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IN SITU INFRARED SPECIATION OF ADSORBED CARBONATE ON ALUMINUM AND IRON OXIDES

机译：原位红外吸附碳酸盐对铝和铁氧化物的影响

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Surface adsorption mechanisms of dissolved inorganic carbon species on soil minerals are not well understood. Traditional infrared (IR) study of adsorbed species of inorganic carbon using air-dried samples may not reveal true species in the solid/water interface in suspension. The purpose of this study was to obtain information on interracial carbonate speciation between solid and aqueous phases. The interaction of bicarbonate and carbonate ions with X-ray amorphous (am) A1 and Fe oxides, gibbsite (y-Al(OH)3 ) and goethite ( α-FeOOH) was examined by electrophoresis and in situ attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy. The presence of carbonate lowered the electrophoretic mobility and decreased the point of zero charge (PZC) of all minerals, implying specific adsorption. Inner-sphere complexation of bicarbonate and carbonate was supported by a lowering in the anion symmetry due to the interaction with Al and Fe oxide surfaces. Only complexed monodentate carbonate was identified in am-Al(OH)3/aqueous solution at pH 4.1-7.8 when the solid was reacted with either NaHCO3 or Na2CO3 solutions. Am-Al(OH)3 was transformed to a crystalline sodium aluminum hydroxy carbonate, dawsonite [NaAl(CO3)(OH)2], and bayerite ( α-Al(OH)3) after reacting with 1.0 M Na2CO3 for 24 h. Gibbsite adsorbed much less carbonate than am-AI(OH)3 such that adsorbed carbonate on gibbsite gave weak IR absorption. It is probable that monodentate carbonate is also the complexed species on gibbsite. Evidence suggesting the presence of both surface complexed bicarbonate and carbonate species in the interfacial region of am-Fe(OH)3 in suspension and the dependence of their relative distribution on solution pH is shown. Only monodentate carbonate was found in the interracial region of goethite in 1.0 M NaHCO3. A ligand exchange reaction was proposed to describe the interaction of bicarbonate and carbonate with the surface functional groups of A1 and Fe oxides.
机译：溶解的无机碳物质在土壤矿物质上的表面吸附机理尚不清楚。使用风干样品对无机碳吸附物种进行的传统红外（IR）研究可能无法揭示悬浮液中固体/水界面的真实物种。这项研究的目的是获得有关固相和水相之间的碳酸盐形态的信息。碳酸氢根和碳酸根离子与X射线无定形（am）Al和Fe氧化物，三水铝石（y-Al（OH）3）和针铁矿（α-FeO​​OH）的相互作用通过电泳和衰减全反射傅里叶变换红外光谱进行了研究（ATR-FTIR）光谱。碳酸盐的存在降低了所有矿物的电泳迁移率并降低了零电荷点（PZC），这意味着特定的吸附。由于与Al和Fe氧化物表面的相互作用，降低了阴离子的对称性，从而支持了碳酸氢根和碳酸根的内层络合。当固体与NaHCO3或Na2CO3溶液反应时，仅在pH 4.1-7.8的am-Al（OH）3 /水溶液中鉴定出复合的单齿碳酸盐。与1.0 M Na2CO3反应24小时后，Am-Al（OH）3转化为结晶性羟基铝碳酸钠，片钠铝石[NaAl（CO3）（OH）2]和三钠铝石（α-Al（OH）3）。硅藻土吸附的碳酸盐比am-Al（OH）3少得多，因此吸附在硅藻土上的碳酸盐的IR吸收较弱。单齿碳酸盐也可能是三水铝石上的络合物种。有证据表明在悬浮液中的am-Fe（OH）3的界面区域中同时存在表面络合的碳酸氢盐和碳酸盐物质，并且表明了它们的相对分布对溶液pH的依赖性。在1.0 M NaHCO3中针铁矿的异族区域仅发现单齿碳酸盐。提出了配体交换反应来描述碳酸氢根和碳酸盐与Al和Fe氧化物的表面官能团的相互作用。

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