de Falco Giacomo, Florent Marc, Jagiello Jacek, Cheng Yongqiang, Daemen Luke L, Ramirez-Cuesta Anibal J, Bandosz Teresa J
Department of Chemistry and Biochemistry, The City College of New York, New York, NY 10031, USA.
Micromeritics Instrument Corporation, Norcross, GA 30093, USA.
iScience. 2021 Feb 23;24(3):102216. doi: 10.1016/j.isci.2021.102216. eCollection 2021 Mar 19.
Electrochemical oxygen reduction reaction (ORR) is an important energy-related process requiring alternative catalysts to expensive platinum-based ones. Although recently some advancements in carbon catalysts have been reported, there is still a lack of understanding which surface features might enhance their efficiency for ORR. Through a detailed study of oxygen adsorption on carbon molecular sieves and using inelastic neutron scattering, we demonstrated here that the extent of oxygen adsorption/interactions with surface is an important parameter affecting ORR. It was found that both the strength of O physical adsorption in small pores and its specific interactions with surface ether functionalities in the proximity of pores positively influence the ORR efficiency. We have shown that ultramicropores and hydrophobic surface rich in ether-based groups and/or electrons enhance ORR on carbon electrocatalysts and the performance parameters are similar to those measured on Pt/C with the number of electron transfer equal to 4.
电化学氧还原反应（ORR）是一个与能源相关的重要过程，需要替代昂贵的铂基催化剂。尽管最近有报道称碳催化剂取得了一些进展，但对于哪些表面特征可能提高其ORR效率仍缺乏了解。通过对氧在碳分子筛上的吸附进行详细研究并使用非弹性中子散射，我们在此证明了氧吸附/与表面相互作用的程度是影响ORR的一个重要参数。研究发现，小孔中O物理吸附的强度及其与孔附近表面醚官能团的特定相互作用均对ORR效率产生积极影响。我们已经表明，富含醚基基团和/或电子的超微孔和疏水表面可增强碳电催化剂上的ORR，其性能参数与在电子转移数等于4的Pt/C上测得的参数相似。
