Nano-Intermetallic InNi3C0.5 Compound Discovered as a Superior Catalyst for CO2 Reutilization
Nano-Intermetallic InNi3C0.5 Compound Discovered as a Superior Catalyst for CO2 Reutilization
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纳米金属间化合物 InNi3C0.5 被发现是二氧化碳再利用的优质催化剂
DOI：
10.1016/j.isci.2019.07.006
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发表时间：
2019-07-26
期刊：
影响因子：
5.8
通讯作者：
Lu, Yong
中科院分区：
文献类型：
--
作者：
Chen, Pengjing;Zhao, Guofeng;Lu, Yong
二氧化碳循环经济迫切需要有效的大规模二氧化碳再利用技术。逆水气转换（RWGS）反应是通过下游成熟的费托合成和甲醇合成处理大量二氧化碳的技术上最经济可行的选择，但所需的突破性催化剂代表着一个巨大的挑战。在这里，我们报道了一种纳米金属间InNi3C0.5催化剂的发现，例如，它对RWGS反应具有特别的活性、选择性和稳定性。InNi3C0.5（111）表面主要暴露并具有双活性位点（3Ni-In和3Ni-C），它们协同作用有效地将CO2解离成CO星（3Ni-C上）和o星（3Ni-In上）。o星能很容易地与3ni - c提供的h星反应生成H2O。有趣的是，CO星在400℃及以上主要被解吸，而在300℃以下则选择性地氢化为CH3OH。此外，这种纳米金属间化合物还可以将CO衍生的草酸二甲酯完全氢化为乙二醇（商品化学品），选择性高（96%以上），稳定性好。
CO2 circular economy is urgently calling for the effective large-scale CO2 reutilization technologies. The reverse water-gas shift (RWGS) reaction is the most techno-economically viable candidate for dealing with massive-volume CO2 via downstream mature Fischer-Tropsch and methanol syntheses, but the desired groundbreaking catalyst represents a grand challenge. Here, we report the discovery of a nano-intermetallic InNi3C0.5 catalyst, for example, being particularly active, selective, and stable for the RWGS reaction. The InNi3C0.5(111) surface is dominantly exposed and gifted with dual active sites (3Ni-In and 3Ni-C), which in synergy efficiently dissociate CO2 into CO star (on 3Ni-C) and O-star (on 3Ni-In). O-star can facilely react with 3Ni-C-offered H-star to form H2O. Interestingly, CO star is mainly desorbed at and above 400 degrees C, whereas alternatively hydrogenated to CH3OH highly selectively below 300 degrees C. Moreover, this nano-intermetallic can also fully hydrogenate CO-derived dimethyl oxalate to ethylene glycol (commodity chemical) with high selectivity (above 96%) and favorable stability.