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
Nikolaev Institute of Inorganic Chemistry SB RAS, 3 Acad. Lavrentiev Ave., 630090 Novosibirsk, Russia.
Boreskov Institute of Catalysis SB RAS, 5 Acad. Lavrentiev Ave., 630090 Novosibirsk, Russia.
Nanomaterials (Basel). 2023 Jan 29;13(3):545. 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.
负载在氮掺杂碳上的镍在传统催化反应中很少被研究。为了填补这一空白，我们比较了在多孔无氮和氮掺杂碳上1 wt%和6 wt%镍物种的结构及其从气态甲酸制氢的效率。在无氮碳载体上，镍形成了平均尺寸为3.2 nm的纳米颗粒。氮掺杂碳载体包含由四个吡啶氮原子（N位）稳定的镍单原子和亚纳米级镍簇。密度泛函理论计算证实了当N位被完全占据时镍的聚集。动力学研究表明单原子和簇的基于镍质量的比反应速率相同。与含6 wt%镍的无氮催化剂相比，含6 wt%镍的氮掺杂催化剂在制氢方面表现出更高的选择性且不失活。所呈现的结果可用于开发用于各种反应的负载在氮掺杂碳上的稳定镍催化剂。
