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Synthesis, Characterization, and High-Temperature HCl Capture Capacity of Different Proportions of Potassium Fluoride-Doped CaMgAl Layered Double Hydroxides.

ABSTRACT: In this work, potassium fluoride-doped Ca-Mg-Al layered double hydroxides (CaMgAl-LDHs) were synthesized by a coprecipitation method, after which they were further used as strong adsorbents for HCl gas adsorption in a quartz reactor at high temperature. The physiochemical properties of the as-prepared KF/CaMgAl-LDHs and CaMgAl-LDHs were investigated by X-ray diffraction, thermogravimetric, scanning electron microscopy, energy-dispersive system, and Brunauer-Emmett-Teller. The HCl adsorption test showed that 25 wt % KF loading of the KF/CaMgAl-LDOs was the optimal adsorbent for HCl removal. The highest adsorption capacity of the KF/CaMgAl-LDH adsorbent was achieved with 0.2968 g at 600 °C, 500 ppm HCl concentration, and 0.5 g adsorbent. Furthermore, the microstructure of the adsorbents after the reaction revealed that the adsorbents were encapsulated by dense chloride. The adsorption process was mainly dominated by chemical adsorption, strong acid-base properties, specific surface area, and mesopore number.

SUBMITTER: Wu W

PROVIDER: S-EPMC6844095 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Layered double hydroxides (LDHs) are an ideal platform to host catalytic metal centers for water oxidation (WO) owing to the high accessibility of water to the interlayer region, which makes all centers potentially reachable and activated. Herein, we report the syntheses of three iridium-doped zinc-aluminum LDHs (Ir-LDHs) nanomaterials (1-3, with about 80 nm of planar size and a thickness of 8 nm as derived by field emission scanning electron microscopy and powder X-ray diffraction studies, respectively), carried out in the confined aqueous environment of reverse micelles, through a very simple and versatile procedure. These materials exhibit excellent catalytic performances in WO driven by NaIO4 at neutral pH and 25 °C, with an iridium content as low as 0.5 mol % (∼0.8 wt %), leading to quantitative oxygen yields (based on utilized NaIO4, turnover number up to ∼10,000). Nanomaterials 1-3 display the highest ever reported turnover frequency values (up to 402 min-1) for any heterogeneous and heterogenized catalyst, comparable only to those of the most efficient molecular iridium catalysts, tested under similar reaction conditions. The boost in activity can be traced to the increased surface area and pore volume (>5 times and 1 order of magnitude, respectively, higher than those of micrometric materials of size 0.3-1 μm) estimated for the nanosized particles, which guarantee higher noble metal accessibility. X-ray absorption spectroscopy (XAS) studies suggest that 1-3 nanomaterials, as-prepared and after catalysis, contain a mixture of isolated, single octahedral Ir(III) sites, with no evidence of Ir-Ir scattering from second-nearest neighbors, excluding the presence of IrO2 nanoparticles. The combination of the results obtained from XAS, elemental analysis, and ionic chromatography strongly suggests that iridium is embedded in the brucite-like structure of LDHs, having four hydroxyls and two chlorides as first neighbors. These results demonstrate that nanometric LDHs can be successfully exploited to engineer efficient WOCs, minimizing the amount of iridium used, consistent with the principle of the noble-metal atom economy.

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Synthesis, Characterization, and High-Temperature HCl Capture Capacity of Different Proportions of Potassium Fluoride-Doped CaMgAl Layered Double Hydroxides.

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