Jang Yeju, Kim Hoyoung, Park Dongmin, Han Sunghoon, Jun Hyunwoo, Park Jinkyu, Kim Seongbeen, Jung Yousung, Choi Chang Hyuck, Jang Jong Hyun, Lee Seonggyu, Lee Jinwoo
Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Republic of Korea.
Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang, 37637, Republic of Korea.
Small. 2025 Apr;21(17):e2411374. doi: 10.1002/smll.202411374. Epub 2025 Mar 28.
The primary hurdle faced in the practical application of proton exchange membrane water electrolyzer (PEMWE) involves improving the intrinsic kinetic activity of oxygen evolution reaction (OER) electrocatalysts while concurrently enhancing their durability. Although electrocatalysts based on lattice oxygen-mediated mechanism (LOM) have the potential to significantly enhance the activity in OER without being restricted by scaling relationships, they are neglected in acidic electrolytes due to limited durability. In this study, an innovative approach is presented to simultaneously promote the activation of lattice oxygen and improve the durability of LOM-based OER electrocatalysts by incorporating d metal ions into the RuO electrocatalyst. Leveraging the unique electronic properties of the d metal ion, the O 2p band center and Ru-O covalency of the electrocatalyst are successfully engineered, resulting in the change in OER mechanism. Furthermore, in a single cell of PEMWE, the LOM-based electrocatalyst demonstrates outstanding performance, achieving 3.0 A cm at 1.81 V and maintaining durability for 100 h at 200 mA cm, surpassing commercial RuO. This innovative strategy challenges the traditional viewpoint that suppressing lattice oxygen activation in OER is essential for enhancing PEMWE durability, offering new perspectives for the development of OER electrocatalysts in acidic electrolytes.
质子交换膜水电解槽(PEMWE)实际应用中面临的主要障碍包括提高析氧反应(OER)电催化剂的本征动力学活性,同时提高其耐久性。尽管基于晶格氧介导机制(LOM)的电催化剂有潜力在不受比例关系限制的情况下显著提高OER活性,但由于耐久性有限,它们在酸性电解质中被忽视。在本研究中,提出了一种创新方法,通过将d金属离子引入RuO电催化剂中,同时促进晶格氧的活化并提高基于LOM的OER电催化剂的耐久性。利用d金属离子独特的电子性质,成功调控了电催化剂的O 2p带中心和Ru - O共价性,导致OER机制发生变化。此外,在PEMWE单电池中,基于LOM的电催化剂表现出优异的性能,在1.81 V下达到3.0 A cm²,在200 mA cm²下保持100 h的耐久性,超过了商业RuO。这种创新策略挑战了传统观点,即抑制OER中的晶格氧活化对于提高PEMWE耐久性至关重要,为酸性电解质中OER电催化剂的开发提供了新的视角。