Yan Tingyu, Li Xinyi, Wang Zhongxu, Cai Qinghai, Zhao Jingxiang
College of Chemistry and Chemical Engineering, Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, Harbin Normal University, Harbin 150025, Heilongjiang, China.
College of Chemistry and Chemical Engineering, Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, Harbin Normal University, Harbin 150025, Heilongjiang, China.
J Colloid Interface Sci. 2023 Nov;649:1-9. doi: 10.1016/j.jcis.2023.06.066. Epub 2023 Jun 14.
Exploring high-efficiency electrocatalysts to boost the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is pivotal to the large-scale applications for clean and renewable energy technologies, such as fuel cells, water splitting, and metal-air batteries. Herein, by means of density functional theory (DFT) computations, we proposed a strategy to modulate the catalytic activity of transition metal-nitrogen-carbon catalysts through their interface engineering with graphdiyne (TMNC/GDY). Our results revealed that these hybrid structures exhibit good stability and excellent electrical conductivity. Especially, CoNC/GDY was identified as a promising bifunctional catalyst for ORR/OER with rather low overpotentials in acidic conditions according to the constant-potential energy analysis. Moreover, the volcano plots were established to describe the activity trend of the ORR/OER on TMNC/GDY using the adsorption strength of the oxygenated intermediates. Remarkably, the d-band center and charge transfer of the TM active sites can be utilized to correlate the ORR/OER catalytic activity and their electronic properties. Our findings not only suggested an ideal bifunctional oxygen electrocatalyst, but also provided a useful strategy to obtain highly efficient catalysts by interface engineering of two-dimensional heterostructures.
探索高效电催化剂以促进氧还原反应（ORR）和析氧反应（OER）对于燃料电池、水分解和金属空气电池等清洁和可再生能源技术的大规模应用至关重要。在此，通过密度泛函理论（DFT）计算，我们提出了一种通过与石墨二炔（TMNC/GDY）进行界面工程来调节过渡金属-氮-碳催化剂催化活性的策略。我们的结果表明，这些杂化结构具有良好的稳定性和优异的导电性。特别是，根据恒电位能量分析，CoNC/GDY被确定为一种在酸性条件下具有相当低过电位的有前途的ORR/OER双功能催化剂。此外，利用含氧中间体的吸附强度建立了火山图来描述TMNC/GDY上ORR/OER的活性趋势。值得注意的是，TM活性位点的d带中心和电荷转移可用于关联ORR/OER催化活性及其电子性质。我们的发现不仅提出了一种理想的双功能氧电催化剂，还提供了一种通过二维异质结构的界面工程获得高效催化剂的有用策略。
