Exploring the Performance Improvement of the Oxygen Evolution Reaction in a Stable Bimetal–Organic Framework System

Wang, Xiaoli; Dong, Long‐Zhang; Qiao, Man; Tang, Yawei; Liu, Jiang; Li, Yafei; Li, Shun-Li; Su, Jiaxin; Lan, Ya‐Qian

doi:10.1002/anie.201803587

Cited by 364 publications

(197 citation statements)

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“…As a consequence, only a limited number of MOFs have been reported which are used as electrocatalysts in acid and alkaline solution. [18][19][20][21] We proposed therefore to rationally design a bimetallic system containing Co-based BIFs incorporated with Fe 3+ to achieve synergistically enhanced OER activity.We report a new Co-based red-block crystal of CoB(im) 4 (ndc) 0.5 (BIF-91, im = imidazolate, ndc = 2, 6-naphthalenedicarboxylate) that was successfully synthesized by reaction of H 4 ndc with cobalt (II) acetate tetrahydrate and presynthesized KB (im) 4 ligand. The result is a destroyed host-framework and loss of active sites.…”

mentioning

confidence: 99%

“…[16] Uniformly distributed 3/4-connected boron components keep the framework rigid. [18][19][20][21] We proposed therefore to rationally design a bimetallic system containing Co-based BIFs incorporated with Fe 3+ to achieve synergistically enhanced OER activity. This means these are, potentially, alkaline-resistant electrocatalysts for oxygen evolution reaction (OER).…”

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confidence: 99%

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Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction

et al. 2019

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Metal–organic frameworks (MOFs) have significant potential for practical application in catalysis. However, many MOFs are shown to be sensitive to aqueous solution. This severely limits application of MOFs in electrocatalytic operations for energy production and storage. Here, a Co (II) boron imidazolate framework CoB(im) 4 (ndc) 0.5 ( BIF‐91 , im = imidazolate, ndc = 2,6‐naphthalenedicarboxylate) that is rationally designed and successfully tested for electrocatalytic application in strong alkaline (pH ≈ 14) solution is reported. In such a BIF system, the inherent carboxylate species segment large channel spaces into multiple domains in which each single channel is filled with ndc ligands through the effect of zeolite channel confinement. These ligands, with strong C—H···π interaction, act as a rigid auxiliary linker to significantly enhance the structural stability of the BIF‐91 framework. Additionally, the π‐conjugated effect in BIF‐91 stabilizes dopant Fe (III) at the atomic scale to construct Fe‐immobilized BIF‐91 ( Fe@BIF‐91 ). Due to the synergistic effect between Fe (III) guest and Co (II) in the framework, the Fe@BIF‐91 acts as an active and stable electrocatalyst for the oxygen evolution reaction in alkaline solution.

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confidence: 99%

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Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction

et al. 2019

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“…[32][33][34] We therefore define the applied potential to overcome the maximum energy barriers as the overpotentials (η) for CO 2 RR or HER. [32][33][34] We therefore define the applied potential to overcome the maximum energy barriers as the overpotentials (η) for CO 2 RR or HER.…”

Section: Reaction Pathways and Scaling Relationshipmentioning

confidence: 99%

Catalytic Mechanisms and Design Principles for Single‐Atom Catalysts in Highly Efficient CO₂ Conversion

