Modulating the Electronic Structure on Cobalt Sites by Compatible Heterojunction Fabrication for Greatly Improved Overall Water/Seawater Electrolysis,ACS Sustainable Chemistry & Engineering

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Modulating the Electronic Structure on Cobalt Sites by Compatible Heterojunction Fabrication for Greatly Improved Overall Water/Seawater Electrolysis
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2022-07-19 , DOI: 10.1021/acssuschemeng.2c02571
Jianpeng Sun ₁ , Jiao Li ₁ , Zizhen Li ₁ , Chunhu Li ₁ , Guangmin Ren ₁ , Zisheng Zhang ₂ , Xiangchao Meng ₁

Affiliation

Optimizing the electronic structure on an electrocatalyst is of primary importance to enhance the electrocatalytic activity in water electrolysis. Herein, motivated by theoretical predictions of the excellent electronic properties and suitable Gibbs free energy of active intermediates (H* for the hydrogen evolution reaction and OH* for the oxygen evolution reaction) on cobalt (Co) sites at the heterointerface between CoSe and MoSe₂, a new hierarchical bimetal selenide microsphere electrocatalyst (CoSe/MoSe₂) with good interfacial compatibility was designed and successfully synthesized. The as-prepared CoSe/MoSe₂ exhibited excellent catalytic performance. In the meantime, it only needed 1.63, 1.69, and 1.77 V in 1.0 M KOH, simulated seawater, and alkaline seawater for overall water splitting, respectively. This was attributed to the well-matched interface between CoSe and MoSe₂ that effectively disperses electrons on Co atoms and adjusts the d-band center on the Co atom, thus regulating the free energy of H*/OH* on Co sites. This work provided insights into the rational design and construction of efficient electrocatalysts with interfacial compatibility for water/seawater electrolysis.

中文翻译：

通过兼容异质结制造调制钴位点上的电子结构，以大大改善整体水/海水电解

优化电催化剂上的电子结构对于提高水电解中的电催化活性至关重要。在此，基于对 CoSe 和 MoSe ₂异质界面处钴 (Co) 位点上活性中间体（析氢反应的 H* 和析氧反应的 OH*）的优异电子特性和合适的吉布斯自由能的理论预测的启发等，设计并成功合成了一种具有良好界面相容性的新型分级双金属硒化物微球电催化剂（CoSe/MoSe _{2 ）。}所制备的 CoSe/MoSe ₂表现出优异的催化性能。同时，在 1.0 M KOH、模拟海水和碱性海水中，整体水分解仅需 1.63、1.69 和 1.77 V。这归因于 CoSe 和 MoSe ₂之间良好匹配的界面，有效地分散了 Co 原子上的电子并调整了 Co 原子上的 d 带中心，从而调节了 Co 位点上 H*/OH* 的自由能。这项工作为合理设计和构建具有水/海水电解界面相容性的高效电催化剂提供了见解。

更新日期：2022-07-19

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