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A stabilization synthesis strategy for atomically dispersed metal-N4 electrocatalysts via aerogel confinement and ammonia pyrolyzing
Nano Energy ( IF 16.8 ) Pub Date : 2022-10-03 , DOI: 10.1016/j.nanoen.2022.107869
Yi Luo , Jiao Wu , Yongting Chen , Junzong Feng , Lukai Wang , Liangjun Li , Yonggang Jiang , Yongpeng Lei , Jian Feng

Catalytically active metals that are atomically dispersed on supports exhibit the highest atom utilization and most cost-effective pathways for electrocatalyst design. However, the high-throughput scalable production of inexpensive, efficient, and durable atomically dispersed electrocatalysts remains challenging. Herein, a hierarchical porous carbon aerogel loaded with atomically dispersed metal-N4 (metal-N-C) was synthesized via the NH3 pyrolysis of a metal-doped polymer aerogel. This novel synthetic strategy requires the tailoring of various materials, such as metal sol, resorcinol formaldehyde sol, hydrogel, and metal-N-C. The synthetic applicability of this strategy was demonstrated via the facile synthesis of Co-N-C, Ni-N-C, and Fe-N-C. Notably, Fe-N-C exhibited a half-wave potential of approximately 0.933 V vs. reversible hydrogen electrode and lost approximately 4 mV after 5000 cycles of accelerated aging test in a 0.1 mol/L KOH solution for the oxygen reduction reaction. In a solid-state zinc-air battery, Fe-N-C exhibited a maximum power density of 167 m W cm−2, an energy density of 956 W h Kg−1, and long-term stability over 120 h, which significantly exceeds that of commercial Pt/C. The high activity and durability of Fe-N-C is attributed to the double Fe-N4 active center, where the synergistic effect of the neighboring Fe-N4 promotes oxygen dissociation and produces less H2O2. The developed strategy provides an aerogel-based solution for fabricating inexpensive, efficient, and durable atomically dispersed electrocatalysts with potential for high-throughput scalable production and expands the understanding of the synthesis of atomically dispersed electrocatalysts.



中文翻译:

一种通过气凝胶约束和氨热解稳定合成原子分散金属-N4电催化剂的策略

原子分散在载体上的催化活性金属表现出最高的原子利用率和最具成本效益的电催化剂设计途径。然而,廉价、高效和耐用的原子分散电催化剂的高通量可扩展生产仍然具有挑战性。在此,通过NH 3合成了负载有原子分散的金属-N 4 (metal-NC)的分级多孔碳气凝胶。金属掺杂聚合物气凝胶的热解。这种新颖的合成策略需要定制各种材料,例如金属溶胶、间苯二酚甲醛溶胶、水凝胶和金属-NC。通过 Co-NC、Ni-NC 和 Fe-NC 的简便合成证明了该策略的合成适用性。值得注意的是,在氧还原反应的 0.1 mol/L KOH 溶液中进行 5000 次加速老化测试后,Fe-NC 与可逆氢电极的半波电位约为 0.933 V,并且损失了约 4 mV。在固态锌空气电池中,Fe-NC 的最大功率密度为 167 m W cm -2,能量密度为 956 W h Kg -1,以及超过 120 小时的长期稳定性,显着超过商业 Pt/C。Fe-NC的高活性和耐久性归因于双Fe-N 4活性中心,其中相邻Fe-N 4的协同作用促进了氧解离并产生较少的H 2 O 2。所开发的策略为制造廉价、高效和耐用的原子分散电催化剂提供了一种基于气凝胶的解决方案,具有高通量可扩展生产的潜力,并扩大了对原子分散电催化剂合成的理解。

更新日期:2022-10-03
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