Methanol synthesis from CO2 and H2 using supported Pd alloy catalysts.
Methanol synthesis from CO2 and H2 using supported Pd alloy catalysts.
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使用负载型 Pd 合金催化剂从 CO2 和 H2 合成甲醇。
DOI：
10.1039/d2fd00119e
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发表时间：
2023
影响因子：
3.4
通讯作者：
Lawes N
中科院分区：
文献类型：
--
作者：
Lawes N
许多钯基材料已被合成并评估为二氧化碳和氢气转化为甲醇的催化剂，甲醇是一种有用的平台化学品和储氢分子。单金属 Pd 催化剂的甲醇选择性较差，但通过 Pd 合金的形成可以改善这种选择性，与单金属 Pd/Al2O3 和 Pd/TiO2 催化剂相比，PdZn 和 PdGa 合金都显示出大大提高的甲醇生产率。催化剂表征表明，1 : 1 β-PdZn 合金存在于所有含 Zn 的反应后样品中，包括 PdZn/Ga2O3，其中 Pd/Ga2O3 样品形成 Pd2Ga 合金。计算了各种合金成分的混合热，其中 PdZn 和 Pd2Ga 合金的高值确定为 ca。每个原子−0.6 eV，约每个原子分别为-0.8 eV。然而，ZnO 比 Ga2O3 更容易被还原，这为当 Ga2O3 存在时优先形成 PdZn 合金而不是 PdGa 提供了可能的解释。
A number of Pd based materials have been synthesised and evaluated as catalysts for the conversion of carbon dioxide and hydrogen to methanol, a useful platform chemical and hydrogen storage molecule. Monometallic Pd catalysts show poor methanol selectivity, but this is improved through the formation of Pd alloys, with both PdZn and PdGa alloys showing greatly enhanced methanol productivity compared with monometallic Pd/Al2O3 and Pd/TiO2 catalysts. Catalyst characterisation shows that the 1 : 1 β-PdZn alloy is present in all Zn containing post-reaction samples, including PdZn/Ga2O3, with the Pd2Ga alloy formed for the Pd/Ga2O3 sample. The heat of mixing was calculated for a variety of alloy compositions with high values determined for both PdZn and Pd2Ga alloys, at ca. −0.6 eV per atom and ca. −0.8 eV per atom, respectively. However, ZnO is more readily reduced than Ga2O3, providing a possible explanation for the preferential formation of the PdZn alloy, rather than PdGa, when in the presence of Ga2O3.