with the H 1s band. Among these catalysts, noble metals such as Pt and Ir exhibit the best HER activity locating at the top of the volcano plot, due to the Sabatier's principle. [15][16][17] However, the earth abundance of noble metals is an inevitable and insurmountable obstacle for the practical application of noble metals. Alloying noble metals with high-abundance metals is a possible way to reducing the usage of noble metals while sustaining their high catalytical performance, which remains a challenging mission. [18][19][20] Metal sites in complexes usually exhibit insufficient adsorption ability for active *H species, due to the Coulomb repulsion. Suffering from the insufficient adsorption, the metal sites in many catalysts are inert. For example, the Mo sites in MoX 2 (X = S, Se) are inactive for HER. [21][22][23] To enhance the HER performance of metal sites in complex, novel metal sites with abundant electrons are proposed to strengthen the interaction with *H. Kobayashi et al. reported negatively charged Pt obtained by light doping of W through electrochemical cleaning of core/shell PtW@WO 3 nanoparticles, to enhance the HER activity significantly. [24] The negatively charged Pt atoms provide favorable hydrogen adsorption energy, resulting in an overpotential superior to commercial Pt. As another example, Wei et al. prepared Pt clusters on TiO 2 with rich O vacancies. [25] Reversed charge transfer from TiO 2 to Pt is realized to boost the hydrogen evolution.In this work, we prepared ternary Ir 1−x Rh x Sb intermetallic alloy as highly active electrocatalyst for HER. Due to the large difference in the reduction potential of Ir, Rh, and Sb cations, the Ir 1−x Rh x Sb cannot be synthesized by common solvothermal method. The arc-melting method was then used for the preparation of Ir 1−x Rh x Sb alloy. The electron transfer can be well regulated by modulating the content ratio. Ir atoms in IrSb exhibit negative valence state owing to the electron transfer form Sb to Ir, as revealed by both experimental data and first-principal calculations. The hydrogen adsorption ability of Ir sites is then highly strengthened due to the accumulated electrons. Furthermore, the HER activity of Ir 1−x Rh x Sb is closely modulated and optimized by Rh doping. As a result, the Ir 0.7 Rh 0.3 Sb sample exhibits the best HER activity, with an overpotential of 22 mV at 10 mA cm -2 and a Tafel slope of 47.6 mV dec -1 . This work provides insights into highly active alloys and sheds lights on the utilization of electron-abundant metal atoms.Alloying noble metals with non-noble metals is a promising method to fabricate catalysts, with the advantages of reduced noble metal usage and excellent activity. In this work, electron-abundant Ir/Rh sites, as highly active centers for the hydrogen evolution reaction (HER), are realized by fabricating Ir 1−x Rh x Sb alloys through the arc-melting method. The electron transfer from Sb to Ir/Rh makes the latter negatively charged, leading to considerably optimized adsorption for active H species dur...

A phosphorus-modified cobalt single atom catalyst supported on crosslinked carbon nanosheets was developed, which showed a superb catalytic activity for alkaline hydrogen evolution reaction.

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We developed an in situ self-corrosion photodeposition method for the fabrication of a self-standing hollow Fe–NiOHx catalyst with an excellent OER activity and remarkable stability in alkaline media.