{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2025,11,2]],"date-time":"2025-11-02T04:36:53Z","timestamp":1762058213701,"version":"build-2065373602"},"reference-count":50,"publisher":"MDPI AG","issue":"7","license":[{"start":{"date-parts":[[2022,7,2]],"date-time":"2022-07-02T00:00:00Z","timestamp":1656720000000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100001871","name":"FCT (Funda\u00e7\u00e3o para a Ci\u00eancia e a Tecnologia)","doi-asserted-by":"publisher","award":["PTDC\/QUI-ELT\/3681\/2020","POCI-01-0247-FEDER-039926","POCI-01-0145-FEDER-032241","UIDB\/00481\/2020","UIDP\/00481\/2020","CEECIND\/04158\/2017","CEECIND\/01117\/2020","CENTRO-01-0145-FEDER-022083"],"award-info":[{"award-number":["PTDC\/QUI-ELT\/3681\/2020","POCI-01-0247-FEDER-039926","POCI-01-0145-FEDER-032241","UIDB\/00481\/2020","UIDP\/00481\/2020","CEECIND\/04158\/2017","CEECIND\/01117\/2020","CENTRO-01-0145-FEDER-022083"]}],"id":[{"id":"10.13039\/501100001871","id-type":"DOI","asserted-by":"publisher"}]},{"name":"Centro Portugal Regional Operational Programme (Centro2020)","award":["PTDC\/QUI-ELT\/3681\/2020","POCI-01-0247-FEDER-039926","POCI-01-0145-FEDER-032241","UIDB\/00481\/2020","UIDP\/00481\/2020","CEECIND\/04158\/2017","CEECIND\/01117\/2020","CENTRO-01-0145-FEDER-022083"],"award-info":[{"award-number":["PTDC\/QUI-ELT\/3681\/2020","POCI-01-0247-FEDER-039926","POCI-01-0145-FEDER-032241","UIDB\/00481\/2020","UIDP\/00481\/2020","CEECIND\/04158\/2017","CEECIND\/01117\/2020","CENTRO-01-0145-FEDER-022083"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Catalysts"],"abstract":"<jats:p>The current study highlights important information regarding how graphene oxide (GO) additive interacts with magnesium hydride (MgH2) and transforms to reduced graphene oxide (rGO). A mild reduction occurs during mechanical milling itself, whereas a strong reduction of GO happens concurrently with the oxidation of Mg formed during the dehydrogenation of MgH2. Owing to the in situ transformation of GO to rGO, the dehydrogenation temperature of MgH2 reduces by about 60 \u00b0C, whereas the hydrogen ab\/desorption reaction kinetics of MgH2 increases by two orders of magnitude and the dehydrogenation activation energy decreases by about 20 kJ\/mol. We have thoroughly scrutinized the transformation of GO to rGO by differential scanning calorimetry (DSC), X-ray diffraction (XRD), Raman spectroscopy, Fourier transform infrared (FTIR) spectroscopy and atomic force microscopy (AFM) techniques. Interestingly, the GO to rGO transformation triggered by magnesium hydride in the current study further paves the way for the facile preparation of rGO- and MgO-decked rGO composites, which are important materials for energy storage applications.<\/jats:p>","DOI":"10.3390\/catal12070735","type":"journal-article","created":{"date-parts":[[2022,7,2]],"date-time":"2022-07-02T11:12:35Z","timestamp":1656760355000},"page":"735","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Elucidating Evidence for the In Situ Reduction of Graphene Oxide by Magnesium Hydride and the Consequence of Reduction on Hydrogen Storage"],"prefix":"10.3390","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2626-2055","authenticated-orcid":false,"given":"D","family":"Pukazhselvan","sequence":"first","affiliation":[{"name":"Nanoengineering Research Group, Centre for Mechanical Technology and Automation (TEMA), Department of Mechanical Engineering, University of Aveiro, 3810-193 Aveiro, Portugal"}]},{"given":"Aliaksandr L.","family":"Shaula","sequence":"additional","affiliation":[{"name":"Nanoengineering Research Group, Centre for Mechanical Technology and Automation (TEMA), Department of Mechanical Engineering, University of Aveiro, 3810-193 Aveiro, Portugal"}]},{"given":"Sergey M.","family":"Mikhalev","sequence":"additional","affiliation":[{"name":"Nanoengineering Research Group, Centre for Mechanical Technology and Automation (TEMA), Department of Mechanical Engineering, University of Aveiro, 3810-193 