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There is no doubt that hydrogen energy can play significant role in promoting the development and progress of modern society. The utilization of hydrogen energy has developed rapidly, but it is far from the requirement of human. Therefore, it is very urgent to develop methodologies and technologies for efficient hydrogen production, especially high activity and durable electrocatalysts. Here a bimetallic oxide cluster on heterostructure of vanadium ruthenium oxides/graphdiyne (VRuOx/GDY) is reported. The unique acetylene‐rich structure of graphdiyne achieves outstanding characteristics of electrocatalyst: i) controlled preparation of catalysts for achieving multiple‐metal clusters; ii) regulation of catalyst composition and morphology for synthesizing high‐performance catalysts; iii) highly active and durable hydrogen evolution reaction (HER) properties. The optimal porous electrocatalyst (VRu0.027Ox/GDY) can deliver 10 mA cm−2 at low overpotentials of 13 and 12 mV together with robust long‐term stability in alkaline and neutral media, respectively, which are much smaller than Pt/C. The results reveal that the synergism of different components can efficiently facilitate the electron/mass transport properties, reduce the energy barrier, and increase the active site number for high catalytic performances. [ABSTRACT FROM AUTHOR]

A highly efficient bifunctional metal‐free catalyst was prepared by growth of three‐dimensional porous fluorographdiyne networks on carbon cloth (p‐FGDY/CC). Our experiments and density functional theory (DFT) calculations show the 3D p‐FGDY/CC network is highly active and it is a high potential metal‐free catalyst for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), as well as overall water splitting (OWS) under both acidic and alkaline conditions. The experimental and theoretical results show very good consistency; for example, in the HER process, p‐FGDY/CC exhibits small overpotentials of 82 and 92 mV to achieve 10 mA cm−2 under alkaline and acidic conditions, respectively. This ensures an even higher selectivity for the adsorption/desorption of various O/H intermediate species. The essential key promotion accomplishes a bifunctional H2O redox performance application under pH‐universal electrochemical conditions. [ABSTRACT FROM AUTHOR]