Gong

Zhang

Lin

et al. 2019

Advanced Energy Materials

190

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energy such as wind and solar energy has attracted enormous interest for its significant roles in mitigating CO 2 emissions and reducing dependence on petrochemicals. [1,2] At the heart of the CO 2 conversion technology, electrocatalysts are needed to promote a critical reaction, CO 2 reduction reaction (CO 2 RR) that determines the efficiency and selectivity. To date, the electrocatalysts have confronted severe bottlenecks issue: poor selectivity about various accessory products in CO 2 conversion process, and loss of efficiency toward competing hydrogen evolution. [3] The former involves associated multielectron transfer process and is difficult to accurately control the reaction process by external conditions, [4] while the latter is mainly due to the fact that the equilibrium potentials for most of the CO 2 RR are very close to hydrogen evolution reaction (HER) toward undesirable side-products in aqueous electrolytes, which degrades the electrocatalytic performance during the CO 2 RR process. [5,6] Therefore, CO 2 RR is much more complex than other energy-related electrochemical reactions such as oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), and it is still a great challenge to design and synthesize electrocatalytic materials with higher product selectivity and catalytic activity for CO 2 RR.Among the electrocatalysts including metals oxides and metal-doped carbon materials, single-atom catalysts (SACs) represent an exciting class of catalysts with monodispersed metal catalytic centers and have emerged as the frontier science in both homogeneous and heterogeneous catalysis, including CO 2 conversion. [7][8][9][10] This type of catalysts contains M-N-C moiety with single atoms and is common in building metalorganic frameworks (MOFs), [11] covalent organic frameworks (COFs) [12] with transition metal macrocyclic clusters, such as porphyrin, phthalocyanine, and tetraazannulene, as well as metal-doped carbon materials [13] (e.g., graphene, carbon nanotubes, fullerene). In nature, the biomolecules, like chlorophyll (Mg-porphyrin) in leaves, and iron porphyrins in cytochrome c oxidase in blood cells, have similar structures as SACs, with special ability in photosynthesis and transforming CO 2 from cells with high efficiency and selectivity. [14] Through the selection of appropriate motifs, the construction principles of Direct conversion of CO 2 into carbon-neutral fuels or industrial chemicals holds a great promise for renewable energy storage and mitigation of greenhouse gas emission. However, experimentally finding an electrocatalyst for specific final products with high efficiency and high selectivity poses serious challenges due to multiple electron transfer, complicated intermediates, and numerous reaction pathways in electrocatalytic CO 2 reduction. Here, an intrinsic descriptor that correlates the catalytic activity with the topological, bonding, and electronic structures of catalytic centers on M-N-C based single-atom catalysts is discovered. The "volcano"-shaped relationships betwee...

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“…and showed outstanding electrocatalytic activity toward the OER . Another effective strategy is to design multivariate MOFs that possess an electronic synergistic effect between different metals and thus deliver a better OER performance than monometallic MOFs …”

Section: Methodsmentioning

confidence: 99%

Stable Iron Hydroxide Nanosheets@Cobalt‐Metal–Organic–Framework Heterostructure for Efficient Electrocatalytic Oxygen Evolution

Gao

Liu

et al. 2019

ChemSusChem

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Most studies are devoted to the use of metal–organic frameworks (MOFs) as templates to construct desirable electrocatalysts in situ by high‐temperature pyrolysis. The emergence of heterostructures invokes new opportunities to use the full potential of pristine MOFs as efficient catalysts in the oxygen evolution reaction (OER). Here, a MOF surface‐reaction strategy is developed to synthesize MOF‐based heterostructures without pyrolysis. Uniform Fe(OH)3 nanosheets are grown controllably on the Co‐MOF‐74 surface by a fast “phenol–Fe” reaction that takes advantage of the hydroxyl sites in Co‐MOF‐74. The resulting Fe(OH)3@Co‐MOF‐74 heterostructure delivers an excellent performance in the OER with a low overpotential of 292 mV at 10 mA cm−2. Notably, the introduction of Fe can improve the intrinsic activity of the original Co atom significantly. The turnover frequency in Fe(OH)3@Co‐MOF‐74 (1.209 s−1) is more than 25 times higher than that in Co‐MOF‐74 (0.048 s−1). This work presents a fresh concept for the fundamental design of advanced pure‐MOF‐based heterostructures and, thereby, provides a new avenue for the fabrication of other energy‐conversion and ‐storage materials.

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Exploring the Performance Improvement of the Oxygen Evolution Reaction in a Stable Bimetal–Organic Framework System

Cited by 364 publications

References 50 publications

Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction

Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction

Catalytic Mechanisms and Design Principles for Single‐Atom Catalysts in Highly Efficient CO₂ Conversion

Stable Iron Hydroxide Nanosheets@Cobalt‐Metal–Organic–Framework Heterostructure for Efficient Electrocatalytic Oxygen Evolution

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Exploring the Performance Improvement of the Oxygen Evolution Reaction in a Stable Bimetal–Organic Framework System

Cited by 364 publications

References 50 publications

Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction

Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction

Catalytic Mechanisms and Design Principles for Single‐Atom Catalysts in Highly Efficient CO2 Conversion

Stable Iron Hydroxide Nanosheets@Cobalt‐Metal–Organic–Framework Heterostructure for Efficient Electrocatalytic Oxygen Evolution

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Catalytic Mechanisms and Design Principles for Single‐Atom Catalysts in Highly Efficient CO₂ Conversion