Designing efficient, economical bifunctional electrocatalysts for overall water splitting is important and challenging. This paper demonstrates a cobalt-based electrocatalyst modified with stable ceria (CeO₂) and adjustable copper metal/oxide (Cu/CuO) to regulate electrochemical reconfigurations during the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Theoretical calculations reveal that CeO₂ substantially impacts the electronic configuration and D-band center of catalysts. Surprisingly, CeO₂ moves the D-band center of cobalt oxyhydroxide closer to the Fermi level but shifts the D-band center of cobalt hydroxide away from the Fermi level. Therefore, CeO₂ optimizes the adsorption energy of the intermediates and boosts the OER activity, while reducing the ability of absorbed hydrogen atoms to bond with the catalyst and enhancing the electron-donor performance of the catalyst in the HER. Furthermore, the presence of Cu/CuO dramatically improves the catalytic activity. Hence, the utilization of CeO₂ and CuO/Cu in cobalt-based nanosheet arrays enhances catalytic efficiency in overall water splitting. The overpotentials are only 94 mV and 246 mV (@10 mA cm⁻²) for the HER and OER, respectively, superior to those of pure cobalt-based catalysts. This study presents an innovative approach to developing efficient overall water splitting catalysts and offers insights into future developments in this field.

中文翻译：

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通过稳定的铈和可调节的铜金属/氧化物调节催化剂的电子结构，以实现高效的整体水分解


为整体分解水设计高效、经济的双功能电催化剂非常重要且具有挑战性。本文展示了一种用稳定铈 （CeO₂） 和可调节铜金属/氧化物 （Cu/CuO） 改性的钴基电催化剂，用于调节析氢反应 （HER） 和析氧反应 （OER） 过程中的电化学重构。理论计算表明，CeO₂ 对催化剂的电子构型和 D 波段中心有很大影响。令人惊讶的是，CeO₂ 使氢氧化钴的 D 带中心更接近费米能级，但将氢氧化钴的 D 带中心从费米能级移开。因此，CeO₂ 优化了中间体的吸附能并提高了 OER 活性，同时降低了吸收的氢原子与催化剂结合的能力，并增强了催化剂在 HER 中的电子供体性能。此外，Cu/CuO 的存在显着提高了催化活性。因此，在钴基纳米片阵列中利用 CeO₂ 和 CuO/Cu 可以提高整体水分解的催化效率。HER 和 OER 的过电位分别仅为 94 mV 和 246 mV （@10 mA ^cm-2），优于纯钴基催化剂的过电位。本研究提出了一种开发高效整体分解水催化剂的创新方法，并为该领域的未来发展提供了见解。