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So, it is urgent to discover cost\u2010effective and earth\u2010abundant materials to replace precious\u2010metal electrocatalysts in order to make this technology economically viable. Herein, we report the preparation and application of three new nanocomposites based on polyoxometalates (POMs) and reduced oxidized\u2010graphene flakes (rGF_ox) as HER electrocatalysts (ECs). In highly acidic medium (pH=0.3), the POM@rGF_ox ECs showed similar overpotentials (0.033\u20130.044\u2005V vs. RHE) for a current density of 10\u2005mA\u2009cm<jats:sup>\u22122<\/jats:sup>, and these are very close to the state\u2010of\u2010the\u2010art HER EC, 20\u2005wt% Pt\/C (0.024\u2005V). The POM\u2010based nanocomposites also exhibited excellent exchange current densities (0.65\u20131.02\u2005mA\u2009cm<jats:sup>\u22122<\/jats:sup>) and very low Tafel slopes (0.033\u20130.041\u2005V\u2009dec<jats:sup>\u22121<\/jats:sup>). P<jats:sub>5<\/jats:sub>W<jats:sub>30<\/jats:sub>@rGF_ox exhibited the best HER metrics and also showed long\u2010term electrochemical stability, as the overpotential only changed 0.009\u2005V for <jats:italic>j<\/jats:italic>=10\u2005mA\u2009cm<jats:sup>\u22122<\/jats:sup> after 1000 linear sweep voltammetry cycles. Besides highlighting POM\u2010oxidized\u2010graphene flakes composites as a new class of nanomaterial with several important electrochemical applications, this work also points out that the POM shape, size, charge, and composition (W\/P ratio) may play an important role in fine\u2010tuning the HER activity, and opens new avenues for designing a new set of highly efficient, cost\u2010effective, and durable non\u2010precious\u2010metal HER ECs in acidic medium.<\/jats:p>","DOI":"10.1002\/celc.201701210","type":"journal-article","created":{"date-parts":[[2017,11,29]],"date-time":"2017-11-29T10:50:52Z","timestamp":1511952652000},"page":"273-283","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":76,"title":["Polyoxometalate\u2010graphene Electrocatalysts for the Hydrogen Evolution Reaction"],"prefix":"10.1002","volume":"5","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5263-2737","authenticated-orcid":false,"given":"Diana M.","family":"Fernandes","sequence":"first","affiliation":[{"name":"REQUIMTE\/LAQV, Departamento de Qu\u00edmica e Bioqu\u00edmica Faculdade de Ci\u00eancias Universidade do Porto  4169-007 Porto Portugal"}]},{"given":"Mariana P.","family":"Ara\u00fajo","sequence":"additional","affiliation":[{"name":"REQUIMTE\/LAQV, Departamento de Qu\u00edmica e Bioqu\u00edmica Faculdade de Ci\u00eancias Universidade do Porto  4169-007 Porto Portugal"}]},{"given":"Ali","family":"Haider","sequence":"additional","affiliation":[{"name":"Jacobs University Department of Life Sciences and Chemistry  Campus Ring 1 28759 Bremen Germany"},{"name":"Current address: Department of Chemistry Quaid-i-Azam University  45320- Islamabad Pakistan"}]},{"given":"Ali S.","family":"Mougharbel","sequence":"additional","affiliation":[{"name":"Jacobs University Department of Life Sciences and Chemistry  Campus Ring 1 28759 Bremen Germany"}]},{"given":"Ant\u00f3nio J. S.","family":"Fernandes","sequence":"additional","affiliation":[{"name":"Instituto de Nanoestruturas Nanomodela\u00e7\u00e3o e Nanofabrica\u00e7\u00e3o (I3N) Departamento de F\u00edsica Universidade de Aveiro  Campus Universit\u00e1rio de Santiago 3810-193 Aveiro Portugal"}]},{"given":"Ulrich","family":"Kortz","sequence":"additional","affiliation":[{"name":"Jacobs University Department of Life Sciences and Chemistry  Campus Ring 1 28759 Bremen Germany"}]},{"given":"Cristina","family":"Freire","sequence":"additional","affiliation":[{"name":"REQUIMTE\/LAQV, Departamento de Qu\u00edmica e Bioqu\u00edmica Faculdade de Ci\u00eancias Universidade do Porto  4169-007 Porto