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Enhancing the methane steam reforming catalytic performance of Ni monolithic catalysts via Ni-Resurface alloying

机译:提高甲烷蒸汽转化催化剂倪通过整体式催化剂的性能Ni-Resurface合金化

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摘要

High cell density Ni monolithic catalysts coated with a series of Ni-Re bimetallic surface layers (Re 0-38 at%) were synthesized and examined for application in methane steam reforming (MSR) under a steam-to-carbon ratio of 1.36 and a gas hourly space velocity of 6400 h-1 in the temperature range of 773-1173 K. The influence of mass and heat transport was verified to be minor below 973 K under the present experimental conditions. The catalytic activities of the Ni monolithic catalysts were effectively improved in the presence of a Ni-Re bimetallic surface layer coating, and the stability in terms of the catalyst activity was significantly enhanced below 973 K upon increasing the Re content to >24 at%. The Ni-Re surface layer was analyzed by using in situ X-ray absorption fine structure spectroscopy, synchrotron radiation X-ray diffraction, scanning electron microscopy, and density functional theory calculations. These results revealed that a Ni-Re alloy consisting of a Ni(Re) solid solution phase and a Re phase was formed during hydrogen pre-reduction and the subsequent MSR reaction. The Re atoms in the Ni-Re alloy promoted hydrogen adsorption on the surface, thereby suppressing the oxidation of the surface Ni atoms during MSR, and enhancing the stability of the monolithic catalysts.
机译:高细胞密度倪整体式催化剂涂层一系列的Ni-Re双金属层表面(重新0-38 %)是合成和检查应用于甲烷蒸汽转化(MSR)steam-to-carbon 1.36和气体的比例每小时速度6400 h -空间773 - 1173 K的温度范围内。验证质量和热传输是次要的低于973 K下目前的实验条件。整体式催化剂是有效地改善的存在Ni-Re双金属表层涂料,和稳定的催化剂活性明显增强低于973 K时增加内容> 24在%。使用原位x射线吸收精细结构光谱、同步辐射x光衍射、扫描电镜和密度泛函理论计算。结果显示,Ni-Re合金组成的倪(重新)固溶体阶段和阶段在氢pre-reduction和形成的随后MSR的反应。Ni-Re合金促进氢的吸附的表面,从而抑制氧化表面镍原子在MSR和提高整体式催化剂的稳定性。

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