A mechanism study on performance of iron metal coordination polymers in the electrosynthesis of hydrogen peroxide

IF 2.7 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Inorganica Chimica Acta Pub Date : 2025-03-31 DOI:10.1016/j.ica.2025.122686

Changzhong Liang , Yixin Feng , Poe Ei Phyu Win , Jiong Wang

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Abstract

To tune the oxidation states of metal active sites represents a classical strategy to achieve efficient two-electron oxygen reduction reaction (2e⁻-ORR) catalysts for electrosynthesis of H₂O₂. In this work, iron (Fe)-1,2,4,5-tetrahydroxybenzene (H₄thb) coordination polymers were obtained by a common hydrothermal synthesis for efficient 2e⁻-ORR electrocatalysis with tuning the oxidation states of Fe sites. This caused tuned coordination in polymers by generating planar Fe-O₄ sites, and octahedral Fe-O₄(H₂O)₂ sites that carrying two extra water molecules at the axial position of Fe sites. Despite the axial water coordination improved the electrical conductivity and numbers of electrochemical active Fe sites of resultant polymers, the Fe-O₄(H₂O)₂ sites exhibited limited performance. While the planar Fe-O₄ coordination greatly promotes the electron delocalization at the Fe center, which facilitates O₂ chemisorption and activation, and intrinsically improved the 2e⁻-ORR performance of Fe sites.

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铁金属配位聚合物在过氧化氢电合成中的性能机理研究

调整金属活性位点的氧化态是实现电合成H2O2的高效双电子氧还原反应（2e−-ORR）催化剂的经典策略。本文通过水热法合成了铁(Fe)-1,2,4,5-四羟基苯（H4thb）配位聚合物，通过调整Fe位的氧化态，获得了高效的2e−-ORR电催化聚合物。这通过产生平面的Fe- o4位点和八面体的Fe- o4 (H2O)2位点，在Fe位点的轴向位置携带两个额外的水分子，导致聚合物中的配位调整。尽管轴向水配位提高了聚合物的电导率和电化学活性铁位的数量，但Fe- o4 (H2O)2位的性能有限。而Fe- o4的平面配位极大地促进了Fe中心的电子离域，促进了O2的化学吸附和活化，从本质上提高了Fe位点的2e−-ORR性能。

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来源期刊

Inorganica Chimica Acta 化学-无机化学与核化学

CiteScore

6.00

自引率

3.60%

发文量

440

审稿时长

35 days

期刊介绍： Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews. Topics covered include: • chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies; • synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs); • reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models; • applications of inorganic compounds, metallodrugs and molecule-based materials. Papers composed primarily of structural reports will typically not be considered for publication.