In the quest to replace fossil fuels and reduce carbon dioxide emissions, developing energy technologies based on clean catalytic processes is fundamental. However, the cost-effectiveness of these technologies strongly relies on the availability of efficient catalysts made of abundant elements. Herein, this study presents a one-step hydrothermal method to obtain a series of Ni₃Se₄ nanoparticles with a layer of amorphous selenium on their surface. When employed as electrocatalysts for the methanol oxidation reaction (MOR), the optimized proper surface Se-coated Ni₃Se₄ nanoparticles exhibit a high current density of 160 mA cm^–2 at 1.6 V, achieving a high methanol-to-formate Faradaic efficiency above 97.8% and excellent stability with less than 20% current decay after an 18 h chronoamperometry test. This excellent performance is rationalized using density functional theory calculations, which unveil that the electrochemical recombination of SeO_x results in a reduction of the energy barrier for the dehydrogenation of methanol during the MOR process.

中文翻译：

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表面硒涂层促进 Ni3Se4 纳米颗粒上的选择性甲醇制甲酸盐电氧化


在寻求替代化石燃料和减少二氧化碳排放的过程中，开发基于清洁催化过程的能源技术至关重要。然而，这些技术的成本效益在很大程度上取决于由丰富元素制成的高效催化剂的可用性。在此，本研究提出了一种一步水热法，以获得一系列表面具有一层无定形硒的 Ni₃Se₄ 纳米颗粒。当用作甲醇氧化反应 （MOR） 的电催化剂时，优化的适当表面 Se 包被的 Ni₃Se₄ 纳米颗粒在 1.6 V 下表现出 160 mA cm^–2 的高电流密度，实现了高于 97.8% 的高甲醇制甲酸盐法拉第效率和出色的稳定性，在 18 h 计时安培测试后电流衰减小于 20%。这种优异的性能使用密度泛函理论计算进行了合理化，该计算揭示了 SeO_x 的电化学复合导致 MOR 过程中甲醇脱氢的能垒减少。