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用于实际海水中稳定析氧反应的动态重构镍铬氧化物电催化剂

Dynamically Restructuring Ni Cr O Electrocatalyst for Stable Oxygen Evolution Reaction in Real Seawater.

作者信息

Malek Abdul, Xue Yanrong, Lu Xu

机构信息

CCRC, Division of Physical Science and Engineering (PSE), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900 (Kingdom of, Saudi Arabia.

KAUST Solar Center (KSC), PSE, KAUST (Kingdom of, Saudi Arabia.

出版信息

Angew Chem Int Ed Engl. 2023 Oct 2;62(40):e202309854. doi: 10.1002/anie.202309854. Epub 2023 Aug 25.

DOI:10.1002/anie.202309854
PMID:37578684
Abstract

In the pursuit of long-term stability for oxygen evolution reaction (OER) in seawater, retaining the intrinsic catalytic activity is essential but has remained challenging. Herein, we developed a Ni Cr O electrocatalyst that manifested exceptional OER stability in alkaline condition while improving the activity over time by dynamic self-restructuring. In 1 M KOH, Ni Cr O required overpotentials of only 270 and 320 mV to achieve current densities of 100 and 500 mA cm , respectively, with excellent long-term stability exceeding 475 h at 100 mA cm and 280 h at 500 mA cm . The combination of electrochemical measurements and in situ studies revealed that leaching and redistribution of Cr during the prolonged electrolysis resulted in increased electrochemically active surface area. This eventually enhanced the catalyst porosity and improved OER activity. Ni Cr O was further applied in real seawater from the Red Sea (without purification, 1 M KOH added), envisaging that the dynamically evolving porosity can offset the adverse active site-blocking effect posed by the seawater impurities. Remarkably, Ni Cr O exhibited stable operation for 2000, 275 and 100 h in seawater at 10, 100 and 500 mA cm , respectively. The proposed catalyst and the mechanistic insights represented a step towards realization of non-noble metal-based direct seawater splitting.

摘要

在追求海水电解析反应(OER)的长期稳定性过程中,保持其固有催化活性至关重要,但仍具有挑战性。在此,我们开发了一种NiCrO电催化剂,该催化剂在碱性条件下表现出优异的OER稳定性,同时通过动态自我重构随时间提高活性。在1 M KOH中,NiCrO分别仅需270和320 mV的过电位即可实现100和500 mA cm²的电流密度,在100 mA cm²时具有超过475 h的优异长期稳定性,在500 mA cm²时具有280 h的优异长期稳定性。电化学测量和原位研究相结合表明,长时间电解过程中Cr的浸出和再分布导致电化学活性表面积增加。这最终提高了催化剂的孔隙率并改善了OER活性。NiCrO进一步应用于红海的实际海水(未纯化,添加1 M KOH),设想动态演变的孔隙率可以抵消海水杂质造成的不利活性位点阻塞效应。值得注意的是,NiCrO在海水中分别在10、100和500 mA cm²下稳定运行2000、275和100 h。所提出的催化剂及其机理见解代表了迈向实现基于非贵金属的直接海水分解的一步。

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