Abdullah Muhammad Imran, Fang Yusheng, Wu Xiaobing, Hu Meiqi, Shao Jing, Tao Youkun, Wang Haijiang
School of Science, Harbin Institute of Technology, Shenzhen, 518055, China.
Shenzhen Key Laboratory of New Lithium-ion Batteries and Mesoporous Materials, College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, 518060, China.
Nat Commun. 2024 Dec 4;15(1):10587. doi: 10.1038/s41467-024-54987-4.
One challenge remaining in the development of Ir-based electrocatalyst is the activity-stability paradox during acidic oxygen evolution reaction (OER), especially for the surface reconstructed IrO catalyst with high efficiency. To address this, a phase selective Ir-based electrocatalyst is constructed by forming bridged W-O moiety in NiIrO electrocatalyst. Through an electrochemical dealloying process, an nano-porous structure with surface-hydroxylated rutile NiWIrO electrocatalyst is engineered via Ni as a sacrificial element. Despite low Ir content, NiWIrO demonstrates a minimal overpotential of 180 mV for the OER at 10 mA·cm. It maintains a stable 300 mA·cm current density during an approximately 300 h OER at 1.8 V and shows a stability number of 3.9 × 10 n · n. The resulting W - O-Ir bridging motif proves pivotal for enhancing the efficacy of OER catalysis by facilitating deprotonation of OER intermediates and promoting a thermodynamically favorable dual-site adsorbent evolution mechanism. Besides, the phase selective insertion of W-O in NiIrO enabling charge balance through the W-O-Ir bridging motif, effectively counteracting lattice oxygen loss by regulating Ir-O co-valency.
铱基电催化剂开发中仍存在的一个挑战是在酸性析氧反应(OER)过程中的活性-稳定性矛盾,特别是对于具有高效率的表面重构氧化铱催化剂而言。为了解决这一问题,通过在镍铱氧化物电催化剂中形成桥连的钨-氧部分构建了一种相选择性铱基电催化剂。通过电化学脱合金过程,以镍作为牺牲元素设计出一种具有表面羟基化金红石型镍钨铱氧化物电催化剂的纳米多孔结构。尽管铱含量低,但镍钨铱氧化物在10 mA·cm²的析氧反应中表现出仅180 mV的最小过电位。在1.8 V下约300小时的析氧反应过程中,它保持稳定的300 mA·cm²电流密度,稳定性数值为3.9×10⁶ n·n。由此产生的钨-氧-铱桥连基序被证明对于通过促进析氧反应中间体的去质子化和促进热力学有利的双位点吸附剂演化机制来提高析氧反应催化效率至关重要。此外,在镍铱氧化物中相选择性插入钨-氧通过钨-氧-铱桥连基序实现电荷平衡,通过调节铱-氧共价性有效抵消晶格氧损失。