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Journal article
Highly efficient CO2 electrochemical reduction on dual metal (Co-Ni)-nitrogen sites
Journal of materials chemistry. A, Materials for energy and sustainability, Vol.12(8), pp.4601-4609
02/20/2024
Web of Science ID: WOS:001146692100001
Abstract
The electrochemical reduction (ECR) of CO2 is a promising approach for CO2 removal and utilization, which is a critical component of the circular carbon economy. However, developing efficient and selective electrocatalysts is still challenging. Single-atom catalysts (SACs) have gained attention because they offer high metal atom utilization and uniform active sites. However, tuning the active metal centres to achieve high activity and selectivity in CO2 reduction remains a significant challenge. This study presents a novel electrocatalyst (Co-Ni-N-C) for CO2 ECR on the diatomic metal-nitrogen sites prepared through ion exchange using a zeolitic imidazolate framework (ZIF) as a precursor. During pyrolysis, nitrogen-doped graphitic carbon serves as the host material, anchoring the diatomic Co-Ni sites. The resulting bimetallic active sites demonstrate exceptional performance, achieving a high CO yield rate of 53.36 mA mg(cat.)(-1) and an impressive CO faradaic efficiency of 94.1% at an overpotential of -0.27 V. Spectroscopic, microscopic, and density functional theory (DFT) analyses collectively unveil the crucial synergistic role of the Co-Ni-N-6 moiety in promoting and sustaining exceptional electrocatalytic activities. The successful utilization of bimetallic sites in enhancing catalyst performance highlights the potential of this approach in developing efficient electrocatalysts for various other reactions.
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- Title
- Highly efficient CO2 electrochemical reduction on dual metal (Co-Ni)-nitrogen sites
- Publication Details
- Journal of materials chemistry. A, Materials for energy and sustainability, Vol.12(8), pp.4601-4609
- Resource Type
- Journal article
- Publisher
- Royal Society of Chemistry
- Number of pages
- 9
- Grant note
- Division of Civil, Mechanical and Manufacturing Innovation: CBET-1856729 National Science Foundation: W911NF-23-1-0196 Department of Defence: DE-AC02-07CH11358 Iowa State UniversityNational Energy Research Scientific Computing Center, a DOE Office of Science User Facility: BES-ERCAP0020838 Office of Science of the U.S. Department of Energy
Financial supports from the National Science Foundation (CMMI-1727553) and Department of Defence (W911NF-23-1-0196) are gratefully acknowledged. Md Robayet Ahasan and Ruigang Wang acknowledge the financial support from the National Science Foundation (CBET-1856729). AC-HAADF-STEM was performed in the Sensitive Instrument Facility at Ames Laboratory, which is operated for the U.S. DOE by Iowa State University under Contract No. DE-AC02-07CH11358. The DFT computational part used resources from the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 using NERSC award BES-ERCAP0020838. High-Performance Computing resources provided by the High-Performance Research Computing (HPRC) Core Facility at Virginia Commonwealth University (https://chipc.vcu.edu) were also used for conducting the research reported in this work.
- Identifiers
- WOS:001146692100001; 99381548016906600
- Academic Unit
- Chemistry; Hal Marcus College of Science and Engineering
- Language
- English