Manohara G V, Norris David, Maroto-Valer M Mercedes, Garcia Susana
Research Centre for Carbon Solutions (RCCS), School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh EH14 4AS, UK.
Dalton Trans. 2021 Jun 1;50(21):7474-7483. doi: 10.1039/d1dt00602a.
Layered double hydroxide (LDH) based mixed metal oxides (MMOs) are promising high temperature CO2 capture sorbents. In order to improve their CO2 capture capacity, it is crucial to bring in changes to their physicochemical properties such as morphology, particle size, surface area and activity by tuning the synthesis method. Here we report a modified amide hydrolysis method to synthesize LDHs with a mixed morphology and better CO2 capture properties. Acetate intercalated Mg-Al LDHs with two different Mg/Al ratios (3 and 4) were synthesized by employing metal hydroxides as the starting precursors and acetamide as the hydrolysing agent. The resultant LDHs crystallized in a new morphology having a combination of both fibrous and sheet like crystallites. The MMOs derived from Mg-Al-acetate LDHs retained the mixed morphology observed in the precursor LDHs. The resultant MMOs showed almost a threefold increase in the BET surface area, 316 (Mg/Al = 3) and 341 (Mg/Al = 4) m2 g-1, compared to MMOs derived from anion exchanged Mg-Al-acetate LDH (118 m2 g-1). The MMOs synthesized by acetamide hydrolysis captured 1.2 mmol g-1 and 0. 87 mmol g-1 of CO2 at 200 and 300 °C (atmospheric pressure), respectively. The CO2 capture capacity realized was increased more than twofold compared to the CO2 capture capacity of MMOs derived from anion exchanged acetate LDH (0.57 mmol g-1) tested under similar conditions. The developed MMOs showed promising CO2 capture (1.0 mmol g-1) capacity at industrially relevant CO2 concentration (14%).
基于层状双氢氧化物(LDH)的混合金属氧化物(MMO)是很有前景的高温二氧化碳捕集吸附剂。为了提高它们的二氧化碳捕集能力,通过调整合成方法来改变其物理化学性质(如形态、粒径、表面积和活性)至关重要。在此,我们报道一种改进的酰胺水解法来合成具有混合形态和更好二氧化碳捕集性能的LDH。以金属氢氧化物为起始前驱体,乙酰胺为水解剂,合成了两种不同镁铝比(3和4)的醋酸根插层的Mg-Al LDH。所得的LDH结晶形成一种新的形态,具有纤维状和片状微晶的组合。由Mg-Al-醋酸盐LDH衍生的MMO保留了前驱体LDH中观察到的混合形态。与由阴离子交换的Mg-Al-醋酸盐LDH衍生的MMO(118 m² g⁻¹)相比,所得的MMO的BET表面积几乎增加了两倍,分别为316(Mg/Al = 3)和341(Mg/Al = 4)m² g⁻¹。通过乙酰胺水解合成的MMO在200和300 °C(大气压)下分别捕获了1.2 mmol g⁻¹和0.87 mmol g⁻¹的二氧化碳。与在类似条件下测试的由阴离子交换醋酸盐LDH衍生的MMO的二氧化碳捕集容量(0.57 mmol g⁻¹)相比,实现的二氧化碳捕集容量增加了两倍多。所开发的MMO在工业相关的二氧化碳浓度(14%)下显示出有前景的二氧化碳捕集容量(1.0 mmol g⁻¹)。