Enhancement of the CO_(2)adsorption and hydrogenation to CH_(4)capacity of Ru–Na–Ca/γ–Al_(2)O_(3)dual function material by controlling the Ru calcination atmosphere  

作　　者：Alejandro Bermejo-López Beñat Pereda-Ayo Jon A.Onrubia-Calvo JoséA.González-Marcos Juan R.González-Velasco 

机构地区：[1]Department of Chemical Engineering,Faculty of Science and Technology,Universidad del País Vasco UPV/EHU,Barrio Sarriena,s/n,48940 Leioa,Bizkaia,Spain

出　　处：《Journal of Environmental Sciences》2024年第6期292-305,共14页环境科学学报（英文版）

基　　金：supported by Ministry of Science and Innovation;National Research Agency(Project PID2019-105960RBC21);by the Basque Government(Project IT1509-2022);One of the authors(JAOC)acknowledges the post-doctoral research grant(DOCREC20/49)provided by the University of the Basque Country。

摘　　要：Integrated CO_(2)capture and utilization(ICCU)technology requires dual functional materials(DFMs)to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8%Na_(2)CO_(3)-8%CaO/γ-Al_(2)O_(3)DFM is studied.The adsorbent precursors are first co-impregnated onto alumina and calcined in air.Then,Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols:static air in muffle or under different mixtures(10%H_(2)/N_(2),50%H_(2)/N_(2)and N_(2))streams.Samples are characterized by XRD,N_(2)adsorption-desorption,H_(2)chemisorption,TEM,XPS,H_(2)-TPD,H_(2)-TPR,CO_(2)-TPD and TPSR.The catalytic behavior is evaluated,in cycles of CO_(2)adsorption and hydrogenation to CH_(4),and temporal evolution of reactants and products concentrations is analyzed.The calcination atmosphere influences the physicochemical properties and,ultimately,activity of DFMs.Characterization data and catalytic performance discover the acccomodation of Ru nanoparticles disposition and basic sites is mostly influencing the catalytic activity.DFM calcined under N_(2)flow(RuNaCa-N_(2))shows the highest CH_(4)production(449μmol/g at 370℃),because a well-controlled decomposition of precursors which favors the better accomodation of adsorbent and Ru phases,maximizing the specific surface area,the Ru-basic sites interface and the participation of different basic sites in the CO_(2)methanation reaction.Thus,the calcination in a N_(2)flow is revealed as the optimal calcination protocol to achieve highly efficient DFM for integrated CO_(2)adsorption and hydrogenation applications.

关 键 词：CO_(2)methanation Integrated CO_(2)capture and utilization(ICCU) Dual functional material(DFM) Ru calcination atmosphere 

分 类 号：X701[环境科学与工程—环境工程] O647.3[理学—物理化学]