Proton exchange membrane water electrolysis (PEMWE) requires Pt-based hydrogen evolution reaction (HER) electrocatalysts, which makes current systems costly. Low-cost alternatives have struggled to meet the requiremen...Proton exchange membrane water electrolysis (PEMWE) requires Pt-based hydrogen evolution reaction (HER) electrocatalysts, which makes current systems costly. Low-cost alternatives have struggled to meet the requirements of both electrocatalytic activity and durability at high-current density operations. Here, we developed phosphorus-modified nickel with ruthenium nanoclusters self-supported on carbon paper (P-NiRu/CP) as efficient HER electrocatalysts. By leveraging metal-organic framework precursors and optimizing the phosphidation process, a dynamic interface between Ru, Ni, and P exhibited optimized hydrogen adsorption/desorption energies and facilitated hydrogen mobility, promoting efficient Tafel recombination. The P-NiRu/CP exhibited an overpotential of 22 mV at 10 mA cm^(−2) and a Tafel slope of 29 mV dec^(−1), outperforming benchmark Pt/C. Computational studies revealed that the dynamic interface in P-NiRu/CP enhanced the electrocatalytic activity. When employed as the cathode in a PEMWE single cell (with commercial IrO2 as the anode) operating with pure deionized water, P-NiRu/CP achieved 2.05 V at 3.0 A cm^(−2) with stable operation over 500 h, highlighting P-NiRu/CP as a cost-effective, durable, and scalable electrocatalyst for sustainable hydrogen production.展开更多
To accomplish mass hydrogen production by electrochemical water-splitting,it is a necessary to develop robust,highly active,stable,and cost-effective hydrogen evolution reaction(HER)electrocatalysts that perform compa...To accomplish mass hydrogen production by electrochemical water-splitting,it is a necessary to develop robust,highly active,stable,and cost-effective hydrogen evolution reaction(HER)electrocatalysts that perform comparably to Pt in the universal pH range.In this work,cobalt phosphide hybrid nanosheets supported on carbon felt(CoP HNS/CF)are presented,which exhibit the superior electrocatalytic hydrogen production under a universal-pH.In these nanosheets,a single CoP HNS is composed of polycrystalline CoP and oxygen-enriched amorphous Co-O-P phase.Benefiting from its unique nanoarchitecture,as-fabricated CoP HNS/CF exhibits a tremendous electrocatalytic HER activity and outperforms Pt/C as well as state-of-the-art CoP electrocatalysts in universal-pH.In acidic and neutral media,the CoP HNS/CF shows superior electrocatalytic activity while maintaining its original hybrid crystalline-amorphous phase and morphology.In alkaline medium,the unexpected phase and morphological reorganization of CoP HNS/CF results in outstanding electrocatalytic operation.CoP HNS/CF not only achieves high electrocatalytic activity and kinetics,but also a stable and long operating lifetime even under a high current density of 500 mA cm'2.Furthermore,the fabrication of CoP HNS/CF can be scaled up easily,and the large CoP HNS/CF electrode also exhibits similar electrocatalytic activity and stability.展开更多
基金supported by the National R&D Program through the National Research Foundation of Korea(NRF),funded by the Ministry of Science and ICT,Republic of Korea(RS-2024-00409901 and RS-2025-02304646).
文摘Proton exchange membrane water electrolysis (PEMWE) requires Pt-based hydrogen evolution reaction (HER) electrocatalysts, which makes current systems costly. Low-cost alternatives have struggled to meet the requirements of both electrocatalytic activity and durability at high-current density operations. Here, we developed phosphorus-modified nickel with ruthenium nanoclusters self-supported on carbon paper (P-NiRu/CP) as efficient HER electrocatalysts. By leveraging metal-organic framework precursors and optimizing the phosphidation process, a dynamic interface between Ru, Ni, and P exhibited optimized hydrogen adsorption/desorption energies and facilitated hydrogen mobility, promoting efficient Tafel recombination. The P-NiRu/CP exhibited an overpotential of 22 mV at 10 mA cm^(−2) and a Tafel slope of 29 mV dec^(−1), outperforming benchmark Pt/C. Computational studies revealed that the dynamic interface in P-NiRu/CP enhanced the electrocatalytic activity. When employed as the cathode in a PEMWE single cell (with commercial IrO2 as the anode) operating with pure deionized water, P-NiRu/CP achieved 2.05 V at 3.0 A cm^(−2) with stable operation over 500 h, highlighting P-NiRu/CP as a cost-effective, durable, and scalable electrocatalyst for sustainable hydrogen production.
基金This work is supported by the National Research Foundation of Korea(NRF)Grant funded by the M inistry of Science and ICT,South Korea(No.2016M3A7B4909318)We thank the Korea Basic Science Institute(KBSI)for the technical support.M icrostructural images were obtained using a Hitachi SU-70 scanning electron microscope at the KBSI.
文摘To accomplish mass hydrogen production by electrochemical water-splitting,it is a necessary to develop robust,highly active,stable,and cost-effective hydrogen evolution reaction(HER)electrocatalysts that perform comparably to Pt in the universal pH range.In this work,cobalt phosphide hybrid nanosheets supported on carbon felt(CoP HNS/CF)are presented,which exhibit the superior electrocatalytic hydrogen production under a universal-pH.In these nanosheets,a single CoP HNS is composed of polycrystalline CoP and oxygen-enriched amorphous Co-O-P phase.Benefiting from its unique nanoarchitecture,as-fabricated CoP HNS/CF exhibits a tremendous electrocatalytic HER activity and outperforms Pt/C as well as state-of-the-art CoP electrocatalysts in universal-pH.In acidic and neutral media,the CoP HNS/CF shows superior electrocatalytic activity while maintaining its original hybrid crystalline-amorphous phase and morphology.In alkaline medium,the unexpected phase and morphological reorganization of CoP HNS/CF results in outstanding electrocatalytic operation.CoP HNS/CF not only achieves high electrocatalytic activity and kinetics,but also a stable and long operating lifetime even under a high current density of 500 mA cm'2.Furthermore,the fabrication of CoP HNS/CF can be scaled up easily,and the large CoP HNS/CF electrode also exhibits similar electrocatalytic activity and stability.
