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Four unprecedented V14 clusters as highly efficient heterogeneous catalyst for CO2 fixation with epoxides and oxidation of sulfides.

Authors :
Wang, Ji-Lei
Cao, Jia-Peng
Zhu, Yin-Hua
Wang, Qin
Li, Ning-Fang
Fan, Xin-Rong
Mei, Hua
Xu, Yan
Source :
SCIENCE CHINA Chemistry; Jan2023, Vol. 66 Issue 1, p107-116, 10p
Publication Year :
2023

Abstract

Chemical fixation of carbon dioxide (CO<subscript>2</subscript>) is an energy-saving method for alleviating the greenhouse gas emissions, whereas it persists a challenge posed by the demand for efficient catalysts. Herein, four unprecedented examples of tetradecanuclear vanadium clusters, namely, [(C<subscript>2</subscript>H<subscript>8</subscript>N<subscript>2</subscript>)<subscript>6</subscript>(CH<subscript>3</subscript>O)<subscript>8</subscript>(CH<subscript>3</subscript>OH)<subscript>2</subscript>V<superscript>IV</superscript><subscript>10</subscript>V<superscript>V</superscript><subscript>4</subscript>O<subscript>26</subscript>] (V<subscript>14</subscript>−1), [(C<subscript>3</subscript>H<subscript>10</subscript>N<subscript>2</subscript>)<subscript>6</subscript>(CH<subscript>3</subscript>O)<subscript>8</subscript>(CH<subscript>3</subscript>OH)<subscript>2</subscript>V<superscript>IV</superscript><subscript>10</subscript>V<superscript>V</superscript><subscript>4</subscript>O<subscript>26</subscript>](V<subscript>14</subscript>−2), [(C<subscript>6</subscript>H<subscript>14</subscript>N<subscript>2</subscript>)<subscript>6</subscript>(CH<subscript>3</subscript>O)<subscript>8</subscript>(CH<subscript>3</subscript>OH)<subscript>2</subscript>V<superscript>IV</superscript><subscript>10</subscript>V<superscript>V</superscript><subscript>4</subscript>O<subscript>26</subscript>]·5H<subscript>2</subscript>O (V<subscript>14</subscript>−3) and [(C<subscript>4</subscript>H<subscript>12</subscript>N<subscript>2</subscript>O)<subscript>4</subscript>(C<subscript>4</subscript>H<subscript>11</subscript>N<subscript>2</subscript>O)<subscript>2</subscript>(CH<subscript>3</subscript>O)<subscript>2</subscript>V<superscript>IV</superscript><subscript>10</subscript>V<superscript>V</superscript><subscript>4</subscript>O<subscript>28</subscript>]·6H<subscript>2</subscript>O (V<subscript>14</subscript>−4), have been triumphantly designed and constructed under solvothermal conditions. Among them, compounds V<subscript>14</subscript>−1–4 are the first cases of tetradecanuclear vanadium clusters without the introduction of inorganic acid radical ions. Two main units [V<superscript>IV</superscript><subscript>10</subscript>V<superscript>V</superscript><subscript>4</subscript>O<subscript>26</subscript>]<superscript>8+</superscript> and [V<superscript>IV</superscript><subscript>10</subscript>V<superscript>V</superscript><subscript>4</subscript>O<subscript>28</subscript>]<superscript>4+</superscript> represent brand-new configurations of tetradecanuclear vanadium clusters. Given the fact that the presence of V<superscript>IV</superscript>/V<superscript>V</superscript> can potentially facilitate electron transfer and consequently expedite catalytic reactions, we explored the catalytic activities of these compounds. Remarkably, V<subscript>14</subscript>−1 was further used as a heterogeneous catalyst in the CO<subscript>2</subscript> fixation into cyclic carbonates under milder conditions (60 °C, 0.5 MPa) and exhibited higher catalytic activity. Also, the experimental results indicated that V<subscript>14</subscript>−1 could efficiently catalyze the sulfoxidation, which could fully convert most sulfides within 40 min at room temperature. Moreover, as a stable heterogeneous catalyst employed in CO<subscript>2</subscript> fixation with epoxides and oxidation of sulfides, V<subscript>14</subscript>−1 could be consecutively used multiple cycles without losing its catalytic activity. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
16747291
Volume :
66
Issue :
1
Database :
Complementary Index
Journal :
SCIENCE CHINA Chemistry
Publication Type :
Academic Journal
Accession number :
161192532
Full Text :
https://doi.org/10.1007/s11426-022-1424-9