Trace level of atomic copper in N-doped graphene quantum dots switching the selectivity from C1 to C2 products in CO electroreduction

X. Lyu; T. Zhang; Z. Li; C. J. Jafta; A. Serov; I. H. Hwang; C. Sun; D. A. Cullen; J. Li; J. Wu

doi:10.1016/j.mtchem.2023.101398

Trace level of atomic copper in N-doped graphene quantum dots switching the selectivity from C₁ to C₂ products in CO electroreduction

X. Lyu, T. Zhang, Z. Li, C. J. Jafta, A. Serov, I. H. Hwang, C. Sun, D. A. Cullen, J. Li, J. Wu

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

To unravel the relationship between trace Cu on the metal-free catalysts toward CO/CO₂ reduction reaction (CO/CO₂RR), we investigated the effect of trace Cu loading in N-doped graphene quantum dots (NGQDs) on CO/CO₂RR. A general trend is that increasing the Cu loading in NGQDs switches the selectivity from C₁ (CH₄) to C₂ products in CORR. When 2.5 μg/cm² Cu with the atomic size is loaded on NGQDs, the selectivity shifts from 62% Faradaic efficiency (FE) of CH₄ to 52% FE of C₂ products in CORR. Further increasing the atomic Cu loading to 3.8 μg/cm² promotes the FE of C₂ products to 78%. CO₂RR requires one order of magnitude higher Cu loading than CORR to switch the selectivity from C₁ to C₂ products due to the low partial pressure of CO. This study clarifies the distinct impact of trace (ppm level) Cu on the activity/selectivity between CORR and CO₂RR.

Original language	English
Article number	101398
Journal	Materials Today Chemistry
Volume	29
DOIs	https://doi.org/10.1016/j.mtchem.2023.101398
State	Published - Apr 2023

Funding

This work is partially supported by the Office of Fossil Energy and Carbon Management of the U.S. Department of Energy under Award Number DE-FE0031919 . This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357 , and the Canadian Light Source and its funding partners.

Funders	Funder number
U.S. Department of Energy	DE-FE0031919, DE-AC02-06CH11357
Office of Science
Argonne National Laboratory
Canadian Light Source
Office of Fossil Energy and Carbon Management

Keywords

Acetate
CORR
CORR
Graphene quantum dots
Trace copper

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.mtchem.2023.101398

Cite this

@article{78629eedcdc7473bad2d0fe114393fd2,

title = "Trace level of atomic copper in N-doped graphene quantum dots switching the selectivity from C1 to C2 products in CO electroreduction",

abstract = "To unravel the relationship between trace Cu on the metal-free catalysts toward CO/CO2 reduction reaction (CO/CO2RR), we investigated the effect of trace Cu loading in N-doped graphene quantum dots (NGQDs) on CO/CO2RR. A general trend is that increasing the Cu loading in NGQDs switches the selectivity from C1 (CH4) to C2 products in CORR. When 2.5 μg/cm2 Cu with the atomic size is loaded on NGQDs, the selectivity shifts from 62% Faradaic efficiency (FE) of CH4 to 52% FE of C2 products in CORR. Further increasing the atomic Cu loading to 3.8 μg/cm2 promotes the FE of C2 products to 78%. CO2RR requires one order of magnitude higher Cu loading than CORR to switch the selectivity from C1 to C2 products due to the low partial pressure of CO. This study clarifies the distinct impact of trace (ppm level) Cu on the activity/selectivity between CORR and CO2RR.",

keywords = "Acetate, CORR, CORR, Graphene quantum dots, Trace copper",

author = "X. Lyu and T. Zhang and Z. Li and Jafta, {C. J.} and A. Serov and Hwang, {I. H.} and C. Sun and Cullen, {D. A.} and J. Li and J. Wu",

note = "Publisher Copyright: {\textcopyright} 2023 Elsevier Ltd",

year = "2023",

month = apr,

doi = "10.1016/j.mtchem.2023.101398",

language = "English",

volume = "29",

journal = "Materials Today Chemistry",

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T1 - Trace level of atomic copper in N-doped graphene quantum dots switching the selectivity from C1 to C2 products in CO electroreduction

AU - Lyu, X.

AU - Zhang, T.

AU - Li, Z.

AU - Jafta, C. J.

AU - Serov, A.

AU - Hwang, I. H.

AU - Sun, C.

AU - Cullen, D. A.

AU - Li, J.

AU - Wu, J.

PY - 2023/4

Y1 - 2023/4

N2 - To unravel the relationship between trace Cu on the metal-free catalysts toward CO/CO2 reduction reaction (CO/CO2RR), we investigated the effect of trace Cu loading in N-doped graphene quantum dots (NGQDs) on CO/CO2RR. A general trend is that increasing the Cu loading in NGQDs switches the selectivity from C1 (CH4) to C2 products in CORR. When 2.5 μg/cm2 Cu with the atomic size is loaded on NGQDs, the selectivity shifts from 62% Faradaic efficiency (FE) of CH4 to 52% FE of C2 products in CORR. Further increasing the atomic Cu loading to 3.8 μg/cm2 promotes the FE of C2 products to 78%. CO2RR requires one order of magnitude higher Cu loading than CORR to switch the selectivity from C1 to C2 products due to the low partial pressure of CO. This study clarifies the distinct impact of trace (ppm level) Cu on the activity/selectivity between CORR and CO2RR.

AB - To unravel the relationship between trace Cu on the metal-free catalysts toward CO/CO2 reduction reaction (CO/CO2RR), we investigated the effect of trace Cu loading in N-doped graphene quantum dots (NGQDs) on CO/CO2RR. A general trend is that increasing the Cu loading in NGQDs switches the selectivity from C1 (CH4) to C2 products in CORR. When 2.5 μg/cm2 Cu with the atomic size is loaded on NGQDs, the selectivity shifts from 62% Faradaic efficiency (FE) of CH4 to 52% FE of C2 products in CORR. Further increasing the atomic Cu loading to 3.8 μg/cm2 promotes the FE of C2 products to 78%. CO2RR requires one order of magnitude higher Cu loading than CORR to switch the selectivity from C1 to C2 products due to the low partial pressure of CO. This study clarifies the distinct impact of trace (ppm level) Cu on the activity/selectivity between CORR and CO2RR.

KW - Acetate

KW - CORR

KW - Graphene quantum dots

KW - Trace copper

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