Sun, Shuzhuang, Chen, Zheng, Xu, Yikai, Wang, Yuanyuan, Zhang, Yingrui, Dejoie, Catherine, Xu, Shaojun, Xu, Xin and Wu, Chunfei
2024.
Potassium-promoted limestone for preferential direct hydrogenation of carbonates in integrated CO 2 capture and utilization.
JACS Au
4
(1)
, pp. 72-79.
10.1021/jacsau.3c00403
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Abstract
Integrated CO2 capture and utilization (ICCU) via the reverse water–gas shift (RWGS) reaction offers a particularly promising route for converting diluted CO2 into CO using renewable H2. Current ICCU-RWGS processes typically involve a gas–gas catalytic reaction whose efficiency is inherently limited by the Le Chatelier principle and side reactions. Here, we show a highly efficient ICCU process based on gas–solid carbonate hydrogenation using K promoted CaO (K-CaO) as a dual functional sorbent and catalyst. Importantly, this material allows ∼100% CO2 capture efficiency during carbonation and bypasses the thermodynamic limitations of conventional gas-phase catalytic processes in hydrogenation of ICCU, achieving >95% CO2-to-CO conversion with ∼100% selectivity. We showed that the excellent functionalities of the K-CaO materials arose from the formation of K2Ca(CO3)2 bicarbonates with septal K2CO3 and CaCO3 layers, which preferentially undergo a direct gas–solid phase carbonates hydrogenation leading to the formation of CO, K2CO3 CaO and H2O. This work highlights the immediate potential of K-CaO as a class of dual-functional material for highly efficient ICCU and provides a new rationale for designing functional materials that could benefit the real-life application of ICCU processes.
Item Type: | Article |
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Date Type: | Publication |
Status: | Published |
Schools: | Chemistry |
Additional Information: | License information from Publisher: LICENSE 1: URL: https://creativecommons.org/licenses/by/4.0/, Start Date: 2023-11-09 |
Publisher: | American Chemical Society |
ISSN: | 2691-3704 |
Date of Acceptance: | 23 October 2023 |
Last Modified: | 24 Jan 2024 10:00 |
URI: | https://orca.cardiff.ac.uk/id/eprint/165796 |
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