Zhu Yinlong, Lin Qian, Hu Zhiwei, Chen Yubo, Yin Yichun, Tahini Hassan A, Lin Hong-Ji, Chen Chien-Te, Zhang Xiwang, Shao Zongping, Wang Huanting
Department of Chemical Engineering, Monash University, Clayton, Victoria, 3800, Australia.
Max Planck Institute for Chemical Physics of Solids, Nothnitzer Strasse 40, Dresden, 01187, Germany.
Small. 2020 May;16(20):e2001204. doi: 10.1002/smll.202001204. Epub 2020 Apr 20.
The oxygen evolution reaction (OER) is pivotal in multiple gas-involved energy conversion technologies, such as water splitting, rechargeable metal-air batteries, and CO /N electrolysis. Emerging anion-redox chemistry provides exciting opportunities for boosting catalytic activity, and thus mastering lattice-oxygen activation of metal oxides and identifying the origins are crucial for the development of advanced catalysts. Here, a strategy to activate surface lattice-oxygen sites for OER catalysis via constructing a Ruddlesden-Popper/perovskite hybrid, which is prepared by a facile one-pot self-assembly method, is developed. As a proof-of-concept, the unique hybrid catalyst (RP/P-LSCF) consists of a dominated Ruddlesden-Popper phase LaSr Co Fe O (RP-LSCF) and second perovskite phase La Sr Co Fe O (P-LSCF), displaying exceptional OER activity. The RP/P-LSCF achieves 10 mA cm at a low overpotential of only 324 mV in 0.1 m KOH, surpassing the benchmark RuO and various state-of-the-art metal oxides ever reported for OER, while showing significantly higher activity and stability than single RP-LSCF oxide. The high catalytic performance for RP/P-LSCF is attributed to the strong metal-oxygen covalency and high oxygen-ion diffusion rate resulting from the phase mixture, which likely triggers the surface lattice-oxygen activation to participate in OER. The success of Ruddlesden-Popper/perovskite hybrid construction creates a new direction to design advanced catalysts for various energy applications.
析氧反应（OER）在多种涉及气体的能量转换技术中至关重要，如水电解、可充电金属空气电池以及CO₂/ N₂电解。新兴的阴离子氧化还原化学为提高催化活性提供了令人兴奋的机遇，因此掌握金属氧化物的晶格氧活化并确定其来源对于先进催化剂的开发至关重要。在此，开发了一种通过构建Ruddlesden-Popper/钙钛矿杂化物来激活表面晶格氧位点以用于OER催化的策略，该杂化物通过简便的一锅自组装方法制备。作为概念验证，独特的杂化催化剂（RP/P-LSCF）由占主导的Ruddlesden-Popper相LaSrCoFeO（RP-LSCF）和第二钙钛矿相LaSrCoFeO（P-LSCF）组成，展现出卓越的OER活性。RP/P-LSCF在0. m KOH中仅324 mV的低过电位下即可达到10 mA cm⁻²，超过了基准RuO₂以及此前报道的各种用于OER的先进金属氧化物，同时比单一的RP-LSCF氧化物表现出显著更高的活性和稳定性。RP/P-LSCF的高催化性能归因于相混合导致的强金属-氧共价性和高氧离子扩散速率，这可能触发表面晶格氧活化以参与OER。Ruddlesden-Popper/钙钛矿杂化物构建的成功为设计用于各种能量应用的先进催化剂开辟了新方向。
