Developing effective electrocatalyst and fundamentally understanding the corresponding working mechanism are both urgently desired to overcome the current challenges facing lithium-oxygen batteries (LOBs). Herein, a series of NiFe-based bimetal-organic frameworks (NiFe-MOFs) with certain internal tensile strain are fabricated via a simple organic linker scission strategy, and served as cathode catalysts for LOBs. The introduced tensile strain broadens the inherent interatomic distances, leading to an upshifted d-band center of metallic sites and thus the enhancement of the adsorption strength of catalysts surface towards intermediates, which is contributed to rationally regulate the crystallinity of discharge product Li₂O₂. As a result, the uniformly distributed amorphous film-like Li₂O₂ tightly deposits on the surface of strain-regulated MOF, resulting in excellent electrochemical performance of LOBs, including a large discharge capacity of 12317.4 mAh g⁻¹ at 100 mA g⁻¹ and extended long-term cyclability of 357 cycles. This work presents a novel insight in adjusting the adsorption strength of cathode catalysts towards intermediates via introducing tensile strain in catalysts, which is a pragmatic strategy for improving the performance of LOBs.

迫切需要开发有效的电催化剂并从根本上了解相应的工作机制，以克服当前锂氧电池（LOB）面临的挑战。在此，通过简单的有机接头断裂策略制备了一系列具有一定内部拉伸应变的 NiFe 基双金属有机骨架 (NiFe-MOF)，并用作 LOB 的阴极催化剂。引入的拉伸应变加宽了固有的原子间距离，导致金属位点的 d 带中心上移，从而增强了催化剂表面对中间体的吸附强度，这有助于合理调节放电产物 Li ₂ O ₂的结晶度. 结果，均匀分布的非晶膜状 Li_2层ö ₂应变调节MOF的表面上紧密地堆积，产生的LOB的优异的电化学性能，包括12317.4毫安g的放电容量大^-1在100mA克^-1和延长的周期357长期的可循环性。这项工作通过在催化剂中引入拉伸应变来调节阴极催化剂对中间体的吸附强度，这是一种提高 LOB 性能的实用策略。