Optimal Geometrical Configuration of Cobalt Cations in Spinel Oxides to Promote Oxygen Evolution Reaction

Liu, Zhijuan; Wang, Guangjin; Zhu, Xiaoyan; Wang, Yanyong; Zou, Yuqin; Zang, Shuang‐Quan; Wang, Shuangyin

doi:10.1002/ange.201914245

Cited by 50 publications

(21 citation statements)

References 36 publications

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“…Among them, hydrogen is considered as the most promising substitute because of its high gravimetric energy density as well as zero CO 2 emission [5][6][7][8] . Recently, electrochemical water splitting, generally including two half-reactions, hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), has aroused increasing interests [9][10][11][12] . HER, producing low-cost and high purity hydrogen gas, is the hot spot in energy-conversion technologies and arouses increasing interests.…”

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confidence: 99%

Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

et al. 2021

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Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu0.13-BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu0.13-BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm−2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H2O and H*, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design.

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Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

et al. 2021

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“…The process is schematically represented in Figure 3e ). [34] In the meantime, the surface reconstruction will also lead to the dissolution of boron atoms, which will transform to metaborate species. Such ions may be adsorbed on the anion-exchange membrane separator for a real device, such as water splitting system.…”

Section: Electrochemical Activation and Surface Reconstructionmentioning

confidence: 99%

Understanding the Surface Reconstruction on Ternary W_xCoB_x for Water Oxidation and Zinc–Air Battery Applications

Gao

Ramière

Chu

et al. 2022

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The catalysts used to decrease the overpotential for this reaction play a pivotal role in realizing these devices. [2] Currently, iridium (Ir) and ruthenium (Ru) based oxides have been used as efficient OER catalysts. However, the scarcity and price of these materials makes them unsuitable for large-scale applications such that they need to be replaced with low-cost nonprecious metal electrocatalysts. [3] Many transition metal-based materials are promising alternatives to promote OER in alkaline media. Among the earth-abundant elements, cobalt was found to be one of the best alternatives to replace noble metals for OER. Cobalt derivatives are widely investigated as OER catalysts, including their oxides, [4] nitrides, [5,6] selenides, [7] borides, [8] carbides, [9] and phosphides. [10] The surfaces of these materials are known to undergo in situ transformations at Co sites to form cobalt oxyhydroxide (CoOOH) under the electric potential applied during the water oxidation process. [11] This surface reconstruction process directly determines the final performance of the catalysts. For instance, Duan et al., reported the controllable anodic leaching of Cr in CoCr 2 O 4 by activating the pristine material at high potential, which enables the transformation of the inactive CoCr 2 O 4 spinel into a highly Here, the synthesis of a series of pure phase metal borides is reported, including WB, CoB, WCoB, and W 2 CoB 2 , and their surface reconstruction is studied under the electrochemical activation in alkaline solution. A cyclic voltammetric activation is found to enhance the activity of the CoB and W 2 CoB 2 precatalysts due to the transformation of their surfaces into the amorphous CoOOH layer with a thickness of 3-4 nm. However, such surface transformation does not happen on the WB and WCoB due to their superior structure stability under the applied voltage, highlighting the importance of metal components for the surface reconstruction process. It is found that, compared with CoB, the W 2 CoB 2 surface shows a quicker reconstruction with a larger active surface area due to the selective leaching of the W from its surface. In the meantime, the metallic W 2 CoB 2 core underneath the CoOOH layer shows a better promotion of its oxygen evolution reaction (OER) performance than CoB. Therefore, the ternary W 2 CoB 2 shows better OER performance than the CoB, as well as the WB and WCoB. It is also found that the mixture of W 2 CoB 2 with Pt/C as the catalysts in air electrode for rechargeable Zn-air battery (ZAB), shows better performance than the IrO 2 -Pt/C couple-based ZAB.

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“…The coordination geometry and the electronic configuration of transition-metal centers can greatly affect the electrocatalytic performance. [34,35] The various orientations of phosphate/phosphonate ligands can lead to diverse structures, making metal phosphates/phosphonates an ideal platform to design active electrocatalysts with specific symmetries and geometries. One prominent illustration is the amorphous cobalt phosphate CoPi, which is formed through oxidative polarization of indium tin oxide electrode in phosphate buffer containing Co 2 + .…”

Section: Tuning Of Transition-metal Center Coordination Environmentmentioning

confidence: 99%

Design Strategies of Transition‐Metal Phosphate and Phosphonate Electrocatalysts for Energy‐Related Reactions

Zhao

Yuan

2020

ChemSusChem

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The key challenge to developing renewable energy conversion and storage devices lies in the exploration and rational engineering of cost‐effective and highly efficient electrocatalysts for various energy‐related electrochemical reactions. Transition‐metal phosphates and phosphonates have shown remarkable performances for these reactions based on their unique physicochemical properties. Compared with transition‐metal oxides, phosphate groups in transition‐metal phosphates and phosphonates show flexible coordination with diverse orientations, making them an ideal platform for designing active electrocatalysts. Although numerous efforts have been spent on the development of transition‐metal phosphate and phosphonate electrocatalysts, some urgent issues, such as low intrinsic catalytic efficiency and low electronic conductivity, have to be resolved in accordance with their applications. In this Review, we focus on the design strategies of highly efficient transition‐metal phosphate and phosphonate electrocatalysts, with special emphasis on the tuning of transition‐metal‐center coordination environment, optimization of electronic structures, increase of catalytically active site densities, and construction of heterostructures. Guided by these strategies, recently developed transition‐metal phosphate and phosphonate materials have exhibited excellent activity, selectivity, and stability for various energy‐related electrocatalytic reactions, showing great potential for replacing noble‐metal‐based catalysts in next‐generation advanced energy techniques. The existing challenges and prospects regarding these materials are also presented.

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Optimal Geometrical Configuration of Cobalt Cations in Spinel Oxides to Promote Oxygen Evolution Reaction

Cited by 50 publications

References 36 publications

Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

Understanding the Surface Reconstruction on Ternary W_xCoB_x for Water Oxidation and Zinc–Air Battery Applications

Design Strategies of Transition‐Metal Phosphate and Phosphonate Electrocatalysts for Energy‐Related Reactions

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Optimal Geometrical Configuration of Cobalt Cations in Spinel Oxides to Promote Oxygen Evolution Reaction

Cited by 50 publications

References 36 publications

Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution

Understanding the Surface Reconstruction on Ternary WxCoBx for Water Oxidation and Zinc–Air Battery Applications

Design Strategies of Transition‐Metal Phosphate and Phosphonate Electrocatalysts for Energy‐Related Reactions

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Understanding the Surface Reconstruction on Ternary W_xCoB_x for Water Oxidation and Zinc–Air Battery Applications