Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions.
Single rhodium atoms anchored in micropores for efficient transformation of methane under mild conditions.
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DOI：
10.1038/s41467-018-03235-7
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发表时间：
2018-03-26
影响因子：
16.6
通讯作者：
Tao FF
中科院分区：
文献类型：
--
作者：
Tang Y;Li Y;Fung V;Jiang DE;Huang W;Zhang S;Iwasawa Y;Sakata T;Nguyen L;Zhang X;Frenkel AI;Tao FF
在化工原料转向页岩气的情况下，甲烷在温和条件下的催化转化对页岩气的高效利用具有重要意义。在此，我们报道了在≤150°C的溶液中，通过锚定在微孔硅酸铝中的单位点rh105，通过CH4、CO和O2的偶联，CH4转化为乙酸和甲醇。在150℃条件下，这些单分散的贵金属位点在一个rh105位点上的活性可达每秒约0.10个乙酸分子，产生乙酸的选择性约为70%。它比自由Rh阳离子的活度高1000倍。计算研究表明，CH4的第一个C-H键被锚定在ZSM-5微孔壁上的rh105激活；形成的CH3然后与CO和OH结合，在低激活势垒上生成乙酸。甲烷在温和条件下的催化转化对页岩气的利用具有重要意义。本文中，作者报道了CH4、CO和O2在固载于微孔铝硅酸盐中的单位点rh105上偶联转化为乙酸的过程。
Catalytic transformation of CH4 under a mild condition is significant for efficient utilization of shale gas under the circumstance of switching raw materials of chemical industries to shale gas. Here, we report the transformation of CH4 to acetic acid and methanol through coupling of CH4, CO and O2 on single-site Rh1O5 anchored in microporous aluminosilicates in solution at ≤150 °C. The activity of these singly dispersed precious metal sites for production of organic oxygenates can reach about 0.10 acetic acid molecules on a Rh1O5 site per second at 150 °C with a selectivity of ~70% for production of acetic acid. It is higher than the activity of free Rh cations by >1000 times. Computational studies suggest that the first C–H bond of CH4 is activated by Rh1O5 anchored on the wall of micropores of ZSM-5; the formed CH3 then couples with CO and OH, to produce acetic acid over a low activation barrier. Catalytic transformation of CH4 under mild conditions has implications to shale gas utilization. Here, the authors report the transformation of CH4 to acetic acid through coupling of CH4, CO and O2 on single-site Rh1O5 anchored in microporous aluminosilicates in liquid phase.
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影响因子：
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Resasco, DE
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