Plasma synthesis of defect-rich flexible carbon cloth decorated with PtRu alloyed nanoclusters for highly efficient pH-universal electrocatalytic hydrogen evolution

Jingsen Zhang; Xiuling Zhang; Chuan Shi; Guangqing Xia; Hong Li; Peng Wang; Lanbo Di

doi:10.1039/d2nr04369f

Plasma synthesis of defect-rich flexible carbon cloth decorated with PtRu alloyed nanoclusters for highly efficient pH-universal electrocatalytic hydrogen evolution

Nanoscale. 2022 Nov 3;14(42):15942-15949. doi: 10.1039/d2nr04369f.

Authors

Jingsen Zhang¹, Xiuling Zhang², Chuan Shi¹, Guangqing Xia^{3

4}, Hong Li², Peng Wang², Lanbo Di^{2

3

4}

Affiliations

¹ State Key Laboratory of Fine Chemicals, College of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.
² College of Physical Science and Technology, Dalian University, Dalian 116622, China. dilanbo@163.com.
³ State Key Laboratory of Structural Analysis for Industrial Equipment, Dalian University of Technology, Dalian 116024, China.
⁴ Key Laboratory of Advanced Technology for Aerospace Vehicles of Liaoning Province, Dalian University of Technology, Dalian 116024, China.

PMID: 36269310
DOI: 10.1039/d2nr04369f

Abstract

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.