Hydrogen, regarded as a promising energy carrier to alleviate the current energy crisis, can be generated from hydrogen evolution reaction (HER), whereas its efficiency is impeded by the activity of catalysts. Herein, effective strategies, such as strain and interfacial engineering, are imposed to tune the catalysis performance of novel two-dimensional (2D) phosphorus carbide (PC) layers using first-principle calculations. The findings show that P site in pristine monolayer PC (ML-PC) exhibits higher HER performance than C site. Intriguingly, constructing bilayer PC sheet (BL-PC) can change the coordinate configuration of P atom to form 3-coordination-P atom (3-co-P) and 4-coordination-P atom (4-co-P), and the original activity of 3-co-P site is higher than the 4-co-P site. When an external compressive strain is applied, the activity of the 4-co-P site is enhanced whereas the external strain can barely affect that of 3-co-P site. Interestingly, the graphene substrate enhances the overall activity of the BL-PC because the graphene substrate optimizes the ΔG _H* value of 4-co-P site, although it can barely affect the HER activity of 3-co-P site and ML-PC. The desirable properties render 2D PC-based material promising candidates for HER catalysts and shed light on the wide utilization in electrocatalysis.

氢被认为是缓解当前能源危机的一种很有前途的能源载体，它可以通过析氢反应（HER）产生，但其效率受到催化剂活性的阻碍。在此，采用有效策略，如应变和界面工程，使用第一性原理计算来调整新型二维 (2D) 碳化磷 (PC) 层的催化性能。研究结果表明，原始单层 PC (ML-PC) 中的 P 位点表现出比 C 位点更高的 HER 性能。有趣的是，构建双层PC片（BL-PC）可以改变P原子的配位构型，形成3-配位-P原子（3-co-P）和4-配位-P原子（4-co-P），并且3-co-P位点的原始活性高于4-co-P位点。当施加外部压缩应变时，4-co-P位点的活性增强，而外部应变几乎不能影响3-co-P位点的活性。有趣的是，石墨烯基板增强了 BL-PC 的整体活性，因为石墨烯基板优化了 Δ4-co-P 位点的G _H*值，虽然对 3-co-P 位点和 ML-PC 的 HER 活性几乎没有影响。理想的特性使二维 PC 基材料成为 HER 催化剂的有希望的候选者，并阐明了在电催化中的广泛应用。