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Theoretical insights of Ni2P (0001) surface towards its potential applicability in CO2 conversion via dry reforming of methane

Ramirez Reina, Tomas, Guharoy, Utsab, Olsson, Emilia, Gu, Sai and Cai, Qiong (2019) Theoretical insights of Ni2P (0001) surface towards its potential applicability in CO2 conversion via dry reforming of methane ACS Catalysis, 9 (4). pp. 3487-3497.

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Abstract

This study reports the potential application of Ni2P as highly effective catalyst for chemical CO2 recycling via dry reforming of methane (DRM). Our DFT calculations reveal that the Ni2P (0001) surface is active towards adsorption of the DRM species, with the Ni hollow site being the most energetically stable site and Ni-P and P contributes as co-adsorption sites in DRM reaction steps. Free energy analysis at 1000 K found CH-O to be the main pathway for CO formation. The competition of DRM and reverse water gas shift (RWGS) is also evidenced with the latter becoming important at relatively low reforming temperatures. Very interestingly oxygen seems to play a key role in making this surface resistant towards coking. From microkinetic analysis we have found greater oxygen surface coverage than that of carbon at high temperatures which may help to oxidize carbon deposits in continuous runs. The tolerance of Ni2P towards carbon deposition was further corroborated by DFT and micro kinetic analysis. Along with the higher probability of C oxidation we identify poor capacity of carbon diffusion on the Ni2P (0001) surface with very limited availability of C nucleation sites. Overall, this study opens new avenues for research in metal-phosphide catalysis and expands the application of these materials to CO2 conversion reactions.

Item Type: Article
Divisions : Faculty of Engineering and Physical Sciences > Chemical and Process Engineering
Authors :
NameEmailORCID
Ramirez Reina, Tomast.ramirezreina@surrey.ac.uk
Guharoy, Utsabu.guharoy@surrey.ac.uk
Olsson, Emiliak.olsson@surrey.ac.uk
Gu, Saisai.gu@surrey.ac.uk
Cai, Qiongq.cai@surrey.ac.uk
Date : 12 March 2019
Funders : University of Surrey, Engineering and Physical Sciences Research Council (EPSRC)
DOI : 10.1021/acscatal.8b04423
Copyright Disclaimer : Copyright © 2019, American Chemical Society.
Uncontrolled Keywords : DRM; nickel phosphide (Ni2P); DFT; reaction mechanism; microkinetics; coking stability.
Depositing User : Users 6648 not found.
Date Deposited : 05 Apr 2019 13:46
Last Modified : 13 Mar 2020 02:08
URI: http://epubs.surrey.ac.uk/id/eprint/850981

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