High-Valence Nickel Single-Atom Catalysts Coordinated to Oxygen Sites for Extraordinarily Activating Oxygen Evolution Reaction.,Advanced Science

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High-Valence Nickel Single-Atom Catalysts Coordinated to Oxygen Sites for Extraordinarily Activating Oxygen Evolution Reaction.
Advanced Science ( IF 14.3 ) Pub Date : 2020-01-20 , DOI: 10.1002/advs.201903089
Yaguang Li _{1,

2} , Zhong-Shuai Wu ₁ , Pengfei Lu ₁ , Xiao Wang _{1,

3} , Wei Liu ₁ , Zhibo Liu ₄ , Jingyuan Ma ₅ , Wencai Ren ₄ , Zheng Jiang ₅ , Xinhe Bao _{1,

6}

Affiliation

Single-atom catalysts (SACs) are efficient for maximizing electrocatalytic activity, but have unsatisfactory activity for the oxygen evolution reaction (OER). Herein, the NaCl template synthesis of individual nickel (Ni) SACs is reported, bonded to oxygen sites on graphene-like carbon (denoted as Ni-O-G SACs) with superior activity and stability for OER. A variety of characterizations unveil that the Ni-O-G SACs present 3D porous framework constructed by ultrathin graphene sheets, single Ni atoms, coordinating nickel atoms to oxygen. Consequently, the catalysts are active and robust for OER with extremely low overpotential of 224 mV at current density of 10 mA cm-2, 42 mV dec-1 Tafel slope, oxygen production turn over frequency of 1.44 S-1 at 300 mV, and long-term durability without significant degradation for 50 h at exceptionally high current of 115 mA cm-1, outperforming the state-of-the-art OER SACs. A theoretical simulation further reveals that the bonding between single nickel and oxygen sites results in the extraordinary boosting of OER performance of Ni-O-G SACs. Therefore, this work opens numerous opportunities for creating unconventional SACs via metal-oxygen bonding.

中文翻译：

高价镍单原子催化剂与氧位点配位，可显着激活析氧反应。

单原子催化剂（SAC）可以有效地最大化电催化活性，但对于析氧反应（OER）的活性却不能令人满意。在此，报道了单个镍 (Ni) SAC 的 NaCl 模板合成，该镍 (Ni) SAC 与类石墨烯碳（表示为 Ni-OG SAC）上的氧位点键合，具有优异的 OER 活性和稳定性。各种表征表明，Ni-OG SAC 呈现出由超薄石墨烯片、单个镍原子、镍原子与氧配位构成的 3D 多孔框架。因此，催化剂对于 OER 具有活性和鲁棒性，在 10 mA cm-2 电流密度下具有 224 mV 的极低过电势，42 mV dec-1 Tafel 斜率，在 300 mV 下产氧转换频率为 1.44 S-1，并且在 115 mA cm-1 的极高电流下 50 小时内具有长期耐用性，不会出现明显退化，优于最先进的 OER SAC。理论模拟进一步表明，单个镍和氧位点之间的键合导致 Ni-OG SAC 的 OER 性能显着提升。因此，这项工作为通过金属-氧键合创建非常规 SAC 提供了许多机会。

更新日期：2020-01-21

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