Department of Plant and Soil Science and Delaware Environmental Institute, University of Delaware, 152 Townsend Hall, Newark, Delaware 19716. , USA.
Environ Sci Technol. 2010 Jan 1;44(1):143-9. doi: 10.1021/es901759w.
The initial kinetics of Cr(III) oxidation on mineral surfaces is poorly understood, yet a significant portion of the oxidation process occurs during the first seconds of reaction. In this study, the initial rates of Cr(III) oxidation on hydrous manganese oxide (HMO) were measured at three different pH values (pH 2.5, 3, and 3.5), using a quick X-ray absorption fine structure spectroscopy (Q-XAFS) batch method. The calculated rate constants were 0.201, 0.242, and 0.322 s(-1) at pH 2.5, 3, and 3.5, respectively. These values were independent of both [Cr(III)] and [Mn(II)] and mixing speed, suggesting that the reaction was "chemically" controlled and not dependent upon diffusion at the time period the rate parameters were measured. A second-order overall rate was found at three pH values. This represents the first study to determine the chemical kinetics of Cr(III) oxidation on Mn-oxides. The results have important implications for the determination of rapid, environmentally important reactions that cannot be measured with traditional batch and flow techniques. An understanding of these reactions is critical to predicting the fate of contaminants in aquatic and terrestrial environments.
矿物表面上 Cr(III)氧化的初始动力学过程还不太清楚,但氧化过程的很大一部分发生在反应的最初几秒钟内。在这项研究中,使用快速 X 射线吸收精细结构光谱(Q-XAFS)批处理方法,在三个不同的 pH 值(pH 2.5、3 和 3.5)下测量了水合氧化锰(HMO)上 Cr(III)氧化的初始速率。计算得到的速率常数分别为 pH 2.5、3 和 3.5 时的 0.201、0.242 和 0.322 s(-1)。这些值与[Cr(III)]和[Mn(II)]以及混合速度无关,表明在测量速率参数的时间段内,反应是“化学”控制的,而不是依赖于扩散。在三个 pH 值下发现了一个二级总速率。这是首次研究确定 Mn-氧化物上 Cr(III)氧化的化学动力学。研究结果对确定无法用传统批处理和流动技术测量的快速、环境重要的反应具有重要意义。了解这些反应对于预测水相和非水相环境中污染物的命运至关重要。