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Electronic structure modulation of molybdenum-iron double-atom catalyst for bifunctional oxygen electrochemistry
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-06-22 , DOI: 10.1016/j.cej.2022.137705
Omeshwari Yadorao Bisen , Ashok Kumar Yadav , B. Pavithra , Karuna Kar Nanda

Exploration of cost effective and high performance electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is becoming the paramount interest towards the emerging renewable energy technologies such as fuel cells, metal air-batteries and water electrolysers, etc. One of such catalysts is single atom catalyst that exhibits well defined active sites with very high atom utilization efficiency but selective mainly towards ORR. We demonstrate one-step synthesis of carbon-nitrogen (CN)-coordinated Fe-Mo double atom catalyst with high atom utilization efficiency towards both ORR and OER. The catalyst exhibits enhanced activity with lower overpotential associated with ORR and OER (ΔE= Ej=10(OER) - E1/2(ORR)) and better mass activity in comparison to that of Mo-N-C and Fe-N-C, even better than the state-of-the-art Pt/C and RuO2 catalysts for ORR and OER, respectively. This place the double atom catalysts in the series of non-precious metal based bifunctional catalysts for overall oxygen electrochemistry and is due to the electronic structure modification around the metal atoms induced by other neighbouring metal atom. The double atom Fe-Mo-N-C exhibits a remarkable and highly durable ORR performance with suppressed peroxide generation due to the muted outer sphere electron transfer mechanism in comparison with the commercially available state-of-the-art Pt/C electrocatalyst. Moreover, Fe-Mo-N-C shows remarkable enhanced overall oxygen electrochemistry at higher temperature (323 K - a temperature 25 K above the room temperature), widening its applicability. Overall, this work paves the way to design multi-atom catalysts towards multi-functional electrocatalytic activities.



中文翻译:

用于双功能氧电化学的钼铁双原子催化剂的电子结构调制

探索用于氧还原反应 (ORR) 和析氧反应 (OER) 的具有成本效益和高性能的电催化剂正成为新兴可再生能源技术(如燃料电池、金属空气电池和水电解槽等)的重中之重。这种催化剂是单原子催化剂,具有明确的活性位点,具有非常高的原子利用效率,但主要对 ORR 具有选择性。我们展示了一步合成碳-氮 (CN) 配位的 Fe-Mo 双原子催化剂,该催化剂对 ORR 和 OER 均具有高原子利用效率。催化剂表现出增强的活性,与 ORR 和 OER 相关的过电势较低 (ΔE= E j=10(OER) - E 1/2(ORR)) 和比 Mo-NC 和 Fe-NC 更好的质量活性,甚至优于最先进的 Pt/C 和 RuO 2分别是 ORR 和 OER 的催化剂。这将双原子催化剂置于用于整体氧电化学的一系列非贵金属基双功能催化剂中,这是由于其他相邻金属原子引起的金属原子周围的电子结构改变。与市售的最先进的 Pt/C 电催化剂相比,双原子 Fe-Mo-NC 表现出显着且高度耐用的 ORR 性能,由于外层电子转移机制的减弱,抑制了过氧化物的产生。此外,Fe-Mo-NC 在较高温度(323 K - 高于室温 25 K 的温度)下显示出显着增强的整体氧电化学,扩大了其适用性。全面的,

更新日期:2022-06-22
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