Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, Anhui 241002, P. R. China.
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, P. R. China.
Inorg Chem. 2023 Jul 17;62(28):11233-11239. doi: 10.1021/acs.inorgchem.3c01485. Epub 2023 Jul 6.
Developing economical, efficient, and durable oxygen evolution catalysts is crucial for achieving sustainable energy conversion and storage. Ruddlesden-Popper-type perovskite oxides are at the forefront of oxygen evolution reaction (OER) research. However, their activity and stability are far from satisfactory. Therefore, we emphasize the paradigm shift in designing efficient perovskite-type OER catalysts through anion defect engineering. The Cl anion-doped ABO-type perovskite oxides, SrLaCoOCl (SLCOCl), were employed as highly efficient OER catalysts, wherein Cl could tune the electronic structure of SrLaCoO (SLCO) to enhance the OER activity effectively. Especially, SLCOCl demonstrates significantly enhanced OER activity, and the overpotential is only 370 mV at 10 mA·cm, which is significantly better than that of SLCO (510 mV). As confirmed by experience results and density functional theory (DFT) calculation, due to the doping of Cl, obviously increasing the ratio of Co/Co, more abundant oxygen vacancies (O/O) are generated, and the electrical conductivity is increased, which together promote the improvement of OER activity.
开发经济、高效、耐用的氧气析出催化剂对于实现可持续的能量转换和存储至关重要。钙钛矿氧化物中的 Ruddlesden-Popper 型处于氧气析出反应 (OER) 研究的前沿。然而，它们的活性和稳定性远不能令人满意。因此，我们强调通过阴离子缺陷工程设计高效钙钛矿型 OER 催化剂的范式转变。采用 Cl 阴离子掺杂的 ABO 型钙钛矿氧化物 SrLaCoOCl (SLCOCl) 作为高效 OER 催化剂，其中 Cl 可以调节 SrLaCoO (SLCO) 的电子结构，从而有效地提高 OER 活性。特别是，SLCOCl 表现出显著增强的 OER 活性，在 10 mA·cm 时的过电势仅为 370 mV，明显优于 SLCO（510 mV）。经验结果和密度泛函理论 (DFT) 计算证实，由于 Cl 的掺杂，Co/Co 的比例明显增加，产生了更多丰富的氧空位 (O/O)，电导率增加，共同促进了 OER 活性的提高。
