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Encapsulated Heterogeneous Rhodium Single-Atom Catalysts for Linear Selective Hydroformylation of 1-Octene.

Muhammad Kamran¹, Salman Qadir¹, Cuizhen Bai¹

¹Center for Carbon-Neutrality Catalysis and Engineering, Institute of Carbon-Neutral Technology and Shenzhen Public Service Platform for Carbon Capture, Utilization and Storage Technology, Shenzhen Polytechnic University, Shenzhen, 518055, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)

|October 16, 2025

Summary

Highly stable, encapsulated rhodium single-atom catalysts (SACs) show excellent linear selectivity in the hydroformylation of higher olefins. These advanced catalysts achieve high conversions and turnover numbers for 1-octene hydroformylation.

Keywords:

1‐octene hydroformylation MFI‐zeolite linear aldehyde one‐pot synthesis single‐atom catalyst

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Area of Science:

Catalysis
Materials Science
Organic Chemistry

Background:

Single-atom catalysts (SACs) offer unique advantages in catalysis due to their maximum atom utilization.
Hydroformylation of higher olefins, particularly for linear products, remains a significant challenge in industrial chemistry.
Heterogeneous SACs are underexplored for selective hydroformylation reactions.

Purpose of the Study:

To develop and investigate encapsulated heterogeneous rhodium single-atom catalysts (SACs) for linear selective hydroformylation of higher olefins.
To evaluate the activity, stability, and selectivity of these novel SACs.
To compare the performance of SACs with sub-nanoparticle catalysts.

Main Methods:

Synthesis of encapsulated rhodium SACs within MFI zeolite channels.
In situ activation and hydroformylation reactions using 1-octene as a model substrate.
Spectroscopy characterizations (e.g., EXAFS, XANES) to confirm atomic dispersion and encapsulation.
Performance evaluation including conversion, linear-to-branched ratio (l/b), turnover numbers (TONs), and turnover frequency (TOF).

Main Results:

Practical-to-synthesize, highly stable, and highly active encapsulated rhodium SACs (0.07 wt% Rh₁@MFI-K) were successfully prepared.
The catalyst achieved >99% conversion of 1-octene with an exceptional linear selectivity (l/b >99).
The optimized SAC (0.07 wt% Rh₁@MFI-K-0.8) exhibited >1073 TONs and TOF >89 h^-1, outperforming sub-nanoparticle catalysts by fourfold TONs and 28.5 times linear selectivity.
Spectroscopic data confirmed the atomic encapsulation of rhodium within MFI zeolite channels.

Conclusions:

Encapsulated heterogeneous rhodium SACs are highly effective for linear selective hydroformylation of higher olefins.
The atomic dispersion and encapsulation within zeolite channels are crucial for achieving high activity and selectivity.
This work presents a promising pathway for developing advanced catalysts for selective olefin functionalization.