Aveiro, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6318-1425","authenticated-orcid":false,"given":"Igor","family":"Bdikin","sequence":"additional","affiliation":[{"name":"Nanoengineering Research Group, Centre for Mechanical Technology and Automation (TEMA), Department of Mechanical Engineering, University of Aveiro, 3810-193 Aveiro, Portugal"}]},{"given":"Duncan P.","family":"Fagg","sequence":"additional","affiliation":[{"name":"Nanoengineering Research Group, Centre for Mechanical Technology and Automation (TEMA), Department of Mechanical Engineering, University of Aveiro, 3810-193 Aveiro, Portugal"}]}],"member":"1968","published-online":{"date-parts":[[2022,7,2]]},"reference":[{"key":"ref_1","unstructured":"U.S. DRIVE Partnership (2022, June 05). Target Explanation Document: Onboard Hydrogen Storage for Light-Duty Fuel Cell Vehicles, Available online: https:\/\/www.energy.gov\/sites\/prod\/files\/2017\/05\/f34\/fcto_targets_onboard_hydro_storage_explanation.pdf."},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"566","DOI":"10.1016\/j.nanoen.2012.05.004","article-title":"High capacity hydrogen storage: Basic aspects, new developments and milestones","volume":"1","author":"Pukazhselvan","year":"2012","journal-title":"Nano Energy"},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"237","DOI":"10.1016\/S0925-8388(00)01284-6","article-title":"Metal oxides as catalysts for improved hydrogen sorption in nanocrystalline Mg-based materials","volume":"315","author":"Oelerich","year":"2001","journal-title":"J. Alloys Compd."},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"7188","DOI":"10.1021\/jp044576c","article-title":"Catalytic effect of nanoparticle 3d-transition metals on hydrogen storage properties in magnesium hydride MgH2 prepared by mechanical milling","volume":"109","author":"Hanada","year":"2005","journal-title":"J. Phys. Chem. B"},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"1195","DOI":"10.1002\/cphc.202000031","article-title":"Transformation of metallic Ti to TiH2 phase in the Ti\/MgH2 composite and its influence on the hydrogen storage behavior of MgH2","volume":"21","author":"Pukazhselvan","year":"2020","journal-title":"ChemPhysChem"},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"2677","DOI":"10.1016\/j.ijhydene.2015.12.077","article-title":"Formation of Mg-Nb-O rock salt structures in a series of mechanochemically activated MgH2 + nNb2O5 (n = 0.083\u20131.50) mixtures","volume":"41","author":"Pukazhselvan","year":"2016","journal-title":"Int. J. Hydrogen Energy"},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"174","DOI":"10.1016\/j.jpowsour.2017.07.032","article-title":"Evolution of reduced Ti containing phase(s) in MgH2\/TiO2 system and its effect on the hydrogen storage behavior of MgH2","volume":"362","author":"Pukazhselvan","year":"2017","journal-title":"J. Power Sources"},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"12973","DOI":"10.1021\/jp402770p","article-title":"Effect of Ti intermetallic catalysts on hydrogen storage properties of magnesium hydride","volume":"117","author":"Zhou","year":"2013","journal-title":"J. Phys. Chem. C"},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"381","DOI":"10.1016\/j.jallcom.2017.01.224","article-title":"Core-Shell Ni3N@nitrogen-doped carbon: Synthesis and application in MgH2","volume":"703","author":"Zhang","year":"2017","journal-title":"J. Alloys Compd."},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"177","DOI":"10.1016\/j.energy.2014.11.001","article-title":"Effect of LaCl3 addition on the hydrogen storage properties of MgH2","volume":"79","author":"Ismail","year":"2015","journal-title":"Energy"},{"key":"ref_11","doi-asserted-by":"crossref","first-page":"S392","DOI":"10.1016\/j.jallcom.2014.12.102","article-title":"Enhanced hydrogen desorption property of MgH2 with the addition of cerium fluorides","volume":"645","author":"Lin","year":"2015","journal-title":"J. Alloys Compd."