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首页> 外文期刊>ACS catalysis >Methane Combustion over Pd/Al2O3 Catalysts in the Presence of Water: Effects of Pd Particle Size and Alumina Crystalline Phase
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Methane Combustion over Pd/Al2O3 Catalysts in the Presence of Water: Effects of Pd Particle Size and Alumina Crystalline Phase

机译:在水存在下Pd / Al2O3催化剂的甲烷燃烧:Pd粒径和氧化铝结晶相的影响

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摘要

The effects of the Pd particle size and the Al2O3 crystalline phase of Pd/Al(2)O(3 )catalysts on the CH4 combustion in the presence of H2O were investigated. According to X-ray absorption fine structure (XAFS) measurements, it was revealed that, during the CH4 combustion, the Pd nanoparticles existed on the Al2O3 support as a PdO phase, while the crystallinity of PdO depended on the Pd particle size. On the basis of X-ray diffraction XRD), amorphous PdO particles with a size of <7 nm exhibited low activity for CH4 combustion. In contrast, as the Pd particle size increased, larger crystalline PdO particles (>7 nm) were formed, which were highly active for CH4 combustion. Comparing the effects of the different Al(2)O(3 )crystalline phases, Pd/alpha-Al2O3 was proved to be more resistant to deactivation by H2O than Pd/gamma-Al(2)O(3 )and Pd/theta-Al2O3. Moreover, according to H2O temperature-programmed desorption (TPD) and infrared (IR) measurements, since alpha-Al2O3 was relatively hydrophobic compared to gamma-Al2O3 and theta-Al2O3, a faster and reversible adsorption/desorption of OH/H2O species was achieved, while the H2O poisoning on PdO species in the vicinity was limited.
机译:研究了Pd / Al(2)o(3)催化剂在H2O存在下在CH4燃烧中的Pd / Al(2)O(3)催化剂的效果。根据X射线吸收细结构(XAFS)测量,揭示了在CH4燃烧期间,在Al 2 O 3载体上存在Pd纳米粒子作为PDO相,而PDO的结晶度依赖于Pd粒径。在X射线衍射XRD的基础上,具有尺寸<7nm的无定形PDO颗粒表现出低活性的CH 4燃烧。相反,随着Pd粒径增加,形成较大的结晶PDO颗粒(> 7nm),其对CH 4燃烧非常有效。比较不同Al(2)O(3)结晶相的效果,证明Pd /α-Al 2O3的耐抗性比Pd /γ-Al(2)o(3)和Pd /θ - Al2O3。此外,根据H2O温度编程的解吸(TPD)和红外(IR)测量,由于与γ-Al2O3和θ-Al2O3相比,α-Al2O3相对疏水,因此实现了OH / H2O物种的更快和可逆的吸附/解吸,而H2O中毒在附近的PDO物种是有限的。

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