论文标题
了解机械菌株对过渡金属催化活性的影响
Understanding the effect of mechanical strains on the catalytic activity of transition metals
论文作者
论文摘要
分析了13个晚期过渡金属：八（111）个FCC金属（Ni，Cu，Cu，cu，pd，pt，ag，pt，pt，pt，au，rh，rh，rh，ir）和hc esals and zn（co），弹性菌株对氢进化反应（HE）和氧还原反应（ORR）的催化活性的影响：八（111）个FCC金属（Ni，Cu，Cu，pd，pd，ag，ag，pt，pt，au，rh，ir，ir）和五个（0001）表面（0001）和kn kncp gem and zn（co），先前通过密度函数理论计算获得了机械稳定性限制指示的不同中间反应的相应吸附能。发现弹性菌株可通过减少速率限制步骤的能屏障甚至到达火山图的尖端来调整不同金属的催化活性。在PT，AU和IR中发现了与HER菌株一起催化活性的最大变化，而CO和Ni对此策略非常不敏感。在ORR的情况下，通过应用拉伸菌株的应用可以增强AU的催化活性，而Cu，Ni，Pt，Pd，Pd，Rh，Co，Ru和OS的催化活性通过应用压缩菌株的应用改善。然而，IR的催化活性对机械变形不敏感。弹性菌株能够修改AU，PT，AG和OS中的速率限制反应，并且可以在这些金属中实现火山图的尖端。最终的机械不稳定性是在Zn和CD中的小菌株中达到的，这并没有导致她和ORR的催化活性发生显着变化。这些结果提供了一个框架，可以系统地研究弹性菌株在新催化剂设计中的应用。
The effect of elastic strains on the catalytic activity for the hydrogen evolution reaction (HER) and the oxygen reduction reaction (ORR) was analyzed on thirteen late transition metals: eight (111) surfaces of fcc metals (Ni, Cu, Pd, Ag, Pt, Au, Rh, Ir) and five (0001) surfaces of hcp metals (Co, Zn, Cd, Ru, and Os). The corresponding adsorption energies for the different intermediate reactions up to strains dictated by the mechanical stability limits were previously obtained by means of density functional theory calculations. It was found that the elastic strains can be used to tune the catalytic activity of different metals by reducing the energy barrier of the rate limiting step and even to reach the cusp of the volcano plot. The largest changes in catalytic activity with strain for the HER were found in Pt, Au, and Ir while Co and Ni were very insensitive to this strategy. In the case of the ORR, the catalytic activity of Au could be enhanced by the application of tensile strains while that of Cu, Ni, Pt, Pd, Rh, Co, Ru, and Os was improved by the application of compressive strains. However, the catalytic activity of Ir was rather insensitive to mechanical deformations. Elastic strains were able to modify the rate limiting reaction in Au, Pt, Ag, and Os and it was possible to achieve the cusp of the volcano plot in these metals. Final, mechanical instabilities were attained at small strains in Zn and Cd, which did not lead to significant changes in the catalytic activity for HER and ORR. These results provide a framework to systematically investigate the application of elastic strains in the design of new catalysts.
