Very low Ru loadings boosting performance of Ni-based dual-function materials during the integrated CO_(2)capture and methanation process  

作　　者：Anastasios I.Tsiotsias Eleana Harkou Nikolaos D.Charisiou Victor Sebastian Dhanaji R.Naikwadi Bart van der Linden Atul Bansode Dragos Stoian George Manos Achilleas Constantinou Maria A.Goula 

机构地区：[1]Laboratory of Alternative Fuels and Environmental Catalysis(LAFEC),Department of Chemical Engineering,University of Western Macedonia,Kozani 50100,Greece [2]Department of Chemical Engineering,Cyprus University of Technology,57 Corner of Athinon and Anexartisias,Limassol 3036,Cyprus [3]Department of Chemical Engineering and Environmental Technology,Universidad de Zaragoza,Campus RióEbro-Edificio I+D,Zaragoza 50018,Spain [4]Instituto de Nanociencia y Materiales de Aragón(INMA),Universidad de Zaragoza,CSIC,c/Mariáde Luna 3,Zaragoza 50018,Spain [5]Networking Research Center on Bioengineering,Biomaterials and Nanomedicine,CIBERBBN,28029 Madrid,Spain [6]Department of Chemical Engineering,Delft University of Technology,Van der Massweg 9,Delft 2629 HZ,the Netherlands [7]The Swiss-Norwegian Beamlines(SNBL),European Synchrotron Radiation Facility(ESRF),Grenoble 38000,France [8]Department of Chemical Engineering,University College London,London WCIE7JE,United Kingdom [9]Centre for Research&Technology Hellas(CERTH),Chemical Process and Energy Resources Institute(CPERI),52 Egialias str,Maroussi,Athens 15125,Greece [10]School of Science and Technology,Hellenic Open University,Parodos Aristotelous 18,Patras 26335,Greece

出　　处：《Journal of Energy Chemistry》2025年第3期309-328,共20页能源化学(英文版)

基　　金：support of this work by the project“Development of new innovative low carbon energy technologies to improve excellence in the Region of Western Macedonia”(MIS 5047197),which is implemented under the Action“Reinforcement of the Research and Innovation Infrastructure”funded by the Operational Program“Competitiveness,Entrepreneurship and Innovation”(NSRF 2014-2020);co-financed by Greece and the European Union(European Regional Development Fund);the Hellenic Foundation for Research and Innovation(HFRI)for supporting this research work under the 3~(rd)Call for HFRI PhD Fellowships(Fellowship Number:6033);the support of ELECMI-LMA node;Nanbiosis ICTSs;funded by the Swiss National Science Foundation(Grant:206021_189629);the Research Council of Norway(Grant:296087)。

摘　　要：Herein,the effect of the Ru:Ni bimetallic composition in dual-function materials(DFMs)for the integrated CO_(2)capture and methanation process(ICCU-Methanation)is systematically evaluated and combined with a thorough material characterization,as well as a mechanistic(in-situ diffuse reflectance infrared fourier-transform spectroscopy(in-situ DRIFTS))and computational(computational fluid dynamics(CFD)modelling)investigation,in order to improve the performance of Ni-based DFMs.The bimetallic DFMs are comprised of a main Ni active metallic phase(20 wt%)and are modified with low Ru loadings in the 0.1-1 wt%range(to keep the material cost low),supported on Na_(2)O/Al_(2)O_(3).It is shown that the addition of even a very low Ru loading(0.1-0.2 wt%)can drastically improve the material reducibility,exposing a significantly higher amount of surface-active metallic sites,with Ru being highly dispersed over the support and the Ni phase,while also forming some small Ru particles.This manifests in a significant enhancement in the CH_(4)yield and the CH_(4)production kinetics during ICCU-Methanation(which mainly proceeds via formate intermediates),with 0.2 wt%Ru addition leading to the best results.This bimetallic DFM also shows high stability and a relatively good performance under an oxidizing CO_(2)capture atmosphere.The formation rate of CH_(4)during hydrogenation is then further validated via CFD modelling and the developed model is subsequently applied in the prediction of the effect of other parameters,including the inlet H_(2)concentration,inlet flow rate,dual-fu nction material weight,and reactor internal diameter.

关 键 词：Dual-function materials Integrated CO_(2)capture and methanation Bimetallic materials Nickel-ruthenium Reducibility in-situ DRIFTS CFD modelling 

分 类 号：TQ426[化学工程]