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Pt,In and Pd,In catalysts for the hydrogenation of nitrates and nitrites in water. FTIR characterization and reaction studies

机译:用于水中硝酸盐和亚硝酸盐加氢的Pt,In和Pd,In催化剂。 FTIR表征和反应研究

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摘要

Pt,In and Pd,In catalysts supported on alumina or silica are active for the reduction of nitrate to N2 in water, using H2 as reducing agent. The characterization of the catalysts using FTIR of adsorbed CO shows the formation of both linear and bridged CO-Pd and CO-Pt bonds. Besides, carbonate species are formed due to the presence of OH groups provided by the support. The presence of In produces a shift in CO-Pd and CO-Pt bands, suggesting the formation of intermetallic particles. After use in reaction, the amount of CO-Pd and CO-Pt species strongly decreases, the main signals being those associated with carbonate groups. The proportion between bridged and linear species also changes after reaction. These results indicate the agglomeration of metallic particles during reaction, which is in agreement with TEM results. Increasing the In loading from 0.25 to 0.5 wt.% results in a moderate decrease in the nitrate conversion for all of the catalysts, which could be associated with a decrease of isolated Pd sites which are responsible for the dissociation of hydrogen. The experimental evidence for this point is the decrease of bridged CO adsorbed observed via FTIR for the samples with higher In loading and for all the catalysts. TPR experiments show low-temperature reduction peaks due to the presence of oxychloride and hydroxychloride particles in monometallic Pd and Pt catalysts. When In is present, the formation of Pd-In and Pt-In compounds provoke the shift of the reduction peaks and the appearance of new reduction signals.
机译:使用H2作为还原剂,负载在氧化铝或二氧化硅上的Pt,In和Pd,In催化剂可将水中的硝酸盐还原为N2。使用FTIR吸附的催化剂对催化剂进行表征,表明线性和桥接的CO-Pd和CO-Pt键均形成。此外,由于载体提供的OH基的存在,形成了碳酸盐物质。 In的存在会导致CO-Pd和CO-Pt谱带发生偏移,表明形成了金属间颗粒。在反应中使用后,CO-Pd和CO-Pt种类的数量大大减少,主要信号是与碳酸酯基团相关的信号。反应后,桥连和线性物种之间的比例也发生变化。这些结果表明反应期间金属颗粒的团聚,这与TEM结果一致。 In负载量从0.25wt。%增加到0.5wt。%导致所有催化剂的硝酸盐转化率适度降低,这可能与负责氢解离的分离的Pd位点的降低有关。关于这一点的实验证据是对于高In含量的样品和所有催化剂,通过FTIR观察到的桥连式CO吸附减少。 TPR实验显示,由于在单金属Pd和Pt催化剂中存在氯氧化物和羟基氯化物颗粒,因此出现了低温还原峰。当存在In时,Pd-In和Pt-In化合物的形成会引起还原峰的移动和新还原信号的出现。

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