},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"130101","DOI":"10.1016\/j.cej.2021.130101","article-title":"Achieving superior hydrogen storage properties of MgH2 by the effect of TiFe and carbon nanotubes","volume":"422","author":"Lu","year":"2021","journal-title":"Chem. Eng. J."},{"key":"ref_13","doi-asserted-by":"crossref","first-page":"957","DOI":"10.1016\/j.energy.2015.06.037","article-title":"Influences and mechanisms of graphene-doping on dehydrogenation properties of MgH2: Experimental and first-principles studies","volume":"89","author":"Zhang","year":"2015","journal-title":"Energy"},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"126","DOI":"10.1016\/j.carbon.2007.10.033","article-title":"Effects of different carbon materials on MgH2 decomposition","volume":"46","author":"Guo","year":"2008","journal-title":"Carbon"},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"278","DOI":"10.1016\/j.jallcom.2005.10.028","article-title":"Hydrogen storage properties of MgH2\/SWNT composite prepared by ball milling","volume":"420","author":"Wu","year":"2006","journal-title":"J. Alloys Compd."},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"16622","DOI":"10.1016\/j.ijhydene.2020.04.104","article-title":"Synergistic effect of RGO supported Ni3Fe on hydrogen storage performance of MgH2","volume":"45","author":"Liu","year":"2020","journal-title":"Int. J. Hydrogen Energy"},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"768","DOI":"10.1016\/j.jallcom.2019.03.149","article-title":"Effect of RGO Supported NiCu derived from layered double hydroxide on hydrogen sorption kinetics of MgH2","volume":"789","author":"Liu","year":"2019","journal-title":"J. Alloys Compd."},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"160644","DOI":"10.1016\/j.jallcom.2021.160644","article-title":"Enhanced catalytic effect of TiO2@RGO synthesized by one-pot ethylene glycol-assisted solvothermal method for MgH2","volume":"881","author":"Liu","year":"2021","journal-title":"J. Alloys Compd."},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"7440","DOI":"10.1016\/j.ijhydene.2018.02.195","article-title":"Improved reversible dehydrogenation properties of MgH2 by the synergetic effects of graphene oxide-based porous carbon and TiCl3","volume":"43","author":"Wang","year":"2018","journal-title":"Int. J. Hydrogen Energy"},{"key":"ref_20","doi-asserted-by":"crossref","first-page":"165153","DOI":"10.1016\/j.jallcom.2022.165153","article-title":"Achieve high-efficiency hydrogen storage of MgH2 catalyzed by nanosheets CoMoO4 and RGO","volume":"911","author":"Zhang","year":"2022","journal-title":"J. Alloys Compd."},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"4146","DOI":"10.1039\/D0DT00230E","article-title":"The remarkably improved hydrogen storage performance of MgH2 by the synergetic effect of an FeNi\/RGO nanocomposite","volume":"49","author":"Ji","year":"2020","journal-title":"Dalton Trans."},{"key":"ref_22","doi-asserted-by":"crossref","first-page":"461","DOI":"10.1016\/j.jma.2019.06.006","article-title":"Catalytic effect of Ni@RGO on the hydrogen storage properties of MgH2","volume":"8","author":"Yao","year":"2020","journal-title":"J. Magnes. Alloy."},{"key":"ref_23","doi-asserted-by":"crossref","unstructured":"Rajendran, S., Naushad, M., Raju, K., and Boukherroub, R. (2019). Metal oxide additives incorporated hydrogen storage systems: Formation of in situ catalysts and mechanistic understanding. Emerging Nanostructured Materials for Energy and Environmental Science, Springer International Publishing.","DOI":"10.1007\/978-3-030-04474-9"},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"11709","DOI":"10.1016\/j.ijhydene.2016.04.029","article-title":"Crystal structure, phase stoichiometry and chemical environment of MgxNbyOx+y nanoparticles and their impact on hydrogen storage in MgH2","volume":"41","author":"Pukazhselvan","year":"2016","journal-title":"Int. J. Hydrogen Energy"},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"740","DOI":"10.1016\/j.apsusc.2017.05.182","article-title":"Role of chemical interaction between MgH2 and TiO2 additive on the hydrogen storage behavior of MgH2","volume":"420","author":"Pukazhselvan","year":"2017","journal-title":"Appl. Surf. Sci."