首页|Tuning the surface electronic structure of noble metal aerogels to promote the electrocatalytic oxygen reduction

Tuning the surface electronic structure of noble metal aerogels to promote the electrocatalytic oxygen reduction

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The sluggish kinetics of the oxygen reduction reaction(ORR)is the bottleneck for various electrochemical energy conversion devices.Regulating the electronic structure of electrocatalysts by ligands has received particular attention in deriving valid ORR electrocatalysts.Here,the surface electronic structure of Pt-based noble metal aerogels(NMAs)was modulated by various organic ligands,among which the electron-withdrawing ligand of 4-methylphenylene effectively boosted the ORR electrocatalysis.Theoretical calculations suggested the smaller energy barrier for the transformation of O* to OH* and downshift the d-band center of Pt due to the interaction between 4-methylphenylene and the surface metals,thus enhancing the ORR intrinsic activity.Both Pt3Ni and PtPd aerogels with 4-methylphenylene decoration performed significant enhancement in ORR activity and durability in different media.Remarkably,the 4-methylphenylene modified PtPd aerogel exhibited the higher half-wave potential of 0.952 V and the mass activity of 10.2 times of commercial Pt/C.This work explained the effect of electronic structure on ORR electrocatalytic properties and would promote functionalized NMAs as efficient ORR electrocatalysts.

Noble metal aerogelsSurface electronic structureORRElectrocatalystOrganic ligands

Hongxing Yuan、Wei Gao、Xinhao Wan、Jianqi Ye、Dan Wen

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State Key Laboratory of Solidification Processing,School of Materials Science and Engineering,Northwestern Polytechnical University,Xi'an 710072,Shaanxi,China

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaChina Postdoctoral Science FoundationResearch Fund of the State Key Laboratory of Solidification Processing(NPU),ChinaKey Project of Natural Science Fund of Shaanxi Province

22374119219021282021M6926202021-QZ-012023-JC-ZD-06

2024

10.1016/j.jechem.2023.11.006

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.89(2)
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