Implementing vanadium peroxides as direct air carbon capture materials

被引:4
|
作者
Ribo, Eduard Garrido [1 ]
Mao, Zhiwei [1 ]
Hirschi, Jacob S. [1 ]
Linsday, Taylor [1 ]
Bach, Karlie [1 ]
Walter, Eric D. [2 ]
Simons, Casey R. [3 ]
Zuehlsdorff, Tim J. [1 ]
Nyman, May [1 ]
机构
[1] Oregon State Univ, Dept Chem, Corvallis, OR 97331 USA
[2] Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA
[3] Univ Oregon, CAMCOR, Eugene, OR 97331 USA
关键词
CRYSTAL-STRUCTURE; VIBRATIONAL-SPECTRA; CO2; CAPTURE; POTASSIUM; PEROXOVANADATE; EPOXIDATION; SUPEROXIDE; COMPLEXES; OXIDATION; CLIMATE;
D O I
10.1039/d3sc05381d
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Direct air capture (DAC) removal of anthropogenic CO2 from the atmosphere is imperative to slow the catastrophic effects of global climate change. Numerous materials are being investigated, including various alkaline inorganic metal oxides that form carbonates via DAC. Here we explore metastable early d(0) transition metal peroxide molecules that undergo stabilization via multiple routes, including DAC. Specifically here, we describe via experiment and computation the mechanistic conversion of A(3)V(O-2)(4) (tetraperoxovanadate, A = K, Rb, Cs) to first a monocarbonate VO(O-2)(2)(CO3)(3-), and ultimately HKCO3 plus KVO4. Single crystal X-ray structures of rubidium and cesium tetraperoxovanadate are reported here for the first time, likely prior-challenged by instability. Infrared spectroscopy (FTIR), powder X-ray diffraction (PXRD), V-51 solid state NMR (nuclear magnetic resonance), tandem thermogravimetry-mass spectrometry (TGA-MS) along with calculations (DFT, density functional theory) all converge on mechanisms of CO2 capture and release that involve the vanadium centre, despite the end product of a 300 days study being bicarbonate and metavanadate. Electron Paramagnetic Resonance (EPR) Spectroscopy along with a wet chemical assay and computational studies evidence the presense of similar to 5% adventitous superoxide, likely formed by peroxide reduction of vanadium, which also stabilizes via the reaction with CO2. The alkalis have a profound effect on the stability of the peroxovanadate compounds, stability trending K > Rb > Cs. While this translates to more rapid CO2 capture with heavier alkalis, it does not necessarily lead to capture of more CO2. All compounds capture approximately two equivalents CO2 per vanadium centre. We cannot yet explain the reactivity trend of the alkali peroxovanadates, because any change in speciation of the alkalis from reactions to product is not quantifiable. This study sets the stage for understanding and implementing transition metal peroxide species, including peroxide-functionalized metal oxides, for DAC.
引用
收藏
页码:1700 / 1713
页数:14
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