Dang Shanshan, Qin Bin, Yang Yong, Wang Hui, Cai Jun, Han Yong, Li Shenggang, Gao Peng, Sun Yuhan
CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203, P.R. China.
University of Chinese Academy of Sciences, Beijing 100049, P.R. China.
Sci Adv. 2020 Jun 17;6(25):eaaz2060. doi: 10.1126/sciadv.aaz2060. eCollection 2020 Jun.
Renewable energy-driven methanol synthesis from CO and green hydrogen is a viable and key process in both the "methanol economy" and "liquid sunshine" visions. Recently, InO-based catalysts have shown great promise in overcoming the disadvantages of traditional Cu-based catalysts. Here, we report a successful case of theory-guided rational design of a much higher performance InO nanocatalyst. Density functional theory calculations of CO hydrogenation pathways over stable facets of cubic and hexagonal InO predict the hexagonal InO(104) surface to have far superior catalytic performance. This promotes the synthesis and evaluation of InO in pure phases with different morphologies. Confirming our theoretical prediction, a novel hexagonal InO nanomaterial with high proportion of the exposed {104} surface exhibits the highest activity and methanol selectivity with high catalytic stability. The synergy between theory and experiment proves highly effective in the rational design and experimental realization of oxide catalysts for industry-relevant reactions.
由一氧化碳和绿色氢气通过可再生能源驱动合成甲醇，在“甲醇经济”和“液态阳光”设想中都是可行的关键过程。最近，基于氧化铟的催化剂在克服传统铜基催化剂的缺点方面显示出巨大潜力。在此，我们报告一个理论指导合理设计出高性能得多的氧化铟纳米催化剂的成功案例。对立方相和六方相氧化铟稳定晶面的一氧化碳加氢路径进行的密度泛函理论计算预测，六方相氧化铟(104)表面具有远为优异的催化性能。这推动了具有不同形貌的纯相氧化铟的合成与评估。证实了我们的理论预测，一种具有高比例暴露{104}表面的新型六方相氧化铟纳米材料表现出最高活性和甲醇选择性以及高催化稳定性。理论与实验之间的协同作用在合理设计和实验实现用于工业相关反应的氧化物催化剂方面证明非常有效。
