Hydrogen production

KW - Nickel catalyst

KW - Nitrogen doping

KW - Porous carbon support

KW - SINGLE ATOMS

KW - OXIDE

KW - formic acid decomposition

KW - DECOMPOSITION

KW - hydrogen production

KW - PD/C

KW - nitrogen doping

KW - COPPER-NICKEL-ALLOYS

KW - nickel catalyst

KW - porous carbon support

UR - http://www.scopus.com/inward/record.url?scp=85075569939&partnerID=8YFLogxK

U2 - 10.3390/en12214111

DO - 10.3390/en12214111

M3 - Article

AN - SCOPUS:85075569939

VL - 12

JO - Energies

JF - Energies

SN - 1996-1073

IS - 21

M1 - 4111

ER -