Mechanochemistry of lithium nitride under hydrogen gas

Literature Information

Publication Date 2015-07-28
DOI 10.1039/C5CP02812D
Impact Factor 3.676
Authors

J. Zhang, S. Wang, L. Jiang, M. Latroche, J. Du, F. Cuevas


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Abstract

Hydrogen uptake during the mechanochemistry of lithium nitride under 9 MPa hydrogen pressure has been analyzed by means of in situ solid–gas absorption and ex situ X-ray diffraction (XRD) measurements. In situ hydrogenation curves show two H-sorption steps leading to an overall hydrogen uptake of 9.8 wt% H after 3 hours of milling. The milled end-products consist of nanocrystalline (∼10 nm) LiNH2 and LiH phases. The first reaction step comprises the transformation of the polymorph α-Li3N (S.G. P6/mmm) into the β-Li3N (S.G. P63/mmc) metastable phase and the reaction of the latter with hydrogen to form lithium imide: β-Li3N + H2 → Li2NH + LiH. Reaction kinetics of the first step is zero-order. Its rate-limiting control is assigned to the collision frequency between milling balls and Li3N powder. In the second absorption step, lithium imide converts to lithium amide following the reaction scheme Li2NH + H2 → LiNH2 + LiH. Reaction kinetics is here limited by one-dimensional nucleation and the growth mechanism, which, in light of structural data, is assigned to the occurrence of lithium vacancies in the imide compound. This study provides new insights into the reaction paths and chemical kinetics of light hydrogen storage materials during their mechanochemical synthesis.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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