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In situ XANES study of methanol decomposition and partial oxidation to syn-gas over supported Pt catalyst on SrTiO3 nanocubes

机译:SrTiO3纳米立方体上负载Pt催化剂上甲醇分解和部分氧化制合成气的原位XANES研究

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摘要

A catalyst of Pt nanoparticles was prepared by atomic layer deposition on SrTiO3 nanocuboids and tested for methanol decomposition and partial oxidation. The catalyst had uniform nanoparticle size of 1.58 ± 0.37 nm and a Pt (111) surface. In situ X-ray absorption near-edge spectroscopy (XANES) measured in a temperature-programmed reduction showed that the Pt particles were easily reduced. However, the as-received catalyst, a reduced catalyst, and an oxidized catalyst all had catalytic activity, differing slightly in methanol conversion and product selectivity. In situ XANES also revealed that CO adsorbed on the Pt sites was the only observed surface species during both methanol decomposition and partial oxidation. It seemed that the breakage of CH and OH bonds overwhelmingly occurred once methanol was adsorbed, forming H2 and adsorbed CO. The latter was then released from the catalyst surface or was oxidized to CO2 when O2 was present.
机译:通过在SrTiO3纳米立方体上原子层沉积制备了Pt纳米颗粒催化剂,并测试了甲醇的分解和部分氧化。该催化剂具有1.58±0.37nm的均匀纳米颗粒尺寸和Pt(111)表面。以程序升温还原法测得的原位X射线吸收近边缘光谱(XANES)表明,Pt颗粒易于还原。但是,原样的催化剂,还原的催化剂和氧化的催化剂均具有催化活性,甲醇转化率和产物选择性略有不同。原位XANES还显示,在甲醇分解和部分氧化过程中,仅在Pt部位吸附的CO是观察到的唯一表面物种。似乎一旦甲醇被吸附,形成H2和被吸附的CO,就会绝大多数发生CH和OH键的断裂。然后,后者从催化剂表面释放出来,或者当存在O2时被氧化成CO2。

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