TY - JOUR
T1 - Descriptor-Based Design Principle for Two-Dimensional Single-Atom Catalysts
T2 - Carbon Dioxide Electroreduction
AU - Yuan, Hao
AU - Li, Zhenyu
AU - Zeng, Xiao Cheng
AU - Yang, Jinlong
N1 - Copyright:
This record is sourced from MEDLINE/PubMed, a database of the U.S. National Library of Medicine
PY - 2020/5/7
Y1 - 2020/5/7
N2 - Single-atom catalysis has recently emerged as a promising approach for catalyzing the carbon dioxide reduction reaction (CO2RR). In this study, we present a principle for designing active single-atom catalysts (SACs) for CO2RR. We systematically examine totally 24 transition metals supported by a graphitic carbon nitride (g-CN) monolayer and find that their catalytic activities are highly correlated with the adsorption free energies of two intermediate species (OH and OCH). We then identify two important intrinsic descriptors, namely, the number of electrons in the outmost d-shell and the enthalpy of vaporization of the transition metal. Test calculations on transition metals supported by a C2N monolayer indicate that both descriptors are quite universal for SACs of CO2RR. Based on these results, we show that Ni@g-CN, Cu@g-CN, and Co@C2N are promising SACs for CO2RR. This study offers an effective principle for designing highly active SACs for CO2RR on the basis of intrinsic properties of transition metals.
AB - Single-atom catalysis has recently emerged as a promising approach for catalyzing the carbon dioxide reduction reaction (CO2RR). In this study, we present a principle for designing active single-atom catalysts (SACs) for CO2RR. We systematically examine totally 24 transition metals supported by a graphitic carbon nitride (g-CN) monolayer and find that their catalytic activities are highly correlated with the adsorption free energies of two intermediate species (OH and OCH). We then identify two important intrinsic descriptors, namely, the number of electrons in the outmost d-shell and the enthalpy of vaporization of the transition metal. Test calculations on transition metals supported by a C2N monolayer indicate that both descriptors are quite universal for SACs of CO2RR. Based on these results, we show that Ni@g-CN, Cu@g-CN, and Co@C2N are promising SACs for CO2RR. This study offers an effective principle for designing highly active SACs for CO2RR on the basis of intrinsic properties of transition metals.
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U2 - 10.1021/acs.jpclett.0c00676
DO - 10.1021/acs.jpclett.0c00676
M3 - Article
C2 - 32298119
AN - SCOPUS:85084379685
VL - 11
SP - 3481
EP - 3487
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 9
ER -