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Investigating the Role of Undercoordinated Pt Sites at the Surface of Layered PtTe for Methanol Decomposition

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Journal Nat Commun
Specialty Biology
Date 2024 Jan 22
PMID 38253575
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Abstract

Transition metal dichalcogenides, by virtue of their two-dimensional structures, could provide the largest active surface for reactions with minimal materials consumed, which has long been pursued in the design of ideal catalysts. Nevertheless, their structurally perfect basal planes are typically inert; their surface defects, such as under-coordinated atoms at the surfaces or edges, can instead serve as catalytically active centers. Here we show a reaction probability > 90 % for adsorbed methanol (CHOH) on under-coordinated Pt sites at surface Te vacancies, produced with Ar bombardment, on layered PtTe - approximately 60 % of the methanol decompose to surface intermediates CHO (x = 2, 3) and 35 % to CH (x = 1, 2), and an ultimate production of gaseous molecular hydrogen, methane, water and formaldehyde. The characteristic reactivity is attributed to both the triangular positioning and varied degrees of oxidation of the under-coordinated Pt at Te vacancies.

References
1.
Xie J, Zhang J, Li S, Grote F, Zhang X, Zhang H . Controllable disorder engineering in oxygen-incorporated MoS2 ultrathin nanosheets for efficient hydrogen evolution. J Am Chem Soc. 2013; 135(47):17881-8. DOI: 10.1021/ja408329q. View

2.
Liu Z, Hu P . General rules for predicting where a catalytic reaction should occur on metal surfaces: a density functional theory study of C-H and C-O bond breaking/making on flat, stepped, and kinked metal surfaces. J Am Chem Soc. 2003; 125(7):1958-67. DOI: 10.1021/ja0207551. View

3.
Li X, Fang Y, Wang J, Fang H, Xi S, Zhao X . Ordered clustering of single atomic Te vacancies in atomically thin PtTe promotes hydrogen evolution catalysis. Nat Commun. 2021; 12(1):2351. PMC: 8060321. DOI: 10.1038/s41467-021-22681-4. View

4.
Du H, Huang Y, Wong D, Tseng M, Lee Y, Wang C . Nanoscale redox mapping at the MoS-liquid interface. Nat Commun. 2021; 12(1):1321. PMC: 7910562. DOI: 10.1038/s41467-021-21660-z. View

5.
Kresse , Furthmuller . Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys Rev B Condens Matter. 1996; 54(16):11169-11186. DOI: 10.1103/physrevb.54.11169. View