Metal–CO₂ rechargeable batteries have immense application potential owing to their high theoretical energy densities and CO₂ capture capabilities. However, batteries relying on carbonate production typically offer low output voltages (<2.6 V) and energy efficiencies. Herein, the six-element high-entropy alloy PtRuZnCoNiCu (PRZCNC-HEA) was employed as a cathode catalyst in metal–CO₂ batteries. The multiple reaction sites on the PRZCNC-HEA surface offered a symbiotic reaction pathway for oxalate product generation with a high discharge voltage and a low bandgap. The metal–oxalate coordination mode and metal–oxalate–carbonate coupling mechanism stabilized the oxalate product. Li–CO₂ batteries with PRZCNC-HEA as the cathode catalyst achieved a high discharge voltage (3.06 V) and low overpotential (0.32 V), representing the best-reported performance to date. Theoretical calculations combined with experimental characterization confirmed the stabilization mechanism. This work can advance the design and modulation of conversion reactions in metal–CO₂ batteries.

中文翻译：

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高熵合金催化剂上的共生反应可实现超高压 Li-CO2 电池


金属-CO₂ 可充电电池由于其高理论能量密度和 CO₂ 捕获能力而具有巨大的应用潜力。然而，依赖碳酸盐生产的电池通常具有低输出电压 （<2.6 V） 和能源效率。在此，六元素高熵合金 PtRuZnCoNiCu （PRZCNC-HEA） 被用作金属-CO₂ 电池的阴极催化剂。PRZCNC-HEA 表面的多个反应位点为草酸盐产物的生成提供了共生反应途径，具有高放电电压和低带隙。金属-草酸盐配位模式和金属-草酸盐-碳酸盐偶联机制稳定了草酸盐产物。以 PRZCNC-HEA 为阴极催化剂的 Li-CO₂ 电池实现了高放电电压 （3.06 V） 和低过电位 （0.32 V），代表了迄今为止报告的最佳性能。理论计算结合实验表征证实了稳定机制。这项工作可以推进金属-CO₂ 电池中转化反应的设计和调制。