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Atomically Dispersed Fe/N4 and Ni/N4 Sites on Separate-Sides of Porous Carbon Nanosheets with Janus Structure for Selective Oxygen Electrocatalysis
Small ( IF 13.0 ) Pub Date : 2023-03-16 , DOI: 10.1002/smll.202300289 Xinghuan Liu 1 , Fei Zhao 2 , Long Jiao 3 , Tianwen Fang 1 , Zeyu Zhao 1 , Xiangfei Xiao 1 , Danya Li 1 , Ke Yi 1 , Rongjie Wang 1 , Xin Jia 1
Small ( IF 13.0 ) Pub Date : 2023-03-16 , DOI: 10.1002/smll.202300289 Xinghuan Liu 1 , Fei Zhao 2 , Long Jiao 3 , Tianwen Fang 1 , Zeyu Zhao 1 , Xiangfei Xiao 1 , Danya Li 1 , Ke Yi 1 , Rongjie Wang 1 , Xin Jia 1
Affiliation
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Dual single atoms catalysts have promising application in bifunctional electrocatalysis due to their synergistic effect. However, how to balance the competition between rate-limiting steps (RDSs) of reversible oxygen reduction and oxygen evolution reaction (OER) and fully expose the active centers by reasonable structure design remain enormous challenges. Herein, Fe/N4 and Ni/N4 sites separated on different sides of the carbon nanosheets with Janus structure (FeNijns/NC) is synthesized by layer-by-layer assembly method. Experiments and calculations reveal that the side of Fe/N4 is beneficial to oxygen reduction reaction (ORR) and the Ni/N4 side is preferred to OER. Such Janus structure can take full advantage of two separate-sides of carbon nanosheets and balance the competition of RDSs during ORR and OER. FeNijns/NC possesses superior ORR and OER activity with ORR half-wave potential of 0.92 V and OER overpotential of 440 mV at J = 10 mA cm−2. Benefiting from the excellent bifunctional activities, FeNijns/NC assembled aqueous Zn–air battery (ZAB) demonstrates better maximum power density, and long-term stability (140 h) than Pt/C+RuO2 catalyst. It also reveals superior flexibility and stability in solid-state ZAB. This work brings a novel perspective for rational design and understanding of the catalytic mechanisms of dual single atom catalysts.
中文翻译：
具有Janus结构的多孔碳纳米片两侧原子分散的Fe/N4和Ni/N4位点用于选择性氧电催化
双单原子催化剂由于其协同效应在双功能电催化中具有广阔的应用前景。然而，如何平衡可逆氧还原反应的限速步骤（RDS）与析氧反应（OER）之间的竞争，并通过合理的结构设计充分暴露活性中心仍然是巨大的挑战。在此，通过层层组装方法合成了具有Janus结构的碳纳米片(FeNi jns /NC)的不同侧面上分离的Fe/N 4和Ni/N 4位点。实验和计算表明Fe/N 4一侧有利于氧还原反应(ORR)，而Ni/N 4一侧有利于氧还原反应(ORR)。侧面优于 OER。这种Janus结构可以充分利用碳纳米片的两个独立面，平衡ORR和OER过程中RDS的竞争。FeNi jns /NC具有优异的ORR和OER活性，在J = 10 mA cm -2时ORR半波电位为0.92 V，OER过电位为440 mV 。得益于优异的双功能活性，FeNi jns /NC组装的水性锌空气电池（ZAB）表现出比Pt/C+RuO 2更好的最大功率密度和长期稳定性（140小时）催化剂。它还揭示了固态 ZAB 卓越的灵活性和稳定性。这项工作为合理设计和理解双单原子催化剂的催化机理带来了新的视角。
更新日期：2023-03-16
中文翻译：
具有Janus结构的多孔碳纳米片两侧原子分散的Fe/N4和Ni/N4位点用于选择性氧电催化
双单原子催化剂由于其协同效应在双功能电催化中具有广阔的应用前景。然而，如何平衡可逆氧还原反应的限速步骤（RDS）与析氧反应（OER）之间的竞争，并通过合理的结构设计充分暴露活性中心仍然是巨大的挑战。在此，通过层层组装方法合成了具有Janus结构的碳纳米片(FeNi jns /NC)的不同侧面上分离的Fe/N 4和Ni/N 4位点。实验和计算表明Fe/N 4一侧有利于氧还原反应(ORR)，而Ni/N 4一侧有利于氧还原反应(ORR)。侧面优于 OER。这种Janus结构可以充分利用碳纳米片的两个独立面，平衡ORR和OER过程中RDS的竞争。FeNi jns /NC具有优异的ORR和OER活性，在J = 10 mA cm -2时ORR半波电位为0.92 V，OER过电位为440 mV 。得益于优异的双功能活性，FeNi jns /NC组装的水性锌空气电池（ZAB）表现出比Pt/C+RuO 2更好的最大功率密度和长期稳定性（140小时）催化剂。它还揭示了固态 ZAB 卓越的灵活性和稳定性。这项工作为合理设计和理解双单原子催化剂的催化机理带来了新的视角。
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