Development of a Highly Stable Ternary Alloy Catalyst for Dry Reforming of Methane
Development of a Highly Stable Ternary Alloy Catalyst for Dry Reforming of Methane
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DOI：
10.1021/acscatal.2c05488
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发表时间：
2023-02-27
期刊：
影响因子：
12.9
通讯作者：
Furukawa, Shinya
中科院分区：
文献类型：
--
作者：
Liu, Ke;Xing, Feilong;Furukawa, Shinya
甲烷干重整是一种很有前途的化学反应，可以利用二氧化碳和天然气生产高附加值的原料。然而，由于缺乏优秀的耐用和可重复使用的催化剂，该工艺的商业化实施一直停滞不前。在这里，我们报道了一种伪二元合金（Ni0.5Co0.5）3Ge/SiO2，它在不改变母体Ni3Ge相的情况下部分用Co取代Ni。高角环形暗场-扫描透射电子显微镜-能量色散系统、x射线衍射和x射线吸收精细结构分析相结合，发现形成了伪二元合金结构。在700℃甚至低于平衡转化的条件下，将Ni与Co和Ge合金化1000 h（平均催化剂寿命：tau = 1300 h），产生了高的催化活性和显著的热稳定性。详细的表征和理论计算表明，Co掺杂Ni3Ge可以优化C-H活化能力，从而最大限度地减少焦炭的形成，提高稳定性。
Dry reforming of methane is a promising chemical reaction that can utilize CO2 and natural gas to produce value-added feedstocks. However, this process's commercialized implementation has been stalled due to the lack of excellent durable and reusable catalysts. Here, we report a pseudo-binary alloy (Ni0.5Co0.5)3Ge/SiO2, which partially substitutes Ni with Co without altering the parent Ni3Ge phase. The combination of high-angle annular dark-field- scanning transmission electron microscopy-energy-dispersive system, X-ray diffraction, and X-ray absorption fine-structure analysis showed the formation of a pseudo-binary alloy structure. High catalytic activity with remarkable thermal stability is produced by alloying Ni with Co and Ge during continuous operation of 1000 h (mean catalyst life: tau = 1300 h) at 700 degrees C even below the equilibrium conversion. Detailed characterization and theoretical calculations revealed that doping Co to Ni3Ge optimally modified the C-H activation ability, which minimized coke formation for high stability.