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介孔 AlOOH 负载层状氢氧化物的合成、表征及 CO2 吸附性能。

Synthesis, characterization, and CO(2) adsorptive behavior of mesoporous AlOOH-supported layered hydroxides.

机构信息

Department of Materials Sciences and Engineering, National Chiao Tung University, 1001 Ta Hsueh Road, Hsinchu Taiwan 300, PR China.

出版信息

ChemSusChem. 2012 Jul;5(7):1249-57. doi: 10.1002/cssc.201100617. Epub 2012 Apr 4.

DOI:10.1002/cssc.201100617
PMID:22488944
Abstract

A novel CO(2) solid sorbent was prepared by synthesizing and modifying AlOOH-supported CaAl layered double hydroxides (CaAl LDHs), which were prepared by using mesoporous alumina (γ-Al(2)O(3)) and calcium chloride (CaCl(2)) in a hydrothermal urea reaction. The nanostructured CaAl LDHs with nanosized platelets (3-30 nm) formed and dispersed inside the crystalline framework of mesoporous AlOOH (boehmite). By calcination of AlOOH-supported LDHs at 700 °C, the mesoporous CaAl metal oxides exhibited ordered hexagonal mesoporous arrays or uniform nanotubes with a large surface area of 273 m(2) g(-1) , a narrow pore size distribution of 6.2 nm, and highly crystalline frameworks. The crystal structure of the calcined mesoporous CaAl metal oxides was multiphasic, consisting of CaO/Ca(OH)(2), Al(2)O(3), and CaAlO mixed oxides. The mesoporous metal oxides were used as a solid sorbent for CO(2) adsorption at high temperatures and displayed a maximum CO(2) capture capacity (≈45 wt %) of the sorbent at 650 °C. Furthermore, it was demonstrated that the mesoporous CaAl oxides showed a more rapid adsorption rate (for 1-2 min) and longer cycle life (weight change retention: 80 % for 30 cycles) of the sorbent because of the greater surface area and increased number of activated sites in the mesostructures. A simple model for the formation mechanism of mesoporous metal oxides is tentatively proposed to account for the synergetic effect of CaAl LDHs on the adsorption of CO(2) at high temperature.

摘要

一种新型的 CO2 固体吸附剂是通过合成和修饰负载在 AlOOH 上的 CaAl 层状双氢氧化物(CaAl LDHs)制备的,该吸附剂是通过在水热尿素反应中使用中孔氧化铝(γ-Al2O3)和氯化钙(CaCl2)制备的。纳米结构的 CaAl LDHs 具有纳米尺寸的薄片(3-30nm),在中孔 AlOOH(薄水铝石)的晶体结构内形成并分散。通过在 700°C 下煅烧负载在 AlOOH 上的 LDHs,可以得到具有有序六方介孔排列或均匀纳米管的介孔 CaAl 金属氧化物,其比表面积高达 273 m2 g-1,孔径分布狭窄为 6.2nm,并且具有高度结晶的骨架。煅烧后的介孔 CaAl 金属氧化物的晶体结构为多相,由 CaO/Ca(OH)2、Al2O3 和 CaAlO 混合氧化物组成。介孔金属氧化物被用作高温下 CO2 吸附的固体吸附剂,在 650°C 时表现出最大的 CO2 捕集容量(≈45wt%)。此外,研究表明,由于介孔结构中具有更大的比表面积和更多的活性位,介孔 CaAl 氧化物显示出更快的吸附速率(1-2min)和更长的循环寿命(重量变化保留率:30 次循环中为 80%)。提出了一种介孔金属氧化物形成机制的简单模型,以解释 CaAl LDHs 在高温下吸附 CO2 的协同效应。

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