Abstract

The use of highly-active and robust catalysts is crucial for producing green hydrogen by water electrolysis as we strive to achieve global carbon neutrality. Noble metals like platinum are currently used catalysts in industry for the hydrogen evolution, but suffer from scarcity, high price and unsatisfied performance and stability at large current density, restrict their large-scale implementations. Here we report the synthesis of a type of monolith catalyst consisting of a metal disulfide (e.g., tantalum sulfides) vertically bonded to a conductive substrate of the same metal tantalum by strong covalent bonds. These features give the monolith catalyst a mechanically-robust and electrically near-zero-resistance interface, leading to an excellent hydrogen evolution performance including rapid charge transfer and excellent durability, together with a low overpotential of 398 mV to achieve a current density of 2,000 mA cm−2 as required by industry. The monolith catalyst has a negligible performance decay after 200 h operation at large current densities. In light of its robust and metallic interface and the various choices of metals giving the same structure, such monolith materials would have broad uses besides catalysis.

Highlights

  • The use of highly-active and robust catalysts is crucial for producing green hydrogen by water electrolysis as we strive to achieve global carbon neutrality

  • The TaTaS2 monolith catalyst (MC), with a current density of 1120 mA cm−2, stands out from them and more importantly, the Ta-TaS2 MC has significant advantages both from large current activity and long-term durability (Fig. 4e and Supplementary Table 3). These results show that a strong catalyst/substrate interface has been built in the MC, which can support hydrogen production at the large current density required by industry

  • We have attempted to solve the challenge of large-current-density water electrolysis by the design and synthesis of MCs

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Summary

Introduction

The use of highly-active and robust catalysts is crucial for producing green hydrogen by water electrolysis as we strive to achieve global carbon neutrality. We report the synthesis of a type of monolith catalyst consisting of a metal disulfide (e.g., tantalum sulfides) vertically bonded to a conductive substrate of the same metal tantalum by strong covalent bonds These features give the monolith catalyst a mechanically-robust and electrically near-zero-resistance interface, leading to an excellent hydrogen evolution performance including rapid charge transfer and excellent durability, together with a low overpotential of 398 mV to achieve a current density of 2,000 mA cm−2 as required by industry. Due to the nature of the monolith, charges can be directly transferred from the substrate to the catalyst without crossing van der Waals interfaces, providing highly efficient charge injection and an excellent HER performance This MC has almost zero interface resistance and offers unimpeded electron transfer. A tantalum–tantalum sulfide (Ta-TaS2) MC with a large area has been synthesized by the OSPS method and shown superior hydrogen evolution activity, achieving 2000 mA cm−2 with a small overpotential of 398 mV and continue working for >200 h under large current densities in a 0.5 M H2SO4 electrolyte without noticeable performance decay

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