Tuning the interaction between Na and Co2C to promote selective CO2 hydrogenation to ethanol
Tuning the interaction between Na and Co2C to promote selective CO2 hydrogenation to ethanol
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调节Na和Co2C之间的相互作用以促进CO2选择性加氢生成乙醇
DOI：
10.1016/j.apcatb.2021.120207
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发表时间：
2021-04
期刊：
影响因子：
--
通讯作者：
Sun Yuhan
中科院分区：
文献类型：
--
作者：
Zhang Shunan;Wu Zhaoxuan;Liu Xiaofang;Shao Zilong;Xia Lin;Zhong Liangshu;Wang Hui;Sun Yuhan
CO2直接加氢制乙醇是实现“碳中和”的最有前途的替代方案之一。然而，稳定催化剂结构和调节CO活化仍然具有挑战性。在此，我们通过调节Na和Co物种之间的相互作用获得了稳定的Nasingle键Co 2C活性位点。Na与Co 2C通过形成Nasingle键和Co键的相互作用，促进了Co 2C的分散和粒径的减小，显著提高了RWGS反应速率和乙醇时空产率（STY）。原位吸附实验和密度泛函理论（DFT）计算表明，随着相互作用的增强，CO2和CO的吸附量增加，同时抑制了CO在Nasingle键Co 2C（111）表面的解离活化，从而调节表面CO/CHx比，促进后续CO偶联合成乙醇.过量的相互作用削弱了CO的吸附强度，导致CO选择性升高。在2wt%的Na时获得了中等的相互作用，乙醇STY高达1.1 mmol g−1h-1（C2+OH/ROH分数为91.3%），比没有Na时高10倍。这项工作为调整反应过程和设计稳定高效的催化剂提供了一种可行的策略。
Direct CO2hydrogenation to ethanol is one of the promising alternatives to realize “carbon-neutral” protocol. However, stabilizing catalyst structure and modulating CO activation remain challenging. Herein, we obtained stable Nasingle bondCo2C active sites by tuning the interaction between Na and Co species. Enhancing the interaction of Na with Co2C through forming Nasingle bondCo bond induced the dispersion of Co2C and the reduction of particle size, evidently improving RWGS reaction rate and ethanol space time yield (STY). In situ adsorption experiments and density functional theory (DFT) calculations demonstrated that the amount of CO2and CO adsorption was increased with the increase of the interaction, while CO dissociative activation on Nasingle bondCo2C (111) surface was inhibited, thereby regulating the surface CO/CHxratio and facilitating subsequent CO coupling to synthesize ethanol. Excessive interaction weakened the strength of CO adsorption resulting in higher CO selectivity. The moderate interaction was obtained at 2 wt% Na and the ethanol STY reached as high as 1.1 mmol g−1h-1(C2+OH/ROH fraction of 91.3 %), which is 10 times higher than that without Na. This work brings an enabling strategy to tune reaction processes and design stable and efficient catalysts.
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DOI：
--
发表时间：
2006
期刊：
--
影响因子：
--
作者：
A. Farrell;R. Plevin;B. Turner;Andrew D. Jones;Michael O’Hare;D. Kammen
通讯作者：
A. Farrell;R. Plevin;B. Turner;Andrew D. Jones;Michael O’Hare;D. Kammen
影响因子：
16.5
作者：
Yan Pei;Yunjie Ding;Juan Zang;Xiangen Song;Wenda Dong;Hejun Zhu;Tao Wang;Weimiao Chen
通讯作者：
Yan Pei;Yunjie Ding;Juan Zang;Xiangen Song;Wenda Dong;Hejun Zhu;Tao Wang;Weimiao Chen
影响因子：
3.7
作者：
Kresse, G;Furthmuller, J
通讯作者：
Furthmuller, J
影响因子：
5.5
作者：
K. Bando;K. Soga;K. Kunimori;H. Arakawa
通讯作者：
K. Bando;K. Soga;K. Kunimori;H. Arakawa
通过钴金属/碳化物界面的费托反应合成高级醇
影响因子：
12.9
作者：
Pei, Yan-Peng;Liu, Jin-Xun;Li, Wei-Xue
通讯作者：
Li, Wei-Xue