Complete Reconstruction of Hydrate Pre-Catalysts for Ultrastable Water Electrolysis in Industrial-Concentration Alkali Media

Liu, Xiong; Meng, Jiashen; Ni, Kun; Guo, Rui; Xia, Fanjie; Xie, Jingjing; Xu, Li; Wen, Bo; Wu, Peijie; Li, Ming; Wu, Jinsong; Wu, Xiaojun; Mai, Liqiang; Zhao, Dongyuan

doi:10.1016/j.xcrp.2020.100241

Cited by 124 publications

(129 citation statements)

References 45 publications

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“…These results further highlight the importance of elaborately designing controllable structures of precatalysts. In addition, factors that affect the reaction conditions such as the concentration of the electrolyte, the applied potential, and the temperature will also affect the degree of surface change [ 56 , 85 ]. Thus, much effort has been devoted to exploring advanced OER electrocatalysts based on surface reconstruction [ 63 , 79 , 86 , 87 ].…”

Section: Fundamental Understanding Of Surface Reconstructionmentioning

confidence: 99%

“…Independent of material types and particle sizes, for most reported OER-precatalysts, the values of reconstruction layer thickness are less than 10 nm [ 85 ]. Considering the highly active of in situ formed metal oxyhydroxides, it is reasonable to expect that the electrochemical performance of precatalysts would be greatly improved with the enhanced surface reconstruction level, namely deep surface reconstruction [ 117 , 118 ].…”

Section: Accelerating Surface Reconstructionmentioning

confidence: 99%

“…For surface reconstruction and deep reconstruction, the in situ formed layer would lead to a core-shell structure, where the in situ-formed active species and the unchanged precatalyst serve as the shell and core, respectively [ 14 , 63 , 75 , 92 , 104 , 120 , 121 , 122 ]. When the core material cannot favorably contribute to the shell or when the core material has the potential to be transformed further into active species, traditional near-surface reconstruction would have considerable limitations [ 85 ]. Complete changes of bulk materials can enhance the active sites to a great extent, but this remains a major challenge [ 85 , 123 ].…”

Section: Making Complete Reconstructionmentioning

confidence: 99%

“…When the core material cannot favorably contribute to the shell or when the core material has the potential to be transformed further into active species, traditional near-surface reconstruction would have considerable limitations [ 85 ]. Complete changes of bulk materials can enhance the active sites to a great extent, but this remains a major challenge [ 85 , 123 ].…”

Section: Making Complete Reconstructionmentioning

confidence: 99%

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Tuning Reconstruction Level of Precatalysts to Design Advanced Oxygen Evolution Electrocatalysts

2021

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Surface reconstruction engineering is an effective strategy to promote the catalytic activities of electrocatalysts, especially for water oxidation. Taking advantage of the physicochemical properties of precatalysts by manipulating their structural self-reconstruction levels provide a promising methodology for achieving suitable catalysts. In this review, we focus on recent advances in research related to the rational control of the process and level of surface transformation ultimately to design advanced oxygen evolution electrocatalysts. We start by discussing the original contributions to surface changes during electrochemical reactions and related factors that can influence the electrocatalytic properties of materials. We then present an overview of current developments and a summary of recently proposed strategies to boost electrochemical performance outcomes by the controlling structural self-reconstruction process. By conveying these insights, processes, general trends, and challenges, this review will further our understanding of surface reconstruction processes and facilitate the development of high-performance electrocatalysts beyond water oxidation.

