Rapid Two Surface Reconstructions of Ni/MnO Heterojunction for Superior Urea Electrolysis,ACS Energy Letters

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Rapid Two Surface Reconstructions of Ni/MnO Heterojunction for Superior Urea Electrolysis
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-09-03 , DOI: 10.1021/acsenergylett.4c01938
Kaili Wang ₁ , Maojun Pei ₁ , Yankang Shuai ₁ , Yao Liu ₁ , Shuqi Deng _{1,

2} , Zewen Zhuang ₁ , Kaian Sun ₁ , Wei Yan ₁ , Jiujun Zhang _{1,

2}

Affiliation

Urea oxidation reaction (UOR) emerges as a promising alternative anodic half-reaction to oxygen evolution reaction (OER) in an electrochemical CO₂ reduction reaction (ECRR) system. Herein, a Ni/MnO heterojunction with extraordinary UOR activity is synthesized on Ni foam. Ex situ/in situ characterization and theoretical calculation reveal that the outstanding UOR performance of Ni/MnO catalyst can be ascribed to two successive surface reconstructions. In the first and second surface reconstructions, Ni(OH)₂/MnOOH and NiOOH/MnOOH heterojunctions are formed on the catalyst surface, and Mn and Ni sites serve as the active sites, respectively. The heterojunctions formed can enhance UOR activity by reducing the surface reconstruction potential and optimizing the adsorption energy of intermediates through electronic structure modulation and d-band center regulation. When employed as the UOR anode in the CO₂ electrolyzer, it requires 375 mV less voltage at 10 mA cm^–2 than the OER, revealing the great potential of applying such Ni/MnO catalyst as the anodic UOR in an ECRR system for carbon neutrality.

中文翻译：

Ni/MnO 异质结的快速两个表面重建以实现优异的尿素电解

尿素氧化反应（UOR）作为电化学CO ₂还原反应（ECRR）系统中析氧反应（OER）的一种有前途的替代阳极半反应而出现。在此，在泡沫镍上合成了具有非凡 UOR 活性的 Ni/MnO 异质结。非原位/原位表征和理论计算表明，Ni/MnO 催化剂出色的 UOR 性能可归因于两次连续的表面重构。在第一和第二表面重构中，在催化剂表面上形成Ni(OH) ₂ /MnOOH和NiOOH/MnOOH异质结，并且Mn和Ni位点分别作为活性位点。形成的异质结可以通过降低表面重构势并通过电子结构调制和d带中心调节优化中间体的吸附能来增强UOR活性。当用作CO ₂电解槽中的UOR阳极时，在10 mA cm ^–2下所需的电压比OER低375 mV，揭示了在ECRR系统中应用这种Ni/MnO催化剂作为阳极UOR以实现碳中和的巨大潜力。

更新日期：2024-09-03

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