},{"key":"ref_26","doi-asserted-by":"crossref","first-page":"786","DOI":"10.1016\/j.jma.2021.09.015","article-title":"Active catalytic species generated in situ in zirconia incorporated hydrogen storage material magnesium hydride","volume":"10","author":"Pukazhselvan","year":"2022","journal-title":"J. Magnes. Alloy."},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"21760","DOI":"10.1016\/j.ijhydene.2022.04.290","article-title":"Interaction of zirconia with magnesium hydride and its Influence on the hydrogen storage behavior of magnesium hydride","volume":"47","author":"Pukazhselvan","year":"2022","journal-title":"Int. J. Hydrogen Energy"},{"key":"ref_28","doi-asserted-by":"crossref","first-page":"150062","DOI":"10.1016\/j.apsusc.2021.150062","article-title":"Chemical transformation of additive phase in MgH2\/CeO2 hydrogen storage system and its effect on catalytic performance","volume":"561","author":"Pukazhselvan","year":"2021","journal-title":"Appl. Surf. Sci."},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"3019","DOI":"10.1016\/j.carbon.2011.02.071","article-title":"Hydrazine-reduction of graphite and graphene oxide","volume":"49","author":"Park","year":"2011","journal-title":"Carbon"},{"key":"ref_30","doi-asserted-by":"crossref","first-page":"3195","DOI":"10.1016\/j.apt.2017.09.032","article-title":"Influence of the reduction strategy in the synthesis of reduced graphene oxide","volume":"28","author":"Valverde","year":"2017","journal-title":"Adv. Powder Technol."},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"3738","DOI":"10.1007\/s10853-020-05461-1","article-title":"Chemical and structural properties of reduced graphene oxide\u2014Dependence on the reducing agent","volume":"56","author":"Lesiak","year":"2021","journal-title":"J. Mater. Sci."},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"9562","DOI":"10.1039\/C7NR02943H","article-title":"Experimental review: Chemical reduction of graphene oxide (GO) to reduced graphene oxide (RGO) by aqueous chemistry","volume":"9","author":"Guex","year":"2017","journal-title":"Nanoscale"},{"key":"ref_33","doi-asserted-by":"crossref","first-page":"1015","DOI":"10.1016\/j.apsusc.2014.09.029","article-title":"Effect of pH on the synthesis and characteristics of RGO-CdS nanocomposites","volume":"317","author":"Johra","year":"2014","journal-title":"Appl. Surf. Sci."},{"key":"ref_34","doi-asserted-by":"crossref","first-page":"2740","DOI":"10.1021\/cm060258+","article-title":"Evolution of surface functional groups in a series of progressively oxidized graphite oxides","volume":"18","author":"Szabo","year":"2006","journal-title":"Chem. Mater."},{"key":"ref_35","doi-asserted-by":"crossref","first-page":"1911","DOI":"10.1016\/j.apsusc.2015.09.128","article-title":"Hydrothermally reduced graphene oxide as a supercapacitor","volume":"357","author":"Johra","year":"2015","journal-title":"Appl. Surf. Sci."},{"key":"ref_36","doi-asserted-by":"crossref","first-page":"178","DOI":"10.1002\/cphc.201500620","article-title":"Formation of MgxNbyOx+y through the mechanochemical reaction of MgH2 and Nb2O5, and its effect on the hydrogen-storage behavior of MgH2","volume":"17","author":"Pukazhselvan","year":"2016","journal-title":"ChemPhysChem"},{"key":"ref_37","unstructured":"Nyquist, R.A., and Kagel, R.O. (2012). Handbook of Infrared and Raman Spectra of Inorganic Compounds and Organic Salts: Infrared Spectra of Inorganic Compounds, Academic Press."},{"key":"ref_38","doi-asserted-by":"crossref","first-page":"3906","DOI":"10.1002\/adma.201001068","article-title":"Graphene and graphene oxide: Synthesis, properties, and applications","volume":"22","author":"Yanwu","year":"2010","journal-title":"Adv. Mater."},{"key":"ref_39","doi-asserted-by":"crossref","first-page":"70012","DOI":"10.1039\/C6RA16400E","article-title":"Thermal reduction to control the spacing in graphene oxide membranes: Effect on ion diffusion and electrical conduction","volume":"6","author":"Alhadhrami","year":"2016","journal-title":"RSC Adv."