Portugal"}]}],"member":"311","published-online":{"date-parts":[[2017,11,28]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1039\/C4CS00448E"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1039\/C4CS00470A"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1039\/C4EE01760A"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/cs500923c"},{"key":"e_1_2_7_5_1","unstructured":"\u00a0"},{"key":"e_1_2_7_6_2","doi-asserted-by":"publisher","DOI":"10.1021\/cr960403a"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1007\/978-3-662-12004-0"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/0368-1874(85)80125-8"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.5b02899"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1021\/la7016853"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201006734"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja201165c"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5b02688"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.1621"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5EE03503A"},{"key":"e_1_2_7_16_1","unstructured":"\u00a0"},{"key":"e_1_2_7_17_2","doi-asserted-by":"publisher","DOI":"10.1002\/celc.201402271"},{"key":"e_1_2_7_18_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2015.12.045"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr500023c"},{"key":"e_1_2_7_20_1","unstructured":"\u00a0"},{"key":"e_1_2_7_21_2","doi-asserted-by":"publisher","DOI":"10.1039\/C3CS60217F"},{"key":"e_1_2_7_22_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2007.02.034"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/ic00220a036"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/ic00061a010"},{"key":"e_1_2_7_25_1","volume-title":"Potassium Octadecatungstodiphosphates(V) and Related Lacunary Compounds, in Inorganic Syntheses, Vol. 27","author":"Contant R.","year":"1990"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6RA28868E"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201310908"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.snb.2014.11.074"},{"key":"e_1_2_7_29_1","unstructured":"\u00a0"},{"key":"e_1_2_7_30_2","doi-asserted-by":"publisher","DOI":"10.1002\/chem.201304131"},{"key":"e_1_2_7_31_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2012.10.013"},{"key":"e_1_2_7_32_1","unstructured":"\u00a0"},{"key":"e_1_2_7_33_2","doi-asserted-by":"publisher","DOI":"10.1021\/jp027482g"},{"key":"e_1_2_7_34_2","doi-asserted-by":"publisher","DOI":"10.1039\/c1jm11266j"},{"key":"e_1_2_7_35_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0020-1693(00)92306-5"},{"key":"e_1_2_7_36_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.carbon.2004.03.005"},{"key":"e_1_2_7_37_1","doi-asserted-by":"publisher","DOI":"10.1039\/c2dt12465c"},{"key":"e_1_2_7_38_1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.97.187401"},{"key":"e_1_2_7_39_1","unstructured":"\u00a0"},{"key":"e_1_2_7_40_2","doi-asserted-by":"publisher","DOI":"10.1021\/jp0494335"},{"key":"e_1_2_7_41_2","doi-asserted-by":"publisher","DOI":"10.1016\/S1388-2481(00)00104-1"},{"key":"e_1_2_7_42_2","doi-asserted-by":"publisher","DOI":"10.1016\/0022-0728(87)80067-0"},{"key":"e_1_2_7_43_2","doi-asserted-by":"publisher","DOI":"10.1016\/0022-0728(88)85031-9"},{"key":"e_1_2_7_44_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.elecom.2009.08.019"},{"key":"e_1_2_7_45_1","unstructured":"\u00a0"},{"key":"e_1_2_7_46_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.electacta.2014.06.098"},{"key":"e_1_2_7_47_2","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.201400013"},{"key":"e_1_2_7_48_1","doi-asserted-by":"publisher","DOI":"10.1007\/978-1-4471-6428-9"},{"key":"e_1_2_7_49_1","doi-asserted-by":"publisher","DOI":"10.1021\/nn5012144"},{"key":"e_1_2_7_50_1","first-page":"8","volume":"7","author":"Li J. 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