Highly Dispersed Ni on Nitrogen-Doped Carbon for Stable and Selective Hydrogen Generation from Gaseous Formic Acid

• Published in: Nanomaterials (Basel, Switzerland) Vol. 13; no. 3; p. 545
• Main Authors: Nishchakova, Alina D, Bulushev, Dmitri A, Trubina, Svetlana V, Stonkus, Olga A, Shubin, Yury V, Asanov, Igor P, Kriventsov, Vladimir V, Okotrub, Alexander V, Bulusheva, Lyubov G
• Format: Journal Article
• Language: English
• Published: Switzerland MDPI AG 29-01-2023; MDPI
• Subjects: Acids; Analysis; Atomic properties; Atoms & subatomic particles; Carbon; Catalysts; Chemical vapor deposition; Clustering; Decomposition; Density functional theory; Density functionals; Energy consumption; Formic acid; Hydrogen; Hydrogen production; Hydrogenation; Metals; Methods; N-doped carbon; Nanoparticles; Ni clusters; Ni nanoparticles; Ni single-atom catalyst; Nickel; Nitrogen; Properties; Selectivity; Spectrum analysis; Structure; Russia; Ni nanoparticles; formic acid; N-doped carbon; Ni clusters; hydrogen production; Ni single-atom catalyst
• ISSN: 2079-4991; 2079-4991
• DOI: 10.3390/nano13030545

Ni supported on N-doped carbon is rarely studied in traditional catalytic reactions. To fill this gap, we compared the structure of 1 and 6 wt% Ni species on porous N-free and N-doped carbon and their efficiency in hydrogen generation from gaseous formic acid. On the N-free carbon support, Ni formed nanoparticles with a mean size of 3.2 nm. N-doped carbon support contained Ni single-atoms stabilized by four pyridinic N atoms (N
-site) and sub-nanosized Ni clusters. Density functional theory calculations confirmed the clustering of Ni when the N
-sites were fully occupied. Kinetic studies revealed the same specific Ni mass-based reaction rate for single-atoms and clusters. The N-doped catalyst with 6 wt% of Ni showed higher selectivity in hydrogen production and did not lose activity as compared to the N-free 6 wt% Ni catalyst. The presented results can be used to develop stable Ni catalysts supported on N-doped carbon for various reactions.