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Effects of the carbon support doping with nitrogen for the hydrogen production from formic acid over Ni catalysts. / Nishchakova, Alina D.; Bulushev, Dmitri A.; Stonkus, Olga A. et al.
In: Energies, Vol. 12, No. 21, 4111, 11.2019.Research output: Contribution to journal › Article › peer-review
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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 -
ID: 22403056