Molecular Ru(II) complexes with universal pH hydrogen evolution performance

IF 3.5 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Dalton Transactions Pub Date : 2025-05-09 DOI:10.1039/d5dt00880h

Rakesh Kumar, Baghendra Singh, Apparao Draksharapu

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Abstract

The development of efficient and robust hydrogen evolution reaction (HER) catalysts that operate across a wide pH range is critical for advancing sustainable hydrogen production. Previously a series of molecular complexes have been immobilized on solid supports to get efficient HER activity. However, achieving HER activity with molecular complexes in universal pH still remains challenging. Herein, we demonstrated two Ru(II) complexes and systematically characterized them using spectroscopic techniques. The (MeTBEN)Ru(II) (2) exhibited outstanding hydrogen evolution activity across a wide pH range, specifically alkaline, neutral, and acidic electrolytes, with the highest performance observed in acidic electrolytes compared to the (BnTBEN)Ru(II) complex (1). The 2 demonstrates outstanding electrocatalytic performance with a low overpotential of 115 mV at 10 mA cm^-2 in 0.5 M H₂SO₄, along with excellent turnover frequency. Furthermore, 2 demonstrated excellent electrochemical stability, sustaining its activity for up to 8 hours under acidic conditions.

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具有普遍pH值析氢性能的Ru（II）配合物

开发在宽pH范围内运行的高效、稳健的析氢反应（HER）催化剂对于推进可持续制氢至关重要。为了获得高效的HER活性，一系列分子配合物已被固定化在固体载体上。然而，在普遍的pH值下实现分子复合物的HER活性仍然具有挑战性。在这里，我们展示了两个Ru（II）配合物，并使用光谱技术系统地表征了它们。（MeTBEN）Ru(II)(2)在较宽的pH范围内表现出出色的析氢活性，特别是在碱性、中性和酸性电解质中，与（BnTBEN）Ru（II）配合物(1)相比，在酸性电解质中表现出最高的性能。2具有优异的电催化性能，在0.5 M H₂SO₄中，在10 mA cm-2下过电位低至115 mV，并且具有优异的周转频率。此外，2表现出优异的电化学稳定性，在酸性条件下保持其活性长达8小时。

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来源期刊

Dalton Transactions 化学-无机化学与核化学

CiteScore

6.60

自引率

7.50%

发文量

1832

审稿时长

1.5 months

期刊介绍： Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.