在 3D Co3O4/Co3S4 异质结构上进行氧和硫双空位工程以提高整体水分解活性,Green Chemistry

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在 3D Co3O4/Co3S4 异质结构上进行氧和硫双空位工程以提高整体水分解活性
Green Chemistry ( IF 9.3 ) Pub Date : 2022-10-25 , DOI: 10.1039/d2gc03315a
Qing Wang ₁ , Hui Xu ₁ , Xingyue Qian ₁ , Guangyu He ₁ , Haiqun Chen ₁

Affiliation

电化学水分解是实现工业制氢的一种高效方法。然而，电催化剂存在效率低和能耗高的问题。在此，本文提出了一种新型空位工程策略，用于制备具有丰富 O 和 S 双空位的 Ni 泡沫负载 Co ₃ O ₄ /Co ₃ S _{4异质结（DV-Co}₃ O ₄ /Co ₃ S ₄@NF) 被提议。氧空位优化了尖晶石表面的电子分布，降低了吸附 OH* 自由基的能垒。同时，由于尖晶石暴露的活性边缘，硫空位为 H* 吸附提供了高活性位点，从而提高了析氢反应 (HER) 的性能。受益于 O 和 S 双空位的协同效应，DV-Co ₃ O ₄ /Co ₃ S ₄ @NF 对 OER 和 HER 均表现出出色的电催化活性，在 10 mA cm ^-2下具有 99 和 26 mV 的小过电势，分别。此外，作为全水分解（OWS）的双功能电催化剂，DV-Co ₃ O₄ /Co₃ S₄ @NF 仅需1.52 V的低电池电压即可获得20 mA cm^-2的大电流密度，并且电池电压在200小时以上基本保持不变。更重要的是，将同时作为阳极和阴极的DV-Co₃ O₄ /Co₃ S₄ @NF组装成一个电池，由单个自组装的1.5 V AA电池装置供电，非常适用于工业制氢的需求。该工作为电催化剂的发展和机理探索提供了理论和实践指导。

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Oxygen and sulfur dual vacancy engineering on a 3D Co3O4/Co3S4 heterostructure to improve overall water splitting activity

Electrochemical water splitting is a highly efficient approach for realizing industrial hydrogen production. Nonetheless, electrocatalysts suffer from low efficiency and high energy consumption. Herein, a novel vacancy engineering strategy for the fabrication of a Ni foam-supported Co₃O₄/Co₃S₄ heterojunction with rich O and S dual vacancies (DV-Co₃O₄/Co₃S₄@NF) is proposed. The oxygen vacancy optimizes the electron distribution on the spinel surface and reduces the energy barrier for the adsorption of OH* free radicals. Meanwhile, the sulfur vacancy provides highly active sites for H* adsorption, thanks to the exposed active edge of spinel, leading to enhanced hydrogen evolution reaction (HER) performance. Benefiting from the synergistic effect of O and S dual vacancies, the DV-Co₃O₄/Co₃S₄@NF exhibits outstanding electrocatalytic activity for both the OER and HER with small overpotentials of 99 and 26 mV at 10 mA cm⁻², respectively. Moreover, as the bifunctional electrocatalyst for overall water splitting (OWS), the DV-Co₃O₄/Co₃S₄@NF requires only a low cell voltage of 1.52 V to obtain a large current density of 20 mA cm⁻², and the cell voltage remains basically unchanged for more than 200 h. More importantly, the DV-Co₃O₄/Co₃S₄@NF acting as both the anode and the cathode was assembled into a cell, powered by a single self-assembled 1.5 V AA battery device, which is very suitable for the needs of industrial hydrogen production. This work provides theoretical and pragmatic guidelines for the development and mechanism exploration of electrocatalysts.

更新日期：2022-10-25

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