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CO2 reactivity with Mg2NiH4 synthesized by in situ monitoring of mechanical milling.
Phys Chem Chem Phys 2020; 22(4):1944-1952PC

Abstract

CO2 capture and conversion are a key research field for the transition towards an economy only based on renewable energy sources. In this regard, hydride materials are a potential option for CO2 methanation since they can provide hydrogen and act as a catalytic species. In this work, Mg2NiH4 complex hydride is synthesized by in situ monitoring of mechanical milling under a hydrogen atmosphere from a 2MgH2:Ni stoichiometric mixture. Temperature and pressure evolution is monitored, and the material is characterized, during milling in situ, thus providing a good insight into the synthesis process. The cubic polymorph of Mg2NiH4 (S.G. Fm3[combining macron]m) starts to be formed in the early beginning of the mechanical treatment due to the mechanical stress induced by the milling process. Then, after 25 hours of milling, Mg2NiH4 with a monoclinic (S.G. C12/c1) structure appears. The formation of the monoclinic polymorph is most likely related to the stress release that follows the continuous refinement of the material's microstructure. At the end of the milling process, after 60 hours, the as-milled material is composed of 90.8 wt% cubic Mg2NiH4, 5.7 wt% monoclinic Mg2NiH4, and 3.5 wt% remnant Ni. The as-milled Mg2NiH4 shows high reactivity for CO2 conversion into CH4. Under static conditions at 400 °C for 5 hours, the interactions between as-milled Mg2NiH4 and CO2 result in total CO2 consumption and in the formation of the catalytic system Ni-MgNi2-Mg2Ni/MgO. Experimental evidence and thermodynamic equilibrium calculations suggest that the global methanation mechanism takes place through the adsorption of C and the direct solid gasification towards CH4 formation.

Authors+Show Affiliations

Department of Physical Chemistry of Materials, Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET) and Centro Atómico Bariloche, Av. Bustillo km 9500, S.C. de Bariloche, Argentina. julianpuszkiel1979@gmail.com.Department of Physical Chemistry of Materials, Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET) and Centro Atómico Bariloche, Av. Bustillo km 9500, S.C. de Bariloche, Argentina. julianpuszkiel1979@gmail.com and Institute of Materials Research, Materials Technology, Helmholtz-Zentrum Geesthacht GmbH, Max-Planck Strasse 1, D-21502 Geesthacht, Schleswig-Holstein, Germany.Department of Physical Chemistry of Materials, Consejo Nacional de Investigaciones Científicas y Técnicas (CONICET) and Centro Atómico Bariloche, Av. Bustillo km 9500, S.C. de Bariloche, Argentina. julianpuszkiel1979@gmail.com.Institute of Materials Research, Materials Technology, Helmholtz-Zentrum Geesthacht GmbH, Max-Planck Strasse 1, D-21502 Geesthacht, Schleswig-Holstein, Germany.Institute of Materials Research, Materials Technology, Helmholtz-Zentrum Geesthacht GmbH, Max-Planck Strasse 1, D-21502 Geesthacht, Schleswig-Holstein, Germany.Institute of Materials Research, Materials Technology, Helmholtz-Zentrum Geesthacht GmbH, Max-Planck Strasse 1, D-21502 Geesthacht, Schleswig-Holstein, Germany.

Pub Type(s)

Journal Article

Language

eng

PubMed ID

31915760

Citation

Grasso, M L., et al. "CO2 Reactivity With Mg2NiH4 Synthesized By in Situ Monitoring of Mechanical Milling." Physical Chemistry Chemical Physics : PCCP, vol. 22, no. 4, 2020, pp. 1944-1952.
Grasso ML, Puszkiel J, Gennari FC, et al. CO2 reactivity with Mg2NiH4 synthesized by in situ monitoring of mechanical milling. Phys Chem Chem Phys. 2020;22(4):1944-1952.
Grasso, M. L., Puszkiel, J., Gennari, F. C., Santoru, A., Dornheim, M., & Pistidda, C. (2020). CO2 reactivity with Mg2NiH4 synthesized by in situ monitoring of mechanical milling. Physical Chemistry Chemical Physics : PCCP, 22(4), pp. 1944-1952. doi:10.1039/c9cp05697a.
Grasso ML, et al. CO2 Reactivity With Mg2NiH4 Synthesized By in Situ Monitoring of Mechanical Milling. Phys Chem Chem Phys. 2020 Jan 28;22(4):1944-1952. PubMed PMID: 31915760.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - CO2 reactivity with Mg2NiH4 synthesized by in situ monitoring of mechanical milling. AU - Grasso,M L, AU - Puszkiel,J, AU - Gennari,F C, AU - Santoru,A, AU - Dornheim,M, AU - Pistidda,C, Y1 - 2020/01/09/ PY - 2020/1/10/pubmed PY - 2020/1/10/medline PY - 2020/1/10/entrez SP - 1944 EP - 1952 JF - Physical chemistry chemical physics : PCCP JO - Phys Chem Chem Phys VL - 22 IS - 4 N2 - CO2 capture and conversion are a key research field for the transition towards an economy only based on renewable energy sources. In this regard, hydride materials are a potential option for CO2 methanation since they can provide hydrogen and act as a catalytic species. In this work, Mg2NiH4 complex hydride is synthesized by in situ monitoring of mechanical milling under a hydrogen atmosphere from a 2MgH2:Ni stoichiometric mixture. Temperature and pressure evolution is monitored, and the material is characterized, during milling in situ, thus providing a good insight into the synthesis process. The cubic polymorph of Mg2NiH4 (S.G. Fm3[combining macron]m) starts to be formed in the early beginning of the mechanical treatment due to the mechanical stress induced by the milling process. Then, after 25 hours of milling, Mg2NiH4 with a monoclinic (S.G. C12/c1) structure appears. The formation of the monoclinic polymorph is most likely related to the stress release that follows the continuous refinement of the material's microstructure. At the end of the milling process, after 60 hours, the as-milled material is composed of 90.8 wt% cubic Mg2NiH4, 5.7 wt% monoclinic Mg2NiH4, and 3.5 wt% remnant Ni. The as-milled Mg2NiH4 shows high reactivity for CO2 conversion into CH4. Under static conditions at 400 °C for 5 hours, the interactions between as-milled Mg2NiH4 and CO2 result in total CO2 consumption and in the formation of the catalytic system Ni-MgNi2-Mg2Ni/MgO. Experimental evidence and thermodynamic equilibrium calculations suggest that the global methanation mechanism takes place through the adsorption of C and the direct solid gasification towards CH4 formation. SN - 1463-9084 UR - https://www.unboundmedicine.com/medline/citation/31915760/CO2_reactivity_with_Mg2NiH4_synthesized_by_in_situ_monitoring_of_mechanical_milling L2 - https://doi.org/10.1039/c9cp05697a DB - PRIME DP - Unbound Medicine ER -