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Section: Fundamental Understanding Of Surface Reconstructionmentioning

confidence: 99%

Section: Accelerating Surface Reconstructionmentioning

confidence: 99%

Section: Making Complete Reconstructionmentioning

confidence: 99%

Section: Making Complete Reconstructionmentioning

confidence: 99%

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Tuning Reconstruction Level of Precatalysts to Design Advanced Oxygen Evolution Electrocatalysts

2021

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“…Although these ECSR phenomena have been captured to extend our cognition of catalytic origins, so far, few attention has been paid to utilizing ECSR as a proactive strategy to produce new substances boosting catalytic OER activity. [38] Nevertheless, it is a great challenge to engineer ECSR because the electro-oxidation-driven reconstruction is a timedependent process with dynamic complexity, [39] relevant to the structural flexibility of precursor pre-catalysts. In this regard, the loose layered structure of TM-LDHs with variable anion interlayers can be reasonably suggestive of their suitability for ECSR engineering, to our best knowledge, which yet remains underexplored by far.…”

Section: Introductionmentioning

confidence: 99%

Engineering Self‐Reconstruction via Flexible Components in Layered Double Hydroxides for Superior‐Evolving Performance

Liu

Ding

Zhu

et al. 2021

Small

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Most transition metal‐based catalysts for electrocatalytic oxygen evolution reaction (OER) undergo surface reconstruction to generate real active sites favorable for high OER performance. Herein, how to use self‐reconstruction as an efficient strategy to develop novel and robust OER catalysts by designing pre‐catalysts with flexible components susceptible to OER conditions is proposed. The NiFe‐based layered double hydroxides (LDHs) intercalated with resoluble molybdate (MoO42−) anions in interlayers are constructed and then demonstrated to achieve complete electrochemical self‐reconstruction (ECSR) into active NiFe‐oxyhydroxides (NiFeOOH) beneficial to alkaline OER. Various ex situ and in situ techniques are used to capture structural evolution process including fast dissolution of MoO42− and deep reconstruction to NiFeOOH upon simultaneous hydroxyl invasion and electro‐oxidation. The obtained NiFeOOH exhibits an excellent OER performance with an overpotential of only 268 mV at 50 mA cm−1 and robust durability over 45 h, much superior to NiFe‐LDH and commercial IrO2 benchmark. This work suggests that the ECSR engineering in component‐flexible precursors is a promising strategy to develop highly active OER catalysts for energy conversion.

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Ligand and Anion Co‐Leaching Induced Complete Reconstruction of Polyoxomolybdate‐Organic Complex Oxygen‐Evolving Pre‐Catalysts

Liu

Xia

Guo

et al. 2021

Adv Funct Materials

Self Cite

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The coordination compounds in the oxygen evolution reaction (OER) have been researched extensively. However, their poor durability (mostly < 100 h) and controversial reconstruction mechanism restrict their practical applications. Herein, a new‐type polyoxomolybdate‐organic complex (POMo) via wet‐chemistry synthesis with fixed coordination between metal centers (Ni2+ and [Mo8O26]4−) and 2‐Methylimidazole ligand is introduced. After introducing iron, a series of Fe‐doped Ni‐POMo with porous and amorphous structures are fabricated. These features accelerate the diffusion‐leaching processes of ligands and anions, resulting in rapid and complete phase reconstruction during alkaline OER. As a result, nickel‐iron (oxy)hydroxides with rich vacancies and poly‐/low‐crystalline features are in situ generated through dissolution‐redeposition, and serve as the OER‐active species. The optimized Fe0.052Ni‐POMo array pre‐catalyst has excellent activity and sustains ultrastable catalysis for 545 h. The complete reconstruction of POMo enables high catalytic durability (230 h) and stable active phase under realistic conditions (30 wt% KOH, 60.9 °C). Accordingly, the completely reconstructed catalysts with unique structures and ultrastable catalysis have the potential to be applied in industry.

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Complete Reconstruction of Hydrate Pre-Catalysts for Ultrastable Water Electrolysis in Industrial-Concentration Alkali Media

Cited by 124 publications

References 45 publications

Tuning Reconstruction Level of Precatalysts to Design Advanced Oxygen Evolution Electrocatalysts

Tuning Reconstruction Level of Precatalysts to Design Advanced Oxygen Evolution Electrocatalysts

Engineering Self‐Reconstruction via Flexible Components in Layered Double Hydroxides for Superior‐Evolving Performance

Ligand and Anion Co‐Leaching Induced Complete Reconstruction of Polyoxomolybdate‐Organic Complex Oxygen‐Evolving Pre‐Catalysts

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