Enhancing hydrogen oxidation electrocatalysis of nickel-based catalyst by simultaneous chemical anchoring and electronic structure regulation
Enhancing hydrogen oxidation electrocatalysis of nickel-based catalyst by simultaneous chemical anchoring and electronic structure regulation
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同时化学锚定和电子结构调控增强镍基催化剂的氢氧化电催化
DOI：
10.1016/j.cej.2021.130654
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发表时间：
2021
影响因子：
15.1
通讯作者：
Xing Wei
中科院分区：
文献类型：
--
作者：
Wang Xiaoning;Li Xuejin;Cai Tonghui;Cui Yongpeng;Kong Dongqing;Xu Jing;Hu Haoyu;Wang Yesheng;Hu Han;Gao Xiuli;Li Yanpeng;Xue Qingzhong;Yan Zifeng;Zhao Lianming;Xing Wei
设计碱性介质中氢氧化反应(HOR)的电催化剂是关键，但也是具有挑战性的。在所有现有的电催化剂中，镍基材料被认为是最有潜力的无贵金属电催化剂。然而，他们仍然面临着活跃度低、稳定性差等严重问题。本文提出了一种化学锚定和电子结构调节相结合的协同策略，使镍基HOR催化剂既具有高的电催化活性，又具有较高的稳定性。N掺杂纳米石墨(N-GFS)载体具有丰富的N锚定中心，可以稳定负载镍基活性物种，使催化剂具有良好的稳定性。同时，在活性Ni3N/Ni中合理设计的异质结构可以触发电子在异质界面上的转移，从而优化反应中间产物的结合能，从而加速Volmer反应。由于设计合理，Ni3N/Ni/N-GFS具有良好的质量活性(在50 mV的过电位下为42.7A GNI-1)和稳定性(连续运行24小时以上)。此外，Ni3N/Ni异质结构比单独的Ni或Ni3N具有更好的电催化性能。理论模拟验证了实验结果的合理性，表明异质结构有效地削弱了氢的吸附，优化了羟基的吸附，降低了水形成反应的势垒。
Designing electrocatalysts for hydrogen oxidation reaction (HOR) in alkaline media is crucial but challenging. Among all available electrocatalysts, Ni-based materials are recognized as the most potential precious-metal-free electrocatalysts for HOR. However, they still suffer from serious problems including low activity and poor stability. In this work, a synergistic chemical anchoring and electronic structure regulation strategy is proposed to gain both high electrocatalytic activity and stability for Ni-based HOR catalyst. N-doped graphite nanoflakes (N-GFs) support with abundant N anchoring sites can stabilize the loading of Ni-based active species, giving rise to an excellent stability of the catalyst. Meanwhile, the rationally designed heterostructure in the active Ni3N/Ni can trigger the electron transfer across the heterointerface, which optimizes the binding energy of the reaction intermediates, resulting in an accelerated the Volmer reaction. Benefited from the rational design, Ni3N/Ni/N-GFs exhibits excellent mass activity (42.7 A gNi-1at the overpotential of 50 mV) and stability (more than 24 h continuous operation). Moreover, the Ni3N/Ni heterostructure performs better in HOR electrocatalysis than individual Ni or Ni3N. These experimental results are rationalized by the theoretical simulations, which demonstrate that the heterostructure effectively weakens the hydrogen adsorption, optimizes the hydroxyl adsorption, and decreases the water formation reaction barrier.
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影响因子：
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