Electro-conversion of methane to alcohols on “capsule-like” binary metal oxide catalysts
Electro-conversion of methane to alcohols on “capsule-like” binary metal oxide catalysts
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DOI：
10.1016/j.apcatb.2020.119572
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发表时间：
2021-03
影响因子：
22.1
通讯作者：
Nengneng Xu;Cameron A. Coco;Yudong Wang;Tianshun Su;Yu Wang;Luwei Peng;Yanxing Zhang;Yuyu Liu-Yuyu
中科院分区：
文献类型：
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作者：
Nengneng Xu;Cameron A. Coco;Yudong Wang;Tianshun Su;Yu Wang;Luwei Peng;Yanxing Zhang;Yuyu Liu-Yuyu
为了解决甲烷在环境条件下氧化为液体产物的关键催化挑战，对甲烷电转化的研究一直受到推动。在这项工作中，我们采用了一系列具有胶囊状形态的二元金属氧化物催化剂，通过将zro2锚定在氧化铜（CuOx）上来氧化甲烷。ZrO2:CuOx（180,24）转化甲烷的电流密度与ZrO2、CuOx和其他ZrO2:CuOx相比差达13.35 mA cm−2。密度泛函理论计算表明，活性的增强是由于zro2簇在Cu2O上生长后，zro2中的电荷分布增加（111），从而增强了ch4的解离活性，改善了Cu2O支撑下的电子传导。得益于这些优点，混合催化剂表现出较高的催化活性和稳定性。令人惊讶的是，在正常条件下运行18 -h后，主要产物是1-丙醇和2-丙醇。
Research on the electro-conversion of methane has been driven by the necessity of addressing a key catalytic challenge to oxidize methane to liquid products at ambient conditions. In this work, we employed a series of binary metal oxide catalysts with capsule-like morphology by anchoring ZrO2on Cu oxide (CuOx) for the oxidation of methane. The ZrO2:CuOx(180, 24)was found to convert methane with a difference in current density up to 13.35 mA cm−2in comparison with ZrO2, CuOx, and other ZrO2:CuOx. The density functional theory calculations show that the enhanced activity originated from the increased charge distribution in ZrO2after the ZrO2cluster grew on the Cu2O(111), which enhances the activity of CH4dissociation and improves the electronic conduction through Cu2O support. Benefiting from these advantages, the hybrids exhibit a high catalytic activity and stability. Surprisingly, 1-propanol and 2-propanol were the main products after 18 -h operation under ambient conditions.