In:
Energy & Environmental Science, Royal Society of Chemistry (RSC), Vol. 16, No. 2 ( 2023), p. 502-512
Abstract:
Electrochemical CO 2 conversion into highly value-added dialkyl carbonate by coupling cathodic CO 2 reduction reactions with anodic oxidation reactions is prospective. However, the structures of electrocatalysts should be well conquered for achieving high faradaic efficiency (FE) of dialkyl carbonate. In this work, a dual-channel superstructured Ni single-atom catalyst (SAC) with a unique site coordination configuration bonded via one axial oxygen atom and four planar nitrogen atoms was controllably constructed and is capable of providing a preeminent performance for CO 2 -to-CO conversion, achieving an exclusively high FE and a partial current density of CO (99% of FE, 325 mA cm −2 @−0.6 V vs. RHE) with excellent stability. By virtue of the atomic to nano- to micro-scopic manipulation of the pentacoordinated Ni SAC for CO production, the convergent paired electrosynthesis of dimethyl carbonate (DMC) from CO 2 was pioneeringly performed, achieving a high FE of DMC up to 80%. The mechanism study unveiled that such axial oxygen coordination configuration is helpful to decrease the energy barriers for the generation of a key *COOH intermediate and the dissociation of H 2 O and CH 3 OH, accelerating the convergent paired electrosynthesis. The proof of concept in the innovative convergent paired electrosynthesis could open up a new horizon in the fields of CO 2 utilization.
Type of Medium:
Online Resource
ISSN:
1754-5692
,
1754-5706
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2023
detail.hit.zdb_id:
2439879-2
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