},{"key":"ref_40","doi-asserted-by":"crossref","first-page":"1118","DOI":"10.1016\/j.materresbull.2005.11.011","article-title":"Using MgO to improve the (de)hydriding properties of magnesium","volume":"41","author":"Klassen","year":"2006","journal-title":"Mater. Res. Bull."},{"key":"ref_41","doi-asserted-by":"crossref","first-page":"330","DOI":"10.3390\/catal2030330","article-title":"Superior MgH2 kinetics with MgO addition: A tribological effect","volume":"2","year":"2012","journal-title":"Catalysts"},{"key":"ref_42","doi-asserted-by":"crossref","first-page":"1198","DOI":"10.1039\/C9TC04916A","article-title":"Reduced graphene oxide today","volume":"8","author":"Tarcan","year":"2020","journal-title":"J. Mater. Chem. C"},{"key":"ref_43","doi-asserted-by":"crossref","first-page":"5642","DOI":"10.1002\/celc.201901517","article-title":"Self-supporting electrode composed of SnSe nanosheets, thermally treated protein, and reduced graphene oxide with enhanced pseudocapacitance for advanced sodium-ion batteries","volume":"6","author":"Peng","year":"2019","journal-title":"ChemElectroChem"},{"key":"ref_44","doi-asserted-by":"crossref","first-page":"135196","DOI":"10.1016\/j.electacta.2019.135196","article-title":"Novel hierarchical sea urchin-like prussian blue@palladium core-shell heterostructures supported on nitrogen-doped reduced graphene oxide: Facile synthesis and excellent guanine sensing performance","volume":"330","author":"Li","year":"2020","journal-title":"Electrochim. Acta"},{"key":"ref_45","doi-asserted-by":"crossref","first-page":"7821","DOI":"10.1039\/D2RA00611A","article-title":"Multi-mode surface plasmon resonance absorber based on dart-type single-layer graphene","volume":"12","author":"Chen","year":"2022","journal-title":"RSC Adv."},{"key":"ref_46","doi-asserted-by":"crossref","first-page":"529","DOI":"10.1016\/j.snb.2018.01.068","article-title":"Facile synthesis of Ag@Cu2O heterogeneous nanocrystals decorated N-doped reduced graphene oxide with enhanced electrocatalytic activity for ultrasensitive detection of H2O2","volume":"260","author":"Li","year":"2018","journal-title":"Sens. Actuators B Chem."},{"key":"ref_47","doi-asserted-by":"crossref","first-page":"1677","DOI":"10.1021\/acssuschemeng.5b00383","article-title":"One-step fabrication of graphene oxide enhanced magnetic composite gel for highly efficient dye adsorption and catalysis","volume":"3","author":"Cheng","year":"2015","journal-title":"ACS Sustain. Chem. Eng."},{"key":"ref_48","doi-asserted-by":"crossref","first-page":"31","DOI":"10.1016\/j.nanoms.2019.02.004","article-title":"Synthesis, properties, and applications of graphene oxide\/reduced graphene oxide and their nanocomposites","volume":"1","author":"Smith","year":"2019","journal-title":"Nano Mater. Sci."},{"key":"ref_49","doi-asserted-by":"crossref","first-page":"3767","DOI":"10.1007\/s11696-020-01196-0","article-title":"Synthetic routes of the reduced graphene oxide","volume":"74","author":"Feng","year":"2020","journal-title":"Chem. Pap."},{"key":"ref_50","doi-asserted-by":"crossref","first-page":"1","DOI":"10.1016\/j.tca.2012.04.008","article-title":"Homer Kissinger and the Kissinger Equation","volume":"540","author":"Blaine","year":"2012","journal-title":"Thermochim. Acta"}],"container-title":["Catalysts"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/2073-4344\/12\/7\/735\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,10,10]],"date-time":"2025-10-10T23:42:07Z","timestamp":1760139727000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/2073-4344\/12\/7\/735"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2022,7,2]]},"references-count":50,"journal-issue":{"issue":"7","published-online":{"date-parts":[[2022,7]]}},"alternative-id":["catal12070735"],"URL":"https:\/\/doi.org\/10.3390\/catal12070735","relation":{},"ISSN":["2073-4344"],"issn-type":[{"type":"electronic","value":"2073-4344"}],"subject":[],"published":{"date-parts":[[2022,7,2]]}}}