Yang Yingju, Liu Jing, Xiong Bo
State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, China.
Nanoscale. 2022 May 19;14(19):7181-7188. doi: 10.1039/d2nr01259f.
Water splitting using renewable electricity provides a promising way for large-scale hydrogen production due to its zero-carbon emission properties. However, the development of highly efficient, low-cost and durable electrocatalysts remains an ongoing challenge in industrial applications. Herein, a strategy integrating vacancy engineering and metal doping was proposed to design and screen M@CuS catalysts with excellent catalytic activity density functional theory (DFT) calculations. TM single atoms anchored by the vacancy of the CuS surface show high stability, and serve as the active centers for water splitting. Ti@CuS and Co@CuS exhibit exceptional performance towards the hydrogen evolution reaction (HER). Ti@CuS and Co@CuS can achieve hydrogen adsorption free energies (Δ) of 0.01 eV and -0.03 eV, respectively. The HER process of Ti@CuS is controlled by the Heyrovsky mechanism. Co@CuS also shows superior catalytic activity towards the oxygen evolution reaction (OER), and presents a relatively lower OER overpotential of 0.41 V. Co@CuS serves as a promising candidate of bifunctional HER/OER electrocatalysts. This work not only provides highly efficient electrocatalysts for water splitting, but also inspires a novel concept to guide the extending design of catalysts in other catalysis fields.
利用可再生电力进行水分解因其零碳排放特性为大规模制氢提供了一条有前景的途径。然而，开发高效、低成本且耐用的电催化剂在工业应用中仍然是一个持续存在的挑战。在此，提出了一种将空位工程和金属掺杂相结合的策略，通过密度泛函理论（DFT）计算来设计和筛选具有优异催化活性的M@CuS催化剂。由CuS表面空位锚定的TM单原子具有高稳定性，并作为水分解的活性中心。Ti@CuS和Co@CuS对析氢反应（HER）表现出优异的性能。Ti@CuS和Co@CuS的氢吸附自由能（Δ）分别可达0.01 eV和 -0.03 eV。Ti@CuS的HER过程受Heyrovsky机制控制。Co@CuS对析氧反应（OER）也表现出优异的催化活性，其OER过电位相对较低，为0.41 V。Co@CuS是一种有前景的双功能HER/OER电催化剂候选材料。这项工作不仅为水分解提供了高效的电催化剂，还启发了一个新的概念，以指导其他催化领域催化剂的扩展设计。
