Understanding the Origin of Highly Selective CO 2 Electroreduction to CO on Ni,N‐doped Carbon Catalysts
[2];
- SUNCAT Center for Interface Science and Catalysis Department of Chemical Engineering Stanford University Stanford CA 94305 USA
- Department of Chemical Engineering McMaster University Hamilton ON Canada
- Department of Materials Science and Engineering Stanford University Stanford CA 94305 USA
- Stanford Synchotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
- SUNCAT Center for Interface Science and Catalysis SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
- SUNCAT Center for Interface Science and Catalysis Department of Chemical Engineering Stanford University Stanford CA 94305 USA, SUNCAT Center for Interface Science and Catalysis SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
Abstract Ni,N‐doped carbon catalysts have shown promising catalytic performance for CO 2 electroreduction (CO 2 R) to CO; this activity has often been attributed to the presence of nitrogen‐coordinated, single Ni atom active sites. However, experimentally confirming Ni−N bonding and correlating CO 2 reduction (CO 2 R) activity to these species has remained a fundamental challenge. We synthesized polyacrylonitrile‐derived Ni,N‐doped carbon electrocatalysts (Ni‐PACN) with a range of pyrolysis temperatures and Ni loadings and correlated their electrochemical activity with extensive physiochemical characterization to rigorously address the origin of activity in these materials. We found that the CO 2 R to CO partial current density increased with increased Ni content before plateauing at 2 wt % which suggests a dispersed Ni active site. These dispersed active sites were investigated by hard and soft X‐ray spectroscopy, which revealed that pyrrolic nitrogen ligands selectively bind Ni atoms in a distorted square‐planar geometry that strongly resembles the active sites of molecular metal–porphyrin catalysts.
- Sponsoring Organization:
- USDOE
- OSTI ID:
- 1595529
- Journal Information:
- Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 132 Journal Issue: 10; ISSN 0044-8249
- Publisher:
- Wiley Blackwell (John Wiley & Sons)Copyright Statement
- Country of Publication:
- Germany
- Language:
- English
Similar Records
Atomically dispersed single Ni site catalysts for high-efficiency CO2 electroreduction at industrial-level current densities
Direct Characterization of Atomically Dispersed Catalysts: Nitrogen-Coordinated Ni Sites in Carbon-Based Materials for CO2 Electroreduction