Nanoporous Gold-Supported Ceria for the Water–Gas Shift Reaction: UHV Inspired Design for Applied Catalysis

Nanoporous Gold-Supported Ceria for the Water–Gas Shift Reaction: UHV Inspired Design for Applied Catalysis
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DOI:
10.1021/jp505433a
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发表时间:
2014-07
影响因子:
3.7
通讯作者:
Junjie Shi;A. Schaefer;A. Wichmann;M. Murshed;T. Gesing;Arne Wittstock;M. Bäumer
Junjie Shi;A. Schaefer;A. Wichmann;M. Murshed;T. Gesing;Arne Wittstock;M. Bäumer
中科院分区:
化学3区
文献类型:
--
作者:
Junjie Shi;A. Schaefer;A. Wichmann;M. Murshed;T. Gesing;Arne Wittstock;M. Bäumer

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受超高真空 (UHV) 条件下模型研究的启发,利用纳米多孔金 (npAu) 基底上硝酸铈前体的热分解制备了反整体式金/二氧化铈催化剂。在整个多孔金材料(孔和韧带 30-40 nm)中形成氧化铈沉积物。 npAu盘和涂层制备成负载有约3至10原子%的二氧化铈。在环境压力条件下,在连续流反应器中测试复合材料的水煤气变换 (WGS) 反应 (H2O + CO → H2 + CO2)。在低至 135 °C 的温度下观察到 CO2 的形成,并且在高达 535 °C 的温度下具有出色的稳定性和重现性。该材料热稳定性的显着提高可能与纳米金韧带上金属氧化物沉积物的存在有关。加热至 535 °C 催化转化约 15 小时后,活性损失仅为约 10%。光电发射光谱表明缺陷 (Ce3+) 浓度...
Inspired by model studies under ultrahigh vacuum (UHV) conditions, inverse monolithic gold/ceria catalysts are prepared using thermal decomposition of a cerium nitrate precursor on a nanoporous gold (npAu) substrate. Cerium oxide deposits throughout the porous gold material (pores and ligaments 30–40 nm) are formed. npAu disks and coatings were prepared with loadings of about 3 to 10 atom % of ceria. The composite material was tested for the water–gas shift (WGS) reaction (H2O + CO → H2 + CO2) in a continuous flow reactor at ambient pressure conditions. Formation of CO2 was observed at temperatures as low as 135 °C with excellent stability and reproducibility up to temperatures of 535 °C. The considerably increased thermal stability of the material can be linked to the presence of metal oxide deposits on the nanosized gold ligaments. The loss of activity after about 15 h of catalytic conversion with heating to 535 °C was only about 10%. Photoemission spectroscopy indicates a defect (Ce3+) concentration of...