Lan, Yang;
Wang, Jingyi;
Li, Xiyi;
Chang, Chia-Hao;
Zhang, Tianyu;
Guan, Xuze;
Liu, Qiong;
... Tang, Junwang; + view all
(2024)
Engineering Single Ni Sites on 3D Cage-like Cucurbit[n]uril Ligands for Efficient and Selective CO2 Photocatalytic Reduction.
Angewandte Chemie International Edition
e202417384.
10.1002/anie.202417384.
(In press).
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Angew Chem Int Ed - 2024 - Lan - Lan_Engineering Single Ni Sites on 3D Cage‐like Cucurbit n uril Ligands for Efficient and.pdf Download (12MB) | Preview |
Abstract
Solar-driven CO2 selective reduction with high conversion is a challenging task yet holds immense promise for both CO2 neutralization and green fuel production. Enhancing CO2 adsorption at the catalytic centre can trigger a highly efficient CO2 capture-to-conversion process. Herein, we introduce cucurbit[n]urils (CB[n]), a new family of molecular ligands, as a key component in the creation of a 3D cage-like metal (nickel, Ni)-complex molecular co-catalyst (CB[7]-Ni) for photocatalysis. It exhibits an unprecedented CO yield rate of 72.1 µmol· h-1 with a high selectivity of 97.9% under visible light irradiation. To verify the origin of the carbon source in the products, a straightforward isotopic tracing method is designed based on tandem reactions. The catalytic process commences with photoelectron transfer from Ru(bpy)32+ to the Ni2+ site, resulting in the reduction of Ni2+ to Ni+. The locally enriched CO2 molecules in the cage ligand CB[7] undergo selective reduction by the Ni+ nearby to form CO product. This work exemplifies the inspiring potential of ligand structure engineering in advancing the development of efficient unanchored molecular co-catalysts.
| Type: | Article |
|---|---|
| Title: | Engineering Single Ni Sites on 3D Cage-like Cucurbit[n]uril Ligands for Efficient and Selective CO2 Photocatalytic Reduction |
| Location: | Germany |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/anie.202417384 |
| Publisher version: | http://dx.doi.org/10.1002/anie.202417384 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | 3D ligand, CO2 reduction, Cucurbit[n]uril, Photocatalysis, molecular co-catalyst |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10199525 |
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