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Spectroscopic Evidences for the Size Dependent Generation of Pd Species Responsible for the Low Temperature CO Oxidation Activity on Pd-SBA-15 Nanocatalyst
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-04-03 , DOI: 10.1016/j.apcatb.2020.118934
Yogita Soni , Sumanta Pradhan , Mahesh K. Bamnia , A.K. Yadav , S.N. Jha , D. Bhattacharyya , Tuhin Suvra Khan , M.A. Haider , C.P. Vinod

A comprehensive size dependent CO oxidation activity has been demonstrated for Pd-SBA-15 catalysts with Pd NPs of varying sizes such as 1-2, 4-6 and 7-10 nm. Pd-SBA-15 catalyst with smallest sized NPs (Pd-S-N) has been synthesized by modified deposition precipitation method recently developed in our lab. Pd-S-N catalyst (reduced at 400 °C) demonstrated CO oxidation activity with lower light off temperature (60 °C), clearly one of the best reported for a Pd-silica system. A detailed XPS and insitu DRIFTS analyses further supported by XAS and DFT calculations reveal the presence of easily decomposable highvalent Pd-oxide on co-ordinatively unsaturated Pd sites (Pdcus). Weak binding of CO on Pdcus sites in small Pd NPs leaving sites for oxygen activation is attributed for the low temperature activity of Pd-S-N for CO oxidation.



中文翻译:

Pd-SBA-15纳米催化剂上负责低温CO氧化活性的Pd物种的尺寸相关生成的光谱证据。

对于具有不同尺寸(例如1-2、4-6和7-10 nm)的Pd NP的Pd-SBA-15催化剂,已证明了其与尺寸有关的全面的CO氧化活性。通过我们实验室最近开发的改进的沉积沉淀法合成了具有最小尺寸NPs的Pd-SBA-15催化剂(Pd-SN)。Pd-SN催化剂(在400°C时还原)具有较低的起燃温度(60°C),具有CO氧化活性,显然是Pd-二氧化硅系统中报道最好的催化剂之一。详细XPS和原位DRIFTS分析由XAS和DFT计算进一步支持揭示易分解highvalent钯氧化物的协同ordinatively不饱和位点的Pd的存在(钯CUS)。在Pd CO的弱结合CUS 小Pd NP中的位点留有氧活化位点,归因于Pd-SN对CO氧化的低温活性。

更新日期:2020-04-20
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