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COMBINATORIAL SYNTHESIS AND REACTIVITY SCREENING OF ELECTRO-OXIDATION CATALYST GRADIENTS

机译:电氧化催化剂梯度的组合合成与反应性筛选

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Combinatorial methods represent an appealing experimental method for the discovery of heterogeneous catalysts. One can efficiently identify candidate materials or sample vast regions of composition space using a combination of dense catalyst libraries and high-throughput reactivity screening techniques. This is particularly appealing for the discovery of novel catalysts for low temperature fuel cells where multi-component systems have shown improved performance. For example, the poison tolerance of typical anode catalysts can be improved by the addition of oxophilic components such as ruthenium, molybdenum, tin or osmium. Consequently, a vast composition space must be sampled in order to identify catalyst compositions or regions of composition space with greater activity. Combinatorial methods represent a practical means to speed-up the catalyst discovery process. In this manuscript, we demonstrate a novel method for combinatorial catalyst discovery based upon the synthesis and reactivity mapping of catalyst composition gradients. Samples consisting of uniform variations in surface composition of metals catalysts (Pt-M| and Pt-M|-M2, where Mi, Mb = Ru, Mo, Sn or Os) are fabricated using a gel-transfer technique. A concentration gradient of source metal ions is produced in a swollen polymer gel and then transferred onto a surface by electrodeposition to create a continuous composition gradient. An in situ reactivity-mapping tool based on the scanning electrochemical microscope is used to interrogate these catalyst gradients for the hydrogen oxidation reaction in the presence of adsorbed carbon monoxide.
机译:组合方法代表了一种发现非均相催化剂的吸引力实验方法。一种可以使用致密催化剂文库和高通量反应性筛选技术的组合有效地识别候选材料或样本的组合空间区域。这对于发现用于低温燃料电池的新型催化剂特别吸引力,其中多组分系统显示出改善的性能。例如,通过添加乳化成分如钌,钼,锡或锇,可以改善典型阳极催化剂的毒耐药性。因此,必须采样巨大的组合空间,以鉴定具有更大活性的组合物空间的催化剂组合物或区域。组合方法代表加速催化剂发现过程的实用手段。在该稿件中,我们证明了基于催化剂组合梯度的合成和反应映射的组合催化剂发现的新方法。由金属催化剂表面组合物的​​均匀变化(Pt-m |和Pt-m | -m2组成的样品,使用凝胶转移技术制造Mi,Mi,Mb = Ru,Mo,Sn或Os的影响。源金属离子的浓度梯度在溶胀的聚合物凝胶中制备,然后通过电沉积转移到表面上以产生连续的组成梯度。基于扫描电化学显微镜的原位反应性 - 映射工具用于在吸附的一氧化碳存在下询问氢氧化反应的这些催化剂梯度。

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