Oxygen Evolution and Reduction on Two-Dimensional Transition Metal Dichalcogenides
Oxygen Evolution and Reduction on Two-Dimensional Transition Metal Dichalcogenides
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DOI：
10.1021/acs.jpclett.1c03431
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发表时间：
2021-12-27
影响因子：
5.7
通讯作者：
Andreussi, Oliviero
中科院分区：
文献类型：
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作者：
Karmodak, Naiwrit;Bursi, Luca;Andreussi, Oliviero
为了寻找用于水氧化和O-2还原的良好的电催化剂，由无毒和富含稀土的元素组成，系统地筛选了二维(2D)过渡金属二卤化物(TMDCs)。为了确定具有本质活性并能充分利用2D催化剂的高比表面积的化合物，本研究重点研究了2D TMDCs在2H、1T和1T‘相的理想基面的性质。通过基于第一性原理的模拟和连续体嵌入模型来解释电化学环境的存在，对计算数据库中提出的200多种材料进行了研究。选择了在酸性条件下氧析出和还原反应(OER和ORR)低于0.5V，以及在电化学环境中具有较高抗降解稳定性的过电位最佳候选者。对于OER，设计的工作流程确定了一种活性和热力学稳定的材料，以及七种在氧化电位和酸性pH下亚稳定的材料。另一方面，对于ORR，我们发现了20种过电位小于0.5V的材料。在这些化合物中，已有6种双功能材料被实验报道，其中1T-NbTe2和1T‘-MoTe2分别是性能最好的OER和ORR催化剂。
Motivated by the need to find good electrocatalysts for water oxidation and O-2 reduction, composed of nontoxic and earth-abundant elements, a systematic screening of two-dimensional ( 2D) transition metal dichalcogenides (TMDCs) is performed. To identify compounds that are intrinsically active and can fully take advantage of the high surface area of 2D catalysts, this study focuses on the properties of the ideal basal planes of 2D TMDCs, in the 2H, 1T, and 1T' phases. Over two hundred materials proposed in computational databases are studied by means of first-principles-based simulations coupled with continuum embedding models to account for the presence of electrochemical environments. The best candidates with overpotentials for the oxygen evolution and reduction reactions (OER and ORR) lower than 0.5 V under acidic conditions and higher stability against degradation in electrochemical environments are selected. For OER, the designed workflow identifies one active and thermodynamically stable material, and seven materials that are metastable at the oxidative potentials and acidic pH. On the other hand, for ORR, we identify 20 materials with overpotentials less than 0.5 V. Among these compounds, six bifunctional materials have been experimentally reported, with 1T-NbTe2 and 1T'-MoTe2 being the best performing catalysts for OER and ORR, respectively.