Solution-Phase Synthesis of PdH0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation

Shi, Yifeng; Schimmenti, Roberto; Zhu, Shangqian; Venkatraman, Kartik; Chen, Ruhui; Chi, Miaofang; Shao, Minhua; Mavrikakis, Manos; Xia, Younan

doi:10.1021/jacs.1c10199

Title: Solution-Phase Synthesis of PdH_0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation

Journal Article · 01 February 2022 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.1c10199 · OSTI ID:1876056

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Georgia Institute of Technology, Atlanta, GA (United States); University of Wisconsin−Madison Department of Chemical and Biological Engineering
University of Wisconsin, Madison, WI (United States)
Hong Kong University of Science and Technology (HKUST) (Hong Kong)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Georgia Institute of Technology, Atlanta, GA (United States)
Georgia Institute of Technology, Atlanta, GA (United States); Hong Kong University of Science and Technology (HKUST) (Hong Kong)

We report palladium is one of the few metals capable of forming hydrides, with the catalytic properties being dependent on the elemental composition and spatial distribution of H atoms in the lattice. Herein, we report a facile method for the complete transformation of Pd nanocubes into a stable phase made of PdH_0.706 by treating them with aqueous hydrazine at a concentration as low as 9.2 mM. Using formic acid oxidation (FAO) as a model reaction, we systematically investigated the structure–catalytic property relationship of the resultant nanocubes with different degrees of hydride formation. The current density at 0.4 V was enhanced by four times when the nanocubes were completely converted from Pd to PdH_0.706. On the basis of a set of slab models with PdH(100) overlayers on Pd(100), we conducted density functional theory calculations to demonstrate that the degree of hybrid formation could influence both the activity and selectivity toward FAO by modulating the relative stability of formate (HCOO) and carboxyl (COOH) intermediates. Furthermore, this work provides a viable strategy for augmenting the performance of Pd-based catalysts toward various reactions without altering the loading of this scarce metal.

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Research Organization:: Univ. of Wisconsin, Madison, WI (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation; Georgia Institute of Technology

Grant/Contract Number:: FG02-05ER15731; AC02-05CH11231; AC05-00OR22725

OSTI ID:: 1876056

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 6 Vol. 144; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Anions
Catalysts
Electrodes
Nanocubes
Palladium

Title: Solution-Phase Synthesis of PdH0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation

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Title: Solution-Phase Synthesis of PdH_0.706 Nanocubes with Enhanced Stability and Activity toward Formic Acid Oxidation