Effects of Controlled Crystalline Surface of Hydroxyapatite on Methane Oxidation Reactions

Oh, Su Cheun; Xu, Jiayi; Tran, Dat T.; Liu, Bin; Liu, Dongxia

doi:10.1021/acscatal.7b04011

Title: Effects of Controlled Crystalline Surface of Hydroxyapatite on Methane Oxidation Reactions

Journal Article · 16 April 2018 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.7b04011 · OSTI ID:1543698

^[1]; Xu, Jiayi ^[2]; Tran, Dat T. ^[3];

^[2]; Liu, Dongxia ^[1]

Univ. of Maryland, College Park, MD (United States). Dept. of Chemical and Biomolecular Engineering
Kansas State Univ., Manhattan, KS (United States). Dept. of Chemical Engineering
U.S. Army Research Lab., Adelphi, MD (United States)

Hydroxyapatite (HAP, Ca₁₀(PO₄)₆(OH)₂) has a hexagonal prismatic structure that exposes two crystalline surfaces: prism-faceted a- and basal-faceted c-surfaces. Here, the predominant exposure of c-surface was controlled, and its influences in methane oxidation reactions (combustion and oxidative coupling over HAP and lead-substituted HAP (Pb-HAP), respectively) were studied. The c-surface exposure was realized by crystal orientation in HAP-based catalyst film, which was created by an electrochemical deposition of HAP seeds on a titanium substrate, followed by hydrothermal crystallization and peeling off of the crystalline films from the substrate. In comparison to a-surface that is prevalently exposed in unoriented HAP-based catalysts, the c-surface (i.e., (002) crystalline plane) of HAP-based catalysts exhibited up to 47-fold enhancement in areal rate in both reactions. The distinct catalytic activity between these two crystalline surfaces is attributed to the preferential formation of oxide ions and vacancies on c-surfaces. The oxide ions and vacancies in turns function as actives sites for promoting methane activation and complete oxidation into CO₂. Density functional theory calculations confirmed the close relationship between different catalytic activities in c-surface of oriented and a-surface of unoriented HAP through the tendency of vacancy formation. Without the presence of vacancies, the methyl or methylene group after methane activation forms ethane or ethylene via coupling. The present study explored the effects of HAP crystal orientation in methane oxidation reactions, which revealed distinct catalytic behaviors of crystal surfaces in HAP-based materials.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1543698

Journal Information:: ACS Catalysis, Vol. 8, Issue 5; ISSN 2155-5435

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
chemistry
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