Light-driven Orderly Assembly of Ir-atomic Chains to Integrate a Dynamic Reaction Pathway for Acidic Oxygen Evolution

Zuozheng Xu; Liqi Zhou; Gang Zhou; Shuyi Wu; Peifang Wang; Hao Li; Peilin Huang; Lizhe Liu

doi:10.1002/anie.202301128

Light-driven Orderly Assembly of Ir-atomic Chains to Integrate a Dynamic Reaction Pathway for Acidic Oxygen Evolution

Angew Chem Int Ed Engl. 2023 May 15;62(21):e202301128. doi: 10.1002/anie.202301128. Epub 2023 Apr 14.

Authors

Zuozheng Xu^{1

2}, Liqi Zhou³, Gang Zhou¹, Shuyi Wu⁴, Peifang Wang¹, Hao Li¹, Peilin Huang¹, Lizhe Liu²

Affiliations

¹ Key Laboratory of Integrated Regulation and Resource Development on Shallow Lake of Ministry of Education, College of Environment, Hohai University, Nanjing, 210093, P. R. China.
² Jiangsu Key Laboratory for Nanotechnology and Collaborative Innovation Center of Advanced Microstructures, National Laboratory of Solid State Microstructures, Nanjing University, Nanjing, 210093, P. R. China.
³ College of Engineering and Applied Sciences and Collaborative Innovation Center of Advanced Microstructures, National Laboratory of Solid State Microstructures, Nanjing University, Nanjing, 210023, P. R. China.
⁴ Jiangsu Key Laboratory of Micro and Nano Heat Fluid Flow Technology and Energy Application, School of Physical Science and Technology, Suzhou University of Science and Technology, Suzhou, 215009, P. R. China.

PMID: 36941208
DOI: 10.1002/anie.202301128

Abstract

This work suggests an intriguing light-driven atomic assembly proposal to orderly configure the distribution of reactive sites to optimize the spin-entropy-related orbital interaction and charge transfer from electrocatalysts to intermediates. Herein, the introduced fluorine (F) atoms acting as photo-corrosion centres in MnO_1.9 F_0.1 effectively soften the bonding interaction of Mn-O bonds in the IrCl₃ solution. Therefore, partial Mn atoms can be successively replaced to form orderly atomic-hybridized catalysts with a spin-related low entropy due to the coexistence of Ir-atomic chains and clusters. The time-related elemental analysis demonstrates that the dynamic dissolution/redeposition of Ir clusters in acidic oxygen evolution leads to a reintegration of the reaction pathway to seek the switchable rate-limiting step with a lower activation energy.

Keywords: Acidic Oxygen Evolution; Cation Exchange; Dynamic Orbital Interaction; Light Driven; Spin-Related Entropy.

Abstract

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