Designing electrocatalysts with superior activity and stability to Pt/C for the highly efficient pH-universal electrochemical hydrogen evolution reaction (HER) still remains an urgent challenge. Herein, we report a facile plasma method for the preparation of defect-rich flexible carbon cloth decorated with ultralow-loading (0.1 wt%) PtRu alloyed nanoclusters (PtRu/CC-P) to resolve these problems. Remarkably, the developed PtRu/CC-P catalyst delivered a high mass activity of 3.77 A mg−1 (η = 100 mV), almost 3.6 times higher than that of the benchmark HER electrocatalyst 20%Pt/C (1.05 A mg−1). Meanwhile, it only required a low overpotential of 44 mV to achieve a current density of 10 mA cm−2 in alkaline media. Systematic experimental and DFT calculation results revealed that the Pt–Ru bridge of PtRu alloyed nanoclusters in PtRu/CC-P can optimize the adsorption strength of HER intermediates at active sites, decrease the H2O dissociation energy barrier, and consequently facilitate the HER kinetics. Inspiringly, when the PtRu content was increased to 1 wt%, PtRu/CC-P still exhibited a relatively low overpotential of 276 mV even at a high current density of 1000 mA cm−2 and maintained excellent durability at a relatively high current density of 50–500 mA cm−2 for more than 15 h in alkaline media. In addition, PtRu/CC-P also showed brilliant HER activity and stability in neutral and acidic media. This facile method provides a feasible route for the rational design of Pt-based alloyed catalysts toward industrial hydrogen production at all-pH values.
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