Emerging covalent organic frameworks tailored materials for electrocatalysis

Cui, Xun; Lei, Sheng; Wang, Aurelia Chi; Gao, Likun; Zhang, Qing; Yang, Yingkui; Lin, Zhiqun

doi:10.1016/j.nanoen.2020.104525

Cited by 174 publications

(126 citation statements)

References 170 publications

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“…When considering framework materials for electrocatalysis, five main aspects for modification and enhancement rise to the forefront: chemical design of the active site, the pore environment, charge transport, the suitability of the framework to electrochemical systems, and stability under electrocatalytic conditions. 25 , 27 − 31 …”

Section: Framework Design Considerations For Electrocatalysismentioning

confidence: 99%

“…Unlike MOFs, covalent organic frameworks are formed exclusively by covalent bonds imparting great structural rigidity, chemical stability, and a higher degree of conductivity. 27 Aiyappa et al presented Co-TpBpy, a COF system containing single Co-Bpy active sites, for the electrocatalytic OER ( Figure 2 c). 70 This system exhibited an excellent performance with an overpotential of 400 mV (at a current density of 1 mA cm –2 ) and a Tafel slope of 59 mV dec –1 ( Figure 2 d).…”

Section: Extending Molecular Active Sites Into Framework Materialsmentioning

confidence: 99%

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From Molecules to Porous Materials: Integrating Discrete Electrocatalytic Active Sites into Extended Frameworks

et al. 2020

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Metal–organic and covalent–organic frameworks can serve as a bridge between the realms of homo- and heterogeneous catalytic systems. While there are numerous molecular complexes developed for electrocatalysis, homogeneous catalysts are hindered by slow catalyst diffusion, catalyst deactivation, and poor product yield. Heterogeneous catalysts can compensate for these shortcomings, yet they lack the synthetic and chemical tunability to promote rational design. To narrow this knowledge gap, there is a burgeoning field of framework-related research that incorporates molecular catalysts within porous architectures, resulting in an exceptional catalytic performance as compared to their molecular analogues. Framework materials provide structural stability to these catalysts, alter their electronic environments, and are easily tunable for increased catalytic activity. This Outlook compares molecular catalysts and corresponding framework materials to evaluate the effects of such integration on electrocatalytic performance. We describe several different classes of molecular motifs that have been included in framework materials and explore how framework design strategies improve on the catalytic behavior of their homogeneous counterparts. Finally, we will provide an outlook on new directions to drive fundamental research at the intersection of reticular-and electrochemistry.

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Section: Framework Design Considerations For Electrocatalysismentioning

confidence: 99%

Section: Extending Molecular Active Sites Into Framework Materialsmentioning

confidence: 99%

From Molecules to Porous Materials: Integrating Discrete Electrocatalytic Active Sites into Extended Frameworks

et al. 2020

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“…Motivated by the need for accelerating sluggish reaction kinetics at the anode, [1,2] the focus of water electrolysis has been centered heavily on oxygen evolution reaction (OER) towards sustainable hydrogen fuel production. To date, there has been much effort in developing low-cost yet high-performance earthabundant transition-metal alternatives to commonly used noble metals for OER.…”

Section: Introductionmentioning

confidence: 99%

Operando Unraveling Photothermal-Promoted Dynamic Active Sites Generation in Spinel NiFe2O4 for Oxygen Evolution

Gao

Cui

Wang

et al. 2020

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The ability to develop highly active and low-cost electrocatalysts represents an important endeavor toward accelerating sluggish water-oxidation kinetics. Herein, we report, for the first time, the implementation and unravelling of photothermal effect of spinel nanoparticles (NPs) on promoting dynamic active sites generation to markedly enhance their oxygen evolution reaction (OER) activity via an integrated operando Raman and density functional theory (DFT) study. Specifically, NiFe2O4 (NFO) NPs are first synthesized by capitalizing on amphiphilic star-like diblock copolymers as nanoreactors. Upon the NIR light irradiation, the photothermal heating of the NFO-based electrode progressively raises the temperature, accompanied by a marked decrease of overpotential. Accordingly, only an overpotential of 309 mV is required to yield a high current density of 100 mA cm-2, greatly lower than recently-reported earth-abundant electrocatalysts. More importantly, photothermal effect of NFO NPs not only significantly reduces the activation energy necessitated for water splitting, but also facilitates surface reconstruction into high-active oxyhydroxides at lower potential (1.36 V) under OER conditions, as revealed by operando Raman spectra-electrochemistry. Moreover, the DFT calculation corroborates that these reconstructed (Ni,Fe)oxyhydroxides are electrocatalytically active sites as the kinetics barrier is largely reduced over pure NFO without surface reconstruction. Given the diversity of materials (metal oxides, sulfides, phosphides, etc.) possessing the photo-to-thermal conversion, this effect may thus provide a unique and robust platform to boost highly-active surface species in nanomaterials for fundamental understanding of enhanced performance that may underpin future advances in electrocatalysis, photocatalysis, solar energy conversion and renewable energy production.

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“…The low cost and wide distribution of carbon materials like carbon nanotubes, pyrolyzed polymers, covalent organic frameworks (COFs) and graphene have been studied extensively as OER and ORR catalyst. [21][22][23][24][25][26][27][28] In addition, doping of single or more heteroatoms such as N, P, S and B to carbon materials are advantageous for electrocatalytic activity. It has been found that the multiple doping of heteroatoms can create strong synergistic coupling effect with unique electronic structure in the carbon framework.…”

Section: Introductionmentioning

confidence: 99%

Co-doped carbon materials synthesized with polymeric precursors as bifunctional electrocatalysts

et al. 2020

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Emerging covalent organic frameworks tailored materials for electrocatalysis

Cited by 174 publications

References 170 publications

From Molecules to Porous Materials: Integrating Discrete