Electronically tailored metal-ion-chelation strategy promotes ionic liquid catalysis at near-ambient condition

Tianhao Zhang, Yuan Tian, Chong Zhang, Tingting Yan, Hanwen Yan, Guoliang Zhang, Jie Li, Zengxi Li, Gang Wang (), Chunshan Li () and Suojiang Zhang ()
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Tianhao Zhang: Chinese Academy of Sciences
Yuan Tian: Chinese Academy of Sciences
Chong Zhang: Chinese Academy of Sciences
Tingting Yan: Chinese Academy of Sciences
Hanwen Yan: Chinese Academy of Sciences
Guoliang Zhang: Chinese Academy of Sciences
Jie Li: Chinese Academy of Sciences
Zengxi Li: Chinese Academy of Sciences
Gang Wang: Chinese Academy of Sciences
Chunshan Li: Chinese Academy of Sciences
Suojiang Zhang: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Electronic properties of active sites profoundly influence catalytic production of value-added chemicals; however, rational description and modulation is still a significant challenge. Herein, we propose an effective metal-ion-chelation strategy guided by density functional theory prediction and in situ Raman observation to structurally tailor and quantitatively correlate the electronic properties of active sites in ionic liquid. Comprehensive characterizations and theoretical calculations, in combination with electronic properties–performance correlations, reveal the electronic peculiarity of nitrogen and oxygen centers can be controllably restructured for remarkable improvement of catalytic performance at near-ambient condition. The turnover frequency is increased by two folds with deactivation rate suppressed by more than one half, while the kilogram-scaled recycling pilot achieves similar performance for the probe methacrolein synthesis. This strategy further exhibits excellent applicability and tolerance in other substrates with representative functional groups. Our work expresses the significance of electronic properties and provides a valid regulation approach for ionic liquid catalysis.

Date: 2025
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DOI: 10.1038/s41467-025-63630-9

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