Synergistic electronic structure modulation in single-atomic Ni sites dispersed on Ni nanoparticles encapsulated in N-rich carbon nanotubes synthesized at low temperature for efficient CO2 electrolysis
Ramireddy Boppella , Youngsam Kim , K. Arun Joshi Reddy , Inae Song , Yaeeun Eom , Eunji Sim , Tae Kyu Kim
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引用次数: 0
Abstract
Ni, N-doped carbon materials (Ni–N–C) are prosperous candidates for the electrochemical CO2 reduction reaction (CO2RR) due to their outstanding activity and selectivity. However, the role of the coexisting uncoordinated N-doped sites and Ni nanoparticles (Ni-NPs) in overall CO2RR has been overlooked in prior studies. To address this gap, a low temperature synthesis method developed for Ni-NP-encapsulated Ni–N–C nanotube (Ni-NCNT) catalysts with atomically dispersed Ni–N4 and abundant uncoordinated N-doped sites, where Ni-NPs increase the electron density on Ni–N–C nanotube through carbon network and synergistically enhances the CO2RR activity. The systematic analysis reveals the cooperative role of Ni-NPs and uncoordinated N-doped sites in altering the electronic structure of Ni–N4 sites. The results of control experimental studies confirm the synergistic interaction of uncoordinated N-doped sites boost the CO2RR activity of Ni–N4 sites. Additionally, density functional theory calculations show that the strong interaction between the Ni-NPs and Ni–N–C did not affect the electronic structures of the Ni–N4 centers, but rather alter the electronic structure of uncoordinated pyridinic-N sites. This variation led to decreased the energy barriers of rate-limiting steps of COOH* formation on Ni–N4 and N-doped sites, resulting in excellent CO2RR performance.
期刊介绍:
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.