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Influence of the Oxidizing Species on the Reactivity of Iron-Based Bimetallic Reductants

机译：氧化物种对铁基双金属还原剂反应性的影响

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Anticipating which pollutants are amenable to treatment by iron-based bimetallic reductants requires an understanding of the mechanism(s) driving pollutant reduction. Here, batch studies with six bimetals (Au/Fe, Co/Fe, Cu/Fe, Ni/ Fe, Pd/Fe, and Pt/Fe) and four oxidants (alkyl polyhalides, vinyl polyhalides, alkynes, and water) explored the influence of the electron acceptor on reductant reactivity. Bimetals exhibited disparate reactivity toward some oxidant classes. For example, Pt/Fe enhanced rates of cis-dichloroethylene reduction, but it inhibited the reduction of several alkyl polyhalides. Moreover, the rate increase for vinyl polyhalide reduction by Ni/Fe (～100-fold) and Pd/Fe (～1000-fold) was far greater than that measured for alkyl polyhalides (～10-fold), and reactivity toward vinyl polyhalides exhibited a more pronounced dependence on Ni and Pd loadings than did reactivity toward alkyl polyhalides. These results suggest that the reactions of alkyl and vinyl polyhalides with iron-based bimetals involve different active reductants. Neither rates of alkyl nor vinyl polyhalide reduction correlated with rates of iron corrosion by water, contrary to expectations if galvanic corrosion was primarily responsible for organohalide reduction. Trends observed for the hydrogenation of 2-butyne did mirrorthe sequence we identified for 1,1,1-trichloroethane reduction, consistent with a role for atomic hydrogen as the principal electron donor in these two systems.
机译：预期哪些污染物适合使用铁基双金属还原剂进行处理，需要了解驱动污染物减少的机理。在这里，对六种双金属（Au / Fe，Co / Fe，Cu / Fe，Ni / Fe，Pd / Fe和Pt / Fe）和四种氧化剂（烷基多卤化物，乙烯基多卤化物，炔烃和水）的批量研究探索了电子受体对还原剂反应性的影响。双金属对某些氧化剂表现出完全不同的反应性。例如，Pt / Fe提高了顺式二氯乙烯的还原速率，但它抑制了几种烷基多卤化物的还原。而且，Ni / Fe（〜100倍）和Pd / Fe（〜1000倍）对乙烯基多卤化物的还原速率增加远大于烷基多卤化物（〜10倍）的测定速率，并且对乙烯基多卤化物的反应性与对烷基多卤化物的反应性相比，其对Ni和Pd负载的依赖性更强。这些结果表明烷基和乙烯基多卤化物与铁基双金属的反应涉及不同的活性还原剂。烷基或乙烯基多卤化物的还原速率均与水对铁的腐蚀速率均不相关，这与电偶腐蚀主要是有机卤化物还原的预期相反。观察到的2-丁炔氢化趋势确实反映了我们确定的1,1,1-三氯乙烷还原的顺序，这与原子氢在这两个系统中作为主要电子供体的作用一致。

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