Defect-Enhanced CO(2)Reduction Catalytic Performance in O-Terminated MXenes
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989100%3A27740%2F20%3A10245534" target="_blank" >RIV/61989100:27740/20:10245534 - isvavai.cz</a>
Result on the web
<a href="https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/cssc.202001624" target="_blank" >https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/cssc.202001624</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1002/cssc.202001624" target="_blank" >10.1002/cssc.202001624</a>
Alternative languages
Result language
angličtina
Original language name
Defect-Enhanced CO(2)Reduction Catalytic Performance in O-Terminated MXenes
Original language description
Electrochemical carbon dioxide reduction reaction (CO2RR) represents a promising way to generate fuels and chemical feedstock sustainably. Recently, studies have shown that two-dimensional metal carbides and nitrides (MXenes) can be promising CO2RR electrocatalysts due to the alternating -C and -H coordination with intermediates that decouples scaling relations seen on transition metal catalysts. However, further by tuning the electronic and surface structure of MXenes it should still be possible to reach higher turnover number and selectivities. To this end, defect engineering of MXenes for electrochemical CO2RR has not been investigated to date. In this work, first-principles modelling simulations are employed to systematically investigate CO2RR on M2XO2-type MXenes with transition metal and carbon/nitrogen vacancies. We found that the -C-coordinated intermediates take the form of fragments (e. g., *COOH, *CHO) whereas the -H-coordinated intermediates form a complete molecule (e. g., *HCOOH, *H2CO). Interestingly, the fragment-type intermediates become more strongly bound when transition-metal vacancies are present on most MXenes, while the molecule-type intermediates are largely unaffected, allowing the CO2RR overpotential to be tuned. The most promising defective MXene is Hf(2)NO(2)containing Hf vacancies, with a low overpotential of 0.45 V. More importantly, through electronic structure analysis it could be observed that the Fermi level of the MXene changes significantly in the presence of vacancies, indicating that the Fermi level shift can be used as an ideal descriptor to rapidly predict the catalytic performance of defective MXenes. Such an evaluation strategy is applicable to other catalysts beyond MXenes, which could enhance high throughput screening efforts for accelerated catalyst discovery.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10302 - Condensed matter physics (including formerly solid state physics, supercond.)
Result continuities
Project
Result was created during the realization of more than one project. More information in the Projects tab.
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)
Others
Publication year
2020
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
ChemSusChem
ISSN
1864-5631
e-ISSN
—
Volume of the periodical
13
Issue of the periodical within the volume
21
Country of publishing house
DE - GERMANY
Number of pages
10
Pages from-to
"5690–5698"
UT code for WoS article
000567456100001
EID of the result in the Scopus database
2-s2.0-85090434186