For the generation of hydrogen peroxide (H₂O₂), a robust electrocatalyst with high activity, selectivity and stability under pH-universal conditions is a formidable challenge. Herein, Pd₄Se nanoparticles (NPs) have been proposed as a highly active, selective and durable electrocatalyst for H₂O₂ production over a wide pH range for the first time. In particular, the Pd₄Se NPs show superior H₂O₂ production selectivities of 93.5%, 89.7%, and 86.7% in 0.1 M HClO₄, 0.1 M KCl and 0.1 M KOH electrolytes, respectively. Density functional theory (DFT) calculations reveal that Se incorporation prevents the OO early-cleavage issue by suppressing the excessive electronegativity of the Pd sites. In addition, a strong p-d repulsive correlation shifts the Pd-4d band towards the electron-depleting centre, allowing near-barrier-free electron transfer and facilitating [OOH^-] stabilization. Owing to a high energy barrier of the dissociation of [OOH^-], the four-electrons oxygen reduction pathway is significantly suppressed for high H₂O₂ selectivity. The Pd₄Se NPs are also highly stable, with only a 2.4%, 9.6% and 3.4% decrease for H₂O₂ selectivity in 0.1 M HClO₄, 0.1 M KCl and 0.1 M KOH electrolytes, respectively, after 5000 cycles, which shows that these NPs are a unique and robust Pd-based electrocatalyst for H₂O₂ generation under pH-universal conditions.

对于过氧化氢 (H ₂ O ₂ )的生成，在通用 pH 条件下具有高活性、选择性和稳定性的强大电催化剂是一项艰巨的挑战。在此，首次提出Pd ₄ Se 纳米粒子 (NPs) 作为一种高活性、选择性和耐用的电催化剂，用于在较宽的 pH 范围内生产H ₂ O ₂。特别是，Pd ₄ Se NPs在 0.1 M HClO ₄、0.1 M KCl 和 0.1 M KOH 电解质中显示出优异的 H ₂ O ₂生产选择性，分别为 93.5%、89.7% 和 86.7% 。密度泛函理论 (DFT) 计算表明，Se 掺入阻止了 O通过抑制 Pd 位点的过度电负性导致 O 早期裂解问题。此外，强烈的 pd 排斥相关性将 Pd-4d 带移向电子耗尽中心，允许近乎无障碍的电子转移并促进 [OOH ^- ] 稳定。由于 [OOH ^- ]解离的高能垒，四电子氧还原途径被显着抑制以实现高 H ₂ O ₂选择性。Pd ₄ Se NPs 也非常稳定，在 0.1 M HClO _{4 中的}H ₂ O ₂选择性仅降低 2.4%、9.6% 和 3.4%、0.1 M KCl 和 0.1 M KOH 电解质，在 5000 次循环后，这表明这些 NPs 是一种独特且稳定的 Pd 基电催化剂，用于在 pH 通用条件下生成H ₂ O ₂。