Demonstrator devices for artificial photosynthesis: general discussion.
Demonstrator devices for artificial photosynthesis: general discussion.
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人工光合作用演示装置：一般讨论。
DOI：
10.1039/c9fd90023c
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发表时间：
2019
影响因子：
3.4
通讯作者：
Abe R
中科院分区：
文献类型：
--
作者：
Abe R
Wilson Smith opened discussion of the paper by Michael Grätzel: For the Cu–Au electrodes, the proposed mechanism is that CO2 is converted to CO on the Au site, then diffuses on the surface to a Cu site where it hydrogenates to form higher order products. Given that the system is highly porous and the local pH may be higher than the bulk solution, can you comment on the likelihood for the proposed mechanism (surface diffusion of CO), or if CO is formed in the gas phase, then re-adsorbs on the Cu surface from the solution? The two pathways have large implications on mechanistic understandings, and different approaches would be needed to optimise these steps in different ways.Michael Grätzel replied: We propose indeed that the CO directly spills over directly from the Au nanoparticles to the Cu support. Nevertheless your point is well taken that the CO adsorption on Au is reversible and hence that there is an equilibrium between the adsorbed and free CO. So the path of CO transfer from Au to Cu via the gas phase is a viable alternative to the direct spillover. It is favored by the fact that desorption of CO can occur from any Au surface site while in order for the spillover to occur the Au site must have adjacent Cu sites. More analysis is required to determine the predominant mechanism.
