Institutes of Physical Science and Information Technology, School of Chemical and Chemistry Science, Anhui University, Hefei, Anhui 230601, China.
The First Affiliated Hospital of Anhui Medical University, Anhui Medical University, Hefei, Anhui 230022, China.
Inorg Chem. 2023 Jul 3;62(26):10490-10496. doi: 10.1021/acs.inorgchem.3c01617. Epub 2023 Jun 21.
Realizing a highly efficient oxygen evolution reaction (OER) process is of great significance for hydrogen energy development. The main challenge still lies in fabricating superior electrocatalysts with favorable performance. Constructing electrocatalysts with ingenious lattice modifications is a considerable way for the rational design of highly active catalytic centers. Here, theoretical calculations predict that the lattice incorporation of Se atoms can effectively enhance the reaction activity of OER with a decreased energy barrier for the rate-determining step. To obtain the corresponding desired electrocatalyst, the optimized lattice Se-modified CoOOH, with the ideal OER performance of low overpotential and stability, was delicately designed and fabricated by the electrochemical activation of the CoSe precatalyst. X-ray absorption spectroscopy (XAS) demonstrates that lattice incorporation is more likely to be generated in CoSe compared to CoSe and CoO precatalysts, which promoted the subsequent OER process. This work clarified the correlation between the precatalyst and the lattice-modified final catalyst in connection with electrochemical reconstruction.
实现高效的氧气析出反应（OER）过程对于氢能的发展具有重要意义。主要的挑战仍然在于构建具有优异性能的卓越电催化剂。通过巧妙的晶格修饰来构建电催化剂是合理设计高活性催化中心的一种重要方法。在这里，理论计算预测，硒原子的晶格掺入可以有效地增强 OER 的反应活性，降低速率决定步骤的能量障碍。为了获得相应的理想电催化剂，通过 CoSe 前催化剂的电化学活化，精心设计和制备了优化晶格硒修饰的 CoOOH，其具有低过电位和稳定性的理想 OER 性能。X 射线吸收光谱（XAS）表明，与 CoSe 和 CoO 前催化剂相比，晶格掺入在 CoSe 中更有可能发生，这促进了随后的 OER 过程。这项工作阐明了与电化学重构相关的前驱体和晶格修饰最终催化剂之间的相关性。
