Journal
NANO ENERGY
Volume 87, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.nanoen.2021.106187
Keywords
Bioelectrochemical system; CO2 electroreduction; Integrated device; Atomic-level Fe-N-4 sites; Hierarchical porous carbon
Categories
Funding
- National Natural Science Foundation of China [21922811, 21878270, 21961160742]
- Zhejiang Provincial Natural Science Foundation of China [LR19B060002]
- Fundamental Research Funds for the Central Universities [2020XZZX002-09]
- Startup Foundation for Hundred-Talent Program of Zhejiang University
- Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang [2019R01006]
- Key Laboratory of Marine Materials and Related Technologies, CAS
- Zhejiang Key Laboratory of Marine Materials and Protective Technologies
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The CO2ER catalyst Fe SA-NC, prepared through a unique Fe-Nx molecular-confined pyrolysis strategy, exhibited superior performance in terms of low overpotential, small Tafel slope, and high Faradaic efficiency. Experimental results and theoretical calculations both demonstrated the crucial role of Fe-N-4 sites in enhancing reaction kinetics.
Integrating a bioelectrochemical system with CO2 electroreduction (CO2ER) can achieve recovery of resources and conversion of value-added chemicals, but it still faces challenge of high overpotential and poor selectivity. Herein, we report a CO2ER catalyst with iron bonded to nitrogen atoms (Fe-Nx) anchored hierarchical porous carbon (Fe SA-NC) by a molecular-confined pyrolysis strategy. Owing to the high surface area and atomic-level Fe-N-4 sites, Fe SA-NC possessed superior CO2-to-CO conversion performance with a low overpotential of 90 mV, a small Tafel slope of 92 mV dec(-1), and high Faradaic efficiency of 95.9% at 0.5 V, superior to almost all previously reported Fe-Nx based carbon materials for CO2ER. Experimental results manifested the atomic-level Fe-N-4 sites in carbon frameworks with a single Fe atom coordinating four N atoms. Theoretical calculations revealed Fe-N-4 sites weaken the free energy for the formation of *COOH intermediate, and the short Fe-C bond length in the structure of *COOH absorbed on Fe-N-4 sites accelerated the electron transfer from Fe-N-4 centers to *COOH, thus boosting the reaction kinetics. An integrated device with cathodic Fe SA-NC and bioanode can recover energy and carbon resource from wastewater, delivering maximum current and CO production rate of 1.54 +/- 0.05 mA and 33.66 +/- 0.58 mmol g(cat)(-1) h(-1).
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