Dataset Information

In Situ Exfoliation and Pt Deposition of Antimonene for Formic Acid Oxidation via a Predominant Dehydrogenation Pathway.

ABSTRACT: Direct formic acid fuel cell (DFAFC) has been considered as a promising energy conversion device for stationary and mobile applications. Advanced platinum (Pt) electrocatalysts for formic acid oxidation reaction (FAOR) are critical for DFAFC. However, the oxidation of formic acid on Pt catalysts often occurs via a dual pathway mechanism, which hinders the catalytic activity owing to the CO poisoning. Herein, we directly exfoliate bulk antimony to 2D antimonene (Sb) and in situ load Pt nanoparticles onto antimonene sheets with the assistance of ethylenediamine. According to the Bader charge analysis, the charge transfer from antimonene to Pt occurs, confirming the electronic interaction between Pt and Sb. Interestingly, antimonene, as a cocatalyst, alters the oxidation pathway for FAOR over Pt catalyst and makes FAOR follow the more efficient dehydrogenation pathway. The density functional theory (DFT) calculation demonstrates that antimonene can activate Pt to be a lower oxidative state and facilitate the oxidation of HCOOH into CO2 via a direct pathway, resulting in a weakened intermediate binding strength and better CO tolerance for FAOR. The specific activity of FAOR on Pt/Sb is 4.5 times, and the mass activity is 2.6 times higher than the conventional Pt/C.

SUBMITTER: Zhang Y

PROVIDER: S-EPMC7054718 | biostudies-literature | 2020

REPOSITORIES: biostudies-literature

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In Situ Exfoliation and Pt Deposition of Antimonene for Formic Acid Oxidation via a Predominant Dehydrogenation Pathway.

Zhang Yiqiong Y Qiao Man M Huang Yucheng Y Zou Yuqin Y Liu Zhijuan Z Tao Li L Li Yafei Y Dong Chung-Li CL Wang Shuangyin S

Research (Washington, D.C.) 20200221

Direct formic acid fuel cell (DFAFC) has been considered as a promising energy conversion device for stationary and mobile applications. Advanced platinum (Pt) electrocatalysts for formic acid oxidation reaction (FAOR) are critical for DFAFC. However, the oxidation of formic acid on Pt catalysts often occurs via a dual pathway mechanism, which hinders the catalytic activity owing to the CO poisoning. Herein, we directly exfoliate bulk antimony to 2D antimonene (Sb) and <i>in situ</i> load Pt nan ...[more]

PMID: 32266330

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Project description:Formic acid is considered as one of the most promising liquid organic hydrogen carriers. Its catalytic dehydrogenation process generally suffers from low activity, low reaction selectivity, low stability of the catalysts, and/or the use of noble-metal-based catalysts. Herein we report a highly selective, efficient, and noble-metal-free photocatalyst for the dehydrogenation of formic acid. This catalyst, UiO-66(COOH)2-Cu, is built by postmetalation of a carboxylic-functionalized Zr-MOF with copper. The visible-light-driven photocatalytic dehydrogenation process through the release of hydrogen and carbon dioxide has been monitored in real-time via operando Fourier transform infrared spectroscopy, which revealed almost 100% selectivity with high stability (over 3 days) and a conversion yield exceeding 60% (around 5 mmol·gcat-1·h-1) under ambient conditions. These performance indicators make UiO-66(COOH)2-Cu among the top photocatalysts for formic acid dehydrogenation. Interestingly, the as-prepared UiO-66(COOH)2-Cu hetero-nanostructure was found to be moderately active under solar irradiation during an induction phase, whereupon it undergoes an in-situ restructuring process through intraframework cross-linking with the formation of the anhydride analogue structure UiO-66(COO)2-Cu and nanoclustering of highly active and stable copper sites, as evidenced by the operando studies coupled with steady-state isotopic transient kinetic experiments, transmission electron microscopy and X-ray photoelectron spectroscopy analyses, and Density Functional Theory calculations. Beyond revealing outstanding catalytic performance for UiO-66(COO)2-Cu, this work delivers an in-depth understanding of the photocatalytic reaction mechanism, which involves evolutive behavior of the postmetalated copper as well as the MOF framework over the reaction. These key findings pave the way toward the engineering of new and efficient catalysts for photocatalytic dehydrogenation of formic acid.

Dataset Information

In Situ Exfoliation and Pt Deposition of Antimonene for Formic Acid Oxidation via a Predominant Dehydrogenation Pathway.

Publications

In Situ Exfoliation and Pt Deposition of Antimonene for Formic Acid Oxidation via a Predominant Dehydrogenation Pathway.

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