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Issue 40, 2020
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Nb2BN2 cluster anions reduce four carbon dioxide molecules: reactivity enhancement by ligands

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Abstract

The thermal gas-phase reactions of Nb2BN2 cluster anions with carbon dioxide have been explored by using the art of time-of-flight mass spectrometry and density functional theory calculations. Four CO2 molecules can be consecutively reduced by Nb2BN2, resulting in the formation of Nb2BN2O1–4 anions and the release of one CO molecule each time. To illustrate the role of ligands in Nb2BN2, the reactivities of Nb2N2 and Nb2B toward CO2 were also investigated; two and three CO2 molecules are activated, respectively, and the rate constants are slower than that of Nb2BN2/CO2 systems. This comparison indicates that metal–metal multiple bonds and appropriate ligands, such as B, are important factors for CO2 reduction. The synergy between a transition metal atom (Nb) and a main-group atom (B) in CO2 reduction mediated by gas-phase clusters is revealed for the first time. To the best of our knowledge, Nb2BN2 anions are gas-phase clusters that reduce the largest number of CO2 molecules. A fundamental understanding of the efficient reduction of carbon dioxide molecules may shed light on the rational design of active sites on supported transition metal/boron nitride catalysts.

Graphical abstract: Nb2BN2− cluster anions reduce four carbon dioxide molecules: reactivity enhancement by ligands

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Supplementary files

Article information


Submitted
30 Jul 2020
Accepted
02 Sep 2020
First published
03 Sep 2020

Dalton Trans., 2020,49, 14081-14087
Article type
Paper

Nb2BN2 cluster anions reduce four carbon dioxide molecules: reactivity enhancement by ligands

H. Zhou, M. Wang, Y. Ding and J. Ma, Dalton Trans., 2020, 49, 14081
DOI: 10.1039/D0DT02680H

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