2026-08-13 上海交通大学(SJTU)

Figure 1. Opening LDH nanosheets for elevated-temperature CO₂ capture. Aqueous miscible organic solvent treatment separates stacked LDH layers and creates open, flower-like particles. Potassium modification then introduces additional active sites, producing higher CO₂ working capacities than conventional commercial potassium-modified LDHs at 400 °C.
<関連情報>
- https://global.sjtu.edu.cn/en/news-events/news/3379
- https://www.sciencedirect.com/science/article/abs/pii/S1385894724082731
- https://www.sciencedirect.com/science/article/abs/pii/S2095495624003607
層状複水酸化物のその場アミングラフト化によるCO2直接空気捕集用吸着剤性能の向上 Enhancing adsorbent performance for direct air capture of CO2 by in-situ amine-grafting of layered double hydroxides
Bingyao Ge, Chunping Chen, Yifei Xu, Samuel Roberts, Man Zhang, Qingyang Shao, Dermot O’Hare, Xuancan Zhu
Chemical Engineering Journal Available online: 16 October 2024
DOI:https://doi.org/10.1016/j.cej.2024.156782
Highlight
- New in-situ amine grafting method based layered double hydroxide nanosheets for direct air capture.
- Doubles CO2 adsorption capacity compared with traditional two-step grafting method.
- Maintains CO2 capture capacity 0.85 mmol g−1 at 70 °C desorption temperature without moisture.
- NMR confirms amine grafting matches traditional method’s chemical modification.
- In-situ adsorbent enables rapid adsorption and desorption with high stability and low cost in DAC conditions.
Abstract
The development of efficient and cost-effective CO2 adsorbents is crucial for carbon capture from ultradilute conditions. Amine-grafted mesoporous materials prepared by silane chemical reactions are well-known CO2 adsorbents with high thermal stabilities, but their capacities for direct air capture (DAC) are usually restricted by low amine loadings and CO2 capture capacity. Herein, we present an in-situ amine grafting method that enables high amine loadings by in-situ grafting initial ultrathin LDHs nanosheets in an organic solvent. For in-situ triamine grafted Mg2Al-CO3 LDH (IN-TRI-LDH) amine loading is boosted to 5.91mmol N g−1 and ultimately achieving a remarkable adsorption capacity of 0.98 mmol g−1 at 25°C and 400 ppm CO2, nearly double that of the amine-LDHs grafted through a conventional two-step process. A further 22 % enhancement of the CO2 capacity is observed under 20 RH%. In addition, IN-TRI-LDH maintains a working capacity of 0.85 mmol g−1 at a low desorption temperature of 70 °C. A 50 adsorption–desorption cyclic test under simulated humid DAC conditions shows minimal performance degradation. Such a sufficient working capacity and low desorption temperature reduces the thermal energy consumption to 2.27 GJ t−1 at a desorption temperature of 40 °C.
CO2の直接空気捕捉のためのポリエチレンイミン官能化Mg-Al混合金属酸化物モノリスの3Dプリント 3D printing of poly(ethyleneimine)-functionalized Mg-Al mixed metal oxide monoliths for direct air capture of CO2
Qingyang Shao, Zhuozhen Gan, Bingyao Ge, Xuyi Liu, Chunping Chen, Dermot O’Hare, Xuancan Zhu
Journal of Energy Chemistry Available online: 18 May 2024
DOI:https://doi.org/10.1016/j.jechem.2024.05.015
Abstract
Direct air capture (DAC) of CO2 plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies. Since large air flows are required to capture the ultradilute CO2 from the air, lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies. A structured adsorbent is essential for the implementation of gas-solid contactors for cost- and energy-efficient DAC systems. In this study, efficient adsorbent poly(ethyleneimine) (PEI)-functionalized Mg-Al-CO3 layered double hydroxide (LDH)-derived mixed metal oxides (MMOs) are three-dimensional (3D) printed into monoliths for the first time with more than 90% adsorbent loadings. The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths. This structure exhibits a 32.7% higher specific surface area and a 46.1% higher pore volume, as compared to the direct printing of the MMO powder into a monolith. After impregnation of PEI, the monolith demonstrates a large adsorption capacity (1.82 mmol/g) and fast kinetics (0.7 mmol/g/h) using a CO2 feed gas at 400 ppm at 25 °C, one of the highest values among the shaped DAC adsorbents. Smearing of the amino-polymers during the post-printing process affects the diffusion of CO2, resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths. The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.


