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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction
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Regulating Spin Density using TEMPOL Molecules for Enhanced CO2-to-Ethylene Conversion by HKUST-1 Framework Derived
Baipeng Yin1, Can Wang2, Shijie Xie3
1Beijing National Laboratory for Molecular Sciences Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
Angewandte Chemie (International Ed. in English)
|May 6, 2024
Summary
Spin catalysts enhance carbon dioxide reduction to ethylene by controlling electron spin alignment at active sites. TEMPOL@HKUST-1 achieves higher selectivity through asymmetric spin configurations, boosting C-C coupling for sustainable chemical production.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- The selectivity of multicarbon products in CO2 reduction reaction (CO2RR) is dictated by the spin alignment of adjacent active sites.
- Developing spin catalysts that promote antiparallel electron spin transfer is crucial for enhancing C-C coupling and CO2RR efficiency.
Purpose of the Study:
- To design and synthesize a novel radical-contained spin catalyst, TEMPOL@HKUST-1, for enhanced CO2-to-ethylene conversion.
- To investigate the role of asymmetric spin configurations in facilitating CO2RR and C-C bond formation.
Main Methods:
- Fabrication of TEMPOL@HKUST-1 by incorporating TEMPOL radicals into HKUST-1, creating coexisting spin-disordered (SDO) and spin-ordered (SO) phases.
- Electrochemical evaluation of the catalyst's performance in CO2RR, including selectivity and current density measurements.
- In situ Attenuated Total Reflection Surface-Enhanced Infrared Absorption Spectroscopy (ATR-SEIRAS) to study reaction intermediates and kinetics.
Main Results:
- TEMPOL@HKUST-1 demonstrated a two-fold increase in ethylene selectivity compared to pristine HKUST-1 at -1.8 V vs. Ag/AgCl.
- The asymmetric SO/SDO spin configuration significantly lowered the kinetic barrier for *CO intermediate dimerization.
- Applying a magnetic field further improved catalyst performance, achieving over 50% ethylene selectivity.
Conclusions:
- The study highlights the importance of spin-polarized kinetics in CO2RR.
- TEMPOL@HKUST-1 serves as a promising spin electrocatalyst for efficient CO2 conversion to valuable multicarbon products like ethylene.
- This work opens avenues for designing advanced spin catalysts by manipulating spin configurations for targeted chemical transformations.
