In:
Journal of Materials Chemistry A, Royal Society of Chemistry (RSC), Vol. 12, No. 18 ( 2024), p. 11090-11100
Abstract:
Electrochemical reduction of CO 2 to chemical fuels with a transition metal-based single atom catalyst (SAC) offers a promising strategy to reduce CO 2 with high catalytic selectivity. To date, the study of atomically dispersed SACs has been mainly conducted by using a conventional H-type cell system with limited solubility of CO 2 in aqueous electrolytes, resulting in large overpotentials and low current density. Here, we reported a pyrrolic N-stabilized Ni SAC with low-coordinated Ni–N x sites by thermal activation of Ni ZIF-8, which was tested in a 3-compartment microfluidic flow cell system at the industrial level. When the pyrolysis temperature increased from 800 °C (Ni SAC-800) to 1000 °C (Ni SAC-1000), the content ratio of pyrrolic N/pyridinic N increased from 0.37 to 1.01 as well as the coordination number of Ni in Ni–N x sites decreased from 3.14 to 2.63. Theoretical calculations revealed that the synergistic effect between the high content ratio of pyrrolic N and low-coordinated Ni can decrease the energy barrier for the desorption of *CO during the CO 2 RR. Therefore, Ni SAC-1000 exhibited superior catalytic performances with high CO selectivity (FE CO = 98.24% at −0.8 V RHE ) compared to that of Ni SAC-800 (FE CO = 40.76% at −0.8 V RHE ). Moreover, Ni SAC-1000 based on the flow cell system showed a higher current density (∼200 mA cm −2 ) compared to that of the H-type cell system (∼20 mA cm −2 ). As a result, this study experimentally demonstrated that the pyrrolic N-stabilized and low-coordinated Ni SAC-1000 in the microfluidic flow cell reactor provides great chances for scaling up the productivity of the CO 2 RR at the industrial level.
Type of Medium:
Online Resource
ISSN:
2050-7488
,
2050-7496
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2024
detail.hit.zdb_id:
2702232-8
detail.hit.zdb_id:
2696984-1
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