The development of inexpensive, highly active, and stable non-precious metal catalysts is the key to efficient H₂ production by the electrolysis of water. Based on initial theoretical predictions, we report the design and synthesis of N-doped, defect-containing, carbon-dots (CDs)-loaded molybdenum phosphide (MoP/CDs) nanoparticles using CDs with different N contents. This optimized composite material performed outstandingly in the hydrogen evolution reaction (HER), with an overpotential of 70 mV at a current density of 10 mA cm⁻² with a 1.0 M KOH electrolyte. N doping changed the electronic arrangement around the reaction site, promoting the adsorption of HER intermediates. Increasing the N content further activated the adjacent C atoms to detach due to the more negative C vacancy formation energies resulting in a defect site with lost atoms and changed bond lengths. The introduction of defects increases the number of dangling bonds adjacent to reaction sites and reduces site coordination numbers, changing their electrocatalytic activity. Results show that N-doped and defect-containing MoP/CDs nanoparticles have excellent H₂ production performance during the electrolysis of alkaline solution. These findings open a new area of application of heteroatom-doped CDs and provide new ideas for the design of efficient carbon-semiconductor composite HER catalysts.

廉价，高活性和稳定的非贵金属催化剂的开发是通过电解水有效生产H ₂的关键。基于初步的理论预测，我们报告了使用具有不同N含量的CD来设计和合成N掺杂，含缺陷的碳点（CDs）负载的磷化钼（MoP / CDs）纳米颗粒的设计和合成。这种经过优化的复合材料在放氢反应（HER）中表现出色，在10 mA cm ^-2的电流密度下具有70 mV的过电势用1.0 M KOH电解质。N掺杂改变了反应部位周围的电子排列，从而促进了HER中间体的吸附。N含量的增加会进一步激活相邻的C原子，因为更多的负C空位形成能导致其脱离，从而导致缺陷部位出现原子损失和键长变化。缺陷的引入增加了反应位点附近的悬空键的数量，并降低了位点配位数，从而改变了它们的电催化活性。结果表明，掺氮和含缺陷的MoP / CDs纳米颗粒具有优异的H ₂碱性溶液电解过程中的生产性能。这些发现为杂原子掺杂的CD开辟了新的应用领域，并为设计高效的碳-半导体复合材料HER催化剂提供了新的思路。