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Single Si-Doped Graphene as a Catalyst in Oxygen Reduction Reactions: An In Silico Study.
ACS Omega ( IF 3.7 ) Pub Date : 2020-06-19 , DOI: 10.1021/acsomega.0c01303 Anton V Kuzmin 1 , Bagrat A Shainyan 1
ACS Omega ( IF 3.7 ) Pub Date : 2020-06-19 , DOI: 10.1021/acsomega.0c01303 Anton V Kuzmin 1 , Bagrat A Shainyan 1
Affiliation
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Single Si-doped graphene C53H18Si with one carbon atom replaced by a three-coordinate silicon atom is studied by density functional theory (DFT) calculations as a catalyst for the oxygen reduction reactions (ORRs) in both acidic and alkaline media. The active sites for oxygen adsorption were determined from the distribution of the charge density difference analysis. At the equilibrium electrode potential, the most stable intermediate was found to have the structure HO*O*–C53H18Si with both oxygen atoms bound to the support, one of them being incorporated in between Si and C atoms, corresponding to the transfer of one hydrogen atom [H+ + e–]. The 2e ORR mechanism is shown to be very unlikely because the alternative 4e ORR pathway occurring via intermediates with a broken O–O bond is much more exothermic. In addition to the commonly adopted ORR mechanism, new reaction pathways have been discovered and shown to be potentially preferable over the traditional mechanism. The new proposed four-electron ORR route was predicted to proceed spontaneously in acidic media at U < 0.99 V and in alkaline media at U < 0.22.
中文翻译：
单硅掺杂石墨烯作为氧还原反应的催化剂：计算机模拟研究。
通过密度泛函理论（DFT）计算，研究了一个碳原子被三配位硅原子取代的单硅掺杂石墨烯C 53 H 18 Si作为酸性和碱性介质中氧还原反应（ORR）的催化剂。由电荷密度差分析的分布确定氧吸附的活性位点。在平衡电极电势下，发现最稳定的中间体具有结构HO * O * –C 53 H 18 Si，两个氧原子均键合到载体上，其中一个结合在Si和C原子之间，对应于一个氢原子的转移[H + + e –]。事实证明2e ORR机制不太可能，因为通过具有断裂的O–O键的中间体发生的替代4e ORR途径放热得多。除了普遍采用的ORR机制外，还发现了新的反应途径，并且显示出比传统机制更可取的途径。预计新提议的四电子ORR途径将在U <0.99 V的酸性介质中和在U <0.22的碱性介质中自发进行。
更新日期：2020-06-30
中文翻译：
单硅掺杂石墨烯作为氧还原反应的催化剂：计算机模拟研究。
通过密度泛函理论（DFT）计算，研究了一个碳原子被三配位硅原子取代的单硅掺杂石墨烯C 53 H 18 Si作为酸性和碱性介质中氧还原反应（ORR）的催化剂。由电荷密度差分析的分布确定氧吸附的活性位点。在平衡电极电势下，发现最稳定的中间体具有结构HO * O * –C 53 H 18 Si，两个氧原子均键合到载体上，其中一个结合在Si和C原子之间，对应于一个氢原子的转移[H + + e –]。事实证明2e ORR机制不太可能，因为通过具有断裂的O–O键的中间体发生的替代4e ORR途径放热得多。除了普遍采用的ORR机制外，还发现了新的反应途径，并且显示出比传统机制更可取的途径。预计新提议的四电子ORR途径将在U <0.99 V的酸性介质中和在U <0.22的碱性介质中自发进行。
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