Construction of Ni‐Co‐Fe Hydr(oxy)oxide@Ni‐Co Layered Double Hydroxide Yolk‐Shelled Microrods for Enhanced Oxygen Evolution

Niu, Qian; Yang, Min; Luan, Deyan; Li, Nianwu; Yu, Le; Lou, Xiong-Wen

doi:10.1002/ange.202213049

Angewandte Chemie

2022

DOI: 10.1002/ange.202213049

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Construction of Ni‐Co‐Fe Hydr(oxy)oxide@Ni‐Co Layered Double Hydroxide Yolk‐Shelled Microrods for Enhanced Oxygen Evolution

Qian Niu

Min Yang

Deyan Luan

et al.

Abstract: The exploration of earth-abundant and efficient electrocatalysts toward the oxygen evolution reaction (OER) is critical for sustainable energy storage and conversion devices. In this work, we report a selfengaged strategy to fabricate a yolk-shelled OER electrocatalyst. Starting with a metal-organic framework, Co-Fe layered double hydroxide (LDH)@zeolitic imidazolate framework-67 (ZIF-67) yolk-shelled structures are formed in one step. Afterwards, these ZIF-67 building blocks are transformed into Ni-Co LDH nan… Show more

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Cited by 6 publications

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The Guest Doping Effects of Fe on Bimetallic NiCo Layered Double Hydroxide for Enhanced Electrochemical Oxygen Evolution Reaction: Theoretical Screening and Experimental Verification

Zhang

Guo

et al. 2023

Adv Funct Materials

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Exploring efficient transition‐metal‐based electrocatalysts for oxygen evolution reaction (OER) is imperative but remain challenging for sustainable energy storage and conversion systems. Foreign species doping is a significant regulation strategy to enhance the intrinsic activity of host matrix. However, the potential relationship of structure‐activity caused by guest doping elements is seldom tracked systematically. In this case, both theoretical screening and experimental verification are complementarily employed to investigate the guest doping effects of ten first‐row transition metals (Sc∼Zn) on bimetallic NiCo layered double hydroxide (NiCo‐LDH). As a result, the optimized Fe‐doped NiCo‐LDH is identified as the most promising candidate toward alkaline electrocatalytic OER, which exhibits the quasi‐industrial current density of 1000 mA cm−2 at overpotential of 400 mV. Meanwhile, it also shows impressively long‐term stability of 500 h at 500 mA cm−2 with a negligible activity loss. Moreover, in situ electrochemical Raman spectroscopy unveils the dynamic structure evolution from pre‐catalytic state (Fe‐NiCo‐LDH) to metal oxyhydroxide (Fe‐(NiCo)OOH) during the oxidation reaction, and ab‐initio molecular dynamics simulations are further performed to confirm the thermodynamic stability of activated Fe‐(NiCo)OOH phase. This work provides a promising platform for exploring the critical role of transition metal guest doping on host matrix in developing industrially required OER electrocatalysts.

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The Guest Doping Effects of Fe on Bimetallic NiCo Layered Double Hydroxide for Enhanced Electrochemical Oxygen Evolution Reaction: Theoretical Screening and Experimental Verification

Zhang

Guo

et al. 2023

Adv Funct Materials

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Oxygen Defect Site Filling Strategy Induced Moderate Enrichment of Reactants for Efficient Electrocatalytic Biomass Upgrading

Cheng,

Zhan,

et al. 2024

Advanced Science

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The electrocatalytic oxidation of 5‐hydroxymethylfurfural (HMF) provides a feasible approach for the efficient utilization of biomass. Defect regulation is an effective strategy in the field of biomass upgrading to enhance the adsorption capacity of reactants and thus increase the activity. However, how to select appropriate strategies to regulate the over‐enrichment of reactants induced by excessive oxygen vacancy is still a huge challenge. In this work, the defect‐filling strategy to design and construct an element‐filled oxygen vacancy site layered double hydroxide (S─Ov─LDH) is adopted, which achieves a significant reduction in the electrolysis potential of biomass platform molecule HMF oxidation reaction and a significant increase in current density. Physical characterizations, electrochemical measurements, and theoretical calculations prove that the formation of metal─S bond in the second shell effectively regulates the electronic structure of the material, thus weakening the over‐strong adsorption of HMF and OH− induced by excessive oxygen vacancy, promoting the formation of high‐valence Co3+ during the reaction, and forming new adsorption sites. This work discusses the catalytic enhancement mechanism of defect filling in detail, fills the gap of defect filling in the field of biomass upgrading, and provides favorable guidance for the further development of defect regulation strategies.

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Regulating Spin States in Oxygen Electrocatalysis

Zhang

Luo

et al. 2023

Angewandte Chemie

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Developing efficient and stable transition metal oxides catalysts for energy conversion processes such as oxygen evolution reaction and oxygen reduction reaction is one of the key measures to solve the problem of energy shortage. The spin state of transition metal oxides is strongly correlated with their catalytic activities. In an octahedral structure of transition metal oxides, the spin state of active centers could be regulated by adjusting the splitting energy and the electron pairing energy. Regulating spin state of active centers could directly modulate the d orbitals occupancy, which influence the strength of metal‐ligand bonds and the adsorption behavior of the intermediates. In this review, we clarified the significance of regulating spin state of the active centers. Subsequently, we discussed several characterization technologies for spin state and some recent strategies to regulate the spin state of the active centers. Finally, we put forward some views on the future research direction of this vital field.

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Construction of Ni‐Co‐Fe Hydr(oxy)oxide@Ni‐Co Layered Double Hydroxide Yolk‐Shelled Microrods for Enhanced Oxygen Evolution

Cited by 6 publications

References 56 publications

The Guest Doping Effects of Fe on Bimetallic NiCo Layered Double Hydroxide for Enhanced Electrochemical Oxygen Evolution Reaction: Theoretical Screening and Experimental Verification

The Guest Doping Effects of Fe on Bimetallic NiCo Layered Double Hydroxide for Enhanced Electrochemical Oxygen Evolution Reaction: Theoretical Screening and Experimental Verification

Oxygen Defect Site Filling Strategy Induced Moderate Enrichment of Reactants for Efficient Electrocatalytic Biomass Upgrading

Regulating Spin States in Oxygen Electrocatalysis

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