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Research Article

Ru complex and N, P-containing polymers confined within mesoporous hollow carbon spheres for hydrogenation of CO2 to formate

Guoxiang Yang1, Yasutaka Kuwahara1,2,3,4, Kohsuke Mori1,2,3, Catherine Louis5, Hiromi Yamashita1,2,3()
Division of Materials and Manufacturing Science, Graduate School of Engineering, Osaka University, 2-1 Yamada-oka, Suita, Osaka 565-0871, Japan
Institute for Open and Transdisciplinary Research Initiatives (OTRI), Osaka University, 2-1 Yamada-oka, Suita, Osaka 565-0871, Japan
Unit of Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, Katsura, Kyoto 615-8520, Japan
JST, PRESTO, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan
Sorbonne Université, CNRS, Laboratoire de Réactivité de Surface, LRS, F-75005 Paris, France
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We found that the encapsulation of an appropriate amount of ruthenium complex and N, P-containing porous organic polymers in mesoporous hollow carbon spheres not only enhances the activity and durability of the catalyst for CO2 hydrogenation to produce formate but also reduces the activation energy of CO2 hydrogenation.

Abstract

The development of reliable catalysts with both excellent activity and recyclability for carbon dioxide (CO2) hydrogenation is challenging. Herein, a ternary hybrid heterogeneous catalyst, involving mononuclear Ru complex, N, P-containing porous organic polymers (POPs), and mesoporous hollow carbon spheres (Ru3+-POPs@MHCS) is reported for CO2 hydrogenation to formate. Based on comprehensive structural analyses, we demonstrated that Ru3+-POPs were successfully immobilized within MHCS. The optimized Ru3+-0.5POPs@MHCS catalyst, which was obtained with about 5 wt.% Ru3+ and 0.5 mmol POPs polymers confined into 0.3 g MHCS, exhibited high catalytic activity for CO2 hydrogenation to formate (turnover number (TON) > 1,200 for 24 h under mild reaction conditions (4.0 MPa, 120 °C)) and improved durability, compared to Ru3+ catalysts without POPs polymers (Ru3+-MHCS) and unencapsulated MHCS (Ru3+-0.5POPs) catalysts. The improved catalytic performance is attributed to the high surface area and large pore volume of MHCS which favors dispersion and stabilization of Ru3+-POPs. Furthermore, the MHCS and POPs showed high CO2 adsorption ability. Ru3+-POPs encapsulated into MHCS reduces the activation energy barrier for CO2 hydrogenation to formate.

Keywords

heterogeneous catalysisporous organic polymers (POPs)mesoporous hollow carbon spheresCO2 hydrogenationformate synthesis

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Nano Research
Volume 16 Issue 4,
April 2023
Pages 4515-4523
DOI: 10.1007/s12274-021-3792-2
Cite this article:
Yang G, Kuwahara Y, Mori K, et al. Ru complex and N, P-containing polymers confined within mesoporous hollow carbon spheres for hydrogenation of CO2 to formate. Nano Research, 2023, 16(4): 4515-4523. https://doi.org/10.1007/s12274-021-3792-2
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