通过碳复合策略增强金属-N-杂环卡宾配合物作为析氢和析氧反应双功能电催化剂的电催化活性,Energy & Fuels

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通过碳复合策略增强金属-N-杂环卡宾配合物作为析氢和析氧反应双功能电催化剂的电催化活性
Energy & Fuels ( IF 5.2 ) Pub Date : 2024-03-08 , DOI: 10.1021/acs.energyfuels.3c04793
Monica Vijayakumar ₁ , Gautam Achar ₁ , Zhoveta Yhobu ₁ , Jan Grzegorz Mal̷ecki ₂ , Doddahalli H. Nagaraju ₃ , Rangappa S. Keri ₁ , Srinivasa Budagumpi ₁

Affiliation

为了通过水电解实现绿色能源的高效转化，需要开发合理的、地球丰富的、强大的用于析氢反应（HER）和析氧反应（OER）的双功能电催化剂。在这方面，N-杂环卡宾（NHC）配位金属配合物由于其易于制备和在立体电子领域的模块化性而成为最令人兴奋和最普遍的有机金属化合物之一。在这里，我们报告了一系列由 NHC 前体与适当金属源反应合成的金属 NHC 配合物，并使用光谱和分析技术进行了彻底表征。金属-NHC复合物及其使用多壁碳纳米管（MWCNT）和石墨烯板（GP）的碳复合材料分别在酸性和碱性电解质中测试了电化学HER和OER性能。与裸复合物相比，MWCNT 和 GP 复合材料表现出更高的 HER 活性。此外，与裸金属-NHC复合物的活性相比，碳复合材料的OER性能明显提高了两倍，以实现超电势（η ₁₀）。此外，电化学阻抗谱技术用于得出证明 HER 和 OER 反应的活性趋势以及电催化剂的电极-电解质相互作用的性质所需的关键信息。

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Augmenting the Electrocatalytic Activities of Metal–N-Heterocyclic Carbene Complexes as Bifunctional Electrocatalysts for Hydrogen and Oxygen Evolution Reactions by Carbon Composite Strategy

The pursuit of efficient transformation of green energy sources through water electrolysis necessitates the expansion of reasonable, earth-abundant, and robust bifunctional electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). In this connection, N-heterocyclic carbenes (NHCs) coordinated metal complexes have become one of the most stimulating and ubiquitous classes of organometallics due to their ease of preparation and modularity in stereoelectronic possessions. Here, we report a series of metal NHC complexes synthesized by the reaction of an NHC precursor with an appropriate metal source and thoroughly characterized using spectral and analytical techniques. Both metal–NHC complexes and their carbon composites using multiwalled carbon nanotubes (MWCNT) and graphene plates (GP) were tested for their electrochemical HER and OER performances in acidic and basic electrolytes, respectively. The MWCNT and GP composites displayed improved HER activity compared with the bare complexes. Furthermore, a two-fold improved OER performance of the carbon composites was evident compared with the activity of the bare metal–NHC complexes to achieve the overpotential (η₁₀). Furthermore, the electrochemical impedance spectroscopic technique was used to bring out the key information required to justify the activity trend in HER and OER reactions and the nature of the electrode–electrolyte interaction of electrocatalysts.

更新日期：2024-03-08

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