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Advanced Trifunctional Electrocatalysis with Cu-, N-, S-Doped Defect-Rich Porous Carbon for Rechargeable Zn–Air Batteries and Self-Driven Water Splitting
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2021-09-17 , DOI: 10.1021/acssuschemeng.1c04745
Mingwen Wang 1 , Kunmei Su 2 , Maliang Zhang 1 , Xi Du 1 , Zhenhuan Li 1
Affiliation  

Fuel cells and water splitting are promising sustainable energy storage and conversion systems that can facilitate the usage of renewable resources and reduce the reliance on fossil fuels. These applications require catalysts to perform the required oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). It would be ideal to use a non-noble metal-based multifunctional catalyst for these reactions. Herein, a new type of porous carbon doped with Cu, N, S was prepared as a trifunctional catalyst for the ORR, OER, and HER from S-rich polyphenylene sulfide (PPS). By oxidatively treating the PPS, we critically prevented high-temperature melting of the precursor. Further, high-temperature pyrolysis using ammonia (NH3) desulfurized and introduced N into the carbon matrix, increasing structural defects and the surface area. By introducing copper during the pyrolysis, the tridoped (Cu, N, S) catalyst was successfully synthesized. The extremely large number of active sites and the local chemical environment enable excellent electrocatalytic performance and stability across ORR, OER, and HER at levels superior or comparable to noble metals. This catalyst was also used as the sole catalyst in Zn–air batteries and overall water splitting to demonstrate excellent performance. This synthesis method can pave the way toward new catalyst design and discovery, enabling more versatile and robust energy applications.

中文翻译:

用于可充电锌空气电池和自驱动水分解的富铜、氮、硫掺杂缺陷多孔碳的先进三功能电催化

燃料电池和水分解是有前途的可持续能源存储和转换系统,可以促进可再生资源的使用并减少对化石燃料的依赖。这些应用需要催化剂来执行所需的氧还原反应 (ORR)、析氧反应 (OER) 和析氢反应 (HER)。在这些反应中使用基于非贵金属的多功能催化剂将是理想的。在此,以富硫聚苯硫醚 (PPS) 为原料制备了一种新型的掺杂 Cu、N、S 的多孔碳,作为 ORR、OER 和 HER 的三功能催化剂。通过对 PPS 进行氧化处理,我们严格防止了前体的高温熔化。此外,使用氨(NH 3) 脱硫并将 N 引入碳基体,增加了结构缺陷和表面积。通过在热解过程中引入铜,成功合成了三掺杂(Cu,N,S)催化剂。极其大量的活性位点和局部化学环境使 ORR、OER 和 HER 的电催化性能和稳定性优于或可与贵金属相媲美。该催化剂还被用作锌-空气电池和整体水分解的唯一催化剂,以证明其优异的性能。这种合成方法可以为新的催化剂设计和发现铺平道路,从而实现更通用和更强大的能源应用。
更新日期:2021-10-04
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