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通过富氧空位的CeO /Ni异质结构提高Ni在碱性介质中的氢氧化活性。

Boosting Hydrogen Oxidation Activity of Ni in Alkaline Media through Oxygen-Vacancy-Rich CeO /Ni Heterostructures.

作者信息

Yang Fulin, Bao Xi, Li Peng, Wang Xuewei, Cheng Gongzhen, Chen Shengli, Luo Wei

机构信息

College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, Hubei, 430072, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2019 Oct 1;58(40):14179-14183. doi: 10.1002/anie.201908194. Epub 2019 Aug 21.

Abstract

The search for highly efficient platinum group metal (PGM)-free electrocatalysts for the hydrogen oxidation reaction (HOR) in alkaline electrolytes remains a great challenge in the development of alkaline exchange membrane fuel cells (AEMFCs). Here we report the synthesis of an oxygen-vacancy-rich CeO /Ni heterostructure and its remarkable HOR performance in alkaline media. Experimental results and density functional theory (DFT) calculations indicate the electron transfer between CeO and Ni could lead to thermoneutral adsorption free energies of H* (ΔG ). This, together with the promoted OH* adsorption strength derived from the abundance of oxygen vacancies in the CeO species, contributes to the excellent HOR performance with the exchange current density and mass activity of 0.038 mA cm and 12.28 mA mg , respectively. This presents a new benchmark for PGM-free alkaline HOR and opens a new avenue toward the rational design of high-performance PGM-free electrocatalysts for alkaline HOR.

摘要

在碱性电解质中寻找用于氢氧化反应(HOR)的高效无铂族金属(PGM)电催化剂仍然是碱性交换膜燃料电池(AEMFCs)发展中的一个巨大挑战。在此,我们报告了一种富含氧空位的CeO /Ni异质结构的合成及其在碱性介质中卓越的HOR性能。实验结果和密度泛函理论(DFT)计算表明,CeO和Ni之间的电子转移可导致H的热中性吸附自由能(ΔG )。这与CeO物种中丰富的氧空位所促进的OH吸附强度一起,促成了优异的HOR性能,其交换电流密度和质量活性分别为0.038 mA cm 和12.28 mA mg 。这为无PGM碱性HOR提供了一个新的基准,并为合理设计用于碱性HOR的高性能无PGM电催化剂开辟了一条新途径。

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