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Thin carbon layer covered Co4N cubes encapsulated in N-doped porous carbon nanocage as tri-functional catalysts with enhanced charge-transfer efficiency for Zn-air battery and overall water-splitting
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-05-11 , DOI: 10.1039/d3ta01509b Guanghui Zhang 1 , Lingxue Zhao 1 , Guangda Li 1 , Liqiang Xu 2
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-05-11 , DOI: 10.1039/d3ta01509b Guanghui Zhang 1 , Lingxue Zhao 1 , Guangda Li 1 , Liqiang Xu 2
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High-efficiency bifunctional catalysts with high energy conversion efficiency and high cycling performance are urgently needed for traditional zinc-air batteries (ZABs). Herein, a composite of highly active carbon layer covered Co4N cubes encapsulated in a nitrogen-doped porous carbon nanocage (Co4NC@NC) as a cathode catalyst was prepared by a hydrothermal acid-assisted strategy combined with subsequent calcination. The precursor is treated with carbon coating and calcination to obtain a double-carbon-layer-coated structure of Co4NC@NC. The inner carbon layer is tightly wrapped on the surface of the Co4N particles, and the outer carbon layer presents a porous structure. Co4NC@NC exhibits significantly enhanced electrocatalytic activities for ORR, OER and HER. In particular, the overpotential is only 166 mV for OER at a current density of 10 mA cm−2. Density functional theory calculations reveal that the synergistic effect between the N-doped graphite carbon layer and Co4N can improve the adsorption efficiency of intermediate products, accelerate the reaction kinetics, and reduce the free energy of rate determining steps. ZABs assembled with Co4NC@NC showed excellent stability during 1050 cycles at 5 mA cm−2. Furthermore, Co4NC@CN can also be used as an HER catalyst for overall water splitting, driven by Co4NC@CN-ZABs. The above results indicate that Co4NC@CN can be used as a high-performance three-function catalyst for ZABs and overall water splitting.
中文翻译：
薄碳层覆盖包裹在 N 掺杂多孔碳纳米笼中的 Co4N 立方体作为三功能催化剂，提高锌空气电池的电荷转移效率和整体水分解
传统的锌空气电池（ZABs）迫切需要具有高能量转换效率和高循环性能的高效双功能催化剂。在此，通过水热酸辅助策略结合随后的煅烧制备了高活性碳层覆盖的复合材料，Co 4 N 立方体包裹在氮掺杂多孔碳纳米笼中 (Co 4 NC@NC) 作为阴极催化剂。前驱体经碳包覆和煅烧处理得到Co 4 NC@NC的双碳层包覆结构。内层碳层紧紧包裹在Co 4 N颗粒表面，外层碳层呈现多孔结构。钴4NC@NC 对 ORR、OER 和 HER 表现出显着增强的电催化活性。特别是，在 10 mA cm -2的电流密度下，OER 的过电势仅为 166 mV 。密度泛函理论计算表明，N掺杂石墨碳层与Co 4 N之间的协同作用可以提高中间产物的吸附效率，加快反应动力学，降低限速步骤的自由能。用 Co 4 NC@NC组装的 ZAB在 5 mA cm -2下在 1050 个循环期间表现出优异的稳定性。此外，Co 4 NC@CN 还可以用作全水分解的 HER 催化剂，由 Co 4驱动NC@CN-ZAB。上述结果表明Co 4 NC@CN可作为ZABs和全分解水的高性能三功能催化剂。
更新日期：2023-05-11
中文翻译：
薄碳层覆盖包裹在 N 掺杂多孔碳纳米笼中的 Co4N 立方体作为三功能催化剂，提高锌空气电池的电荷转移效率和整体水分解
传统的锌空气电池（ZABs）迫切需要具有高能量转换效率和高循环性能的高效双功能催化剂。在此，通过水热酸辅助策略结合随后的煅烧制备了高活性碳层覆盖的复合材料，Co 4 N 立方体包裹在氮掺杂多孔碳纳米笼中 (Co 4 NC@NC) 作为阴极催化剂。前驱体经碳包覆和煅烧处理得到Co 4 NC@NC的双碳层包覆结构。内层碳层紧紧包裹在Co 4 N颗粒表面，外层碳层呈现多孔结构。钴4NC@NC 对 ORR、OER 和 HER 表现出显着增强的电催化活性。特别是，在 10 mA cm -2的电流密度下，OER 的过电势仅为 166 mV 。密度泛函理论计算表明，N掺杂石墨碳层与Co 4 N之间的协同作用可以提高中间产物的吸附效率，加快反应动力学，降低限速步骤的自由能。用 Co 4 NC@NC组装的 ZAB在 5 mA cm -2下在 1050 个循环期间表现出优异的稳定性。此外，Co 4 NC@CN 还可以用作全水分解的 HER 催化剂，由 Co 4驱动NC@CN-ZAB。上述结果表明Co 4 NC@CN可作为ZABs和全分解水的高性能三功能催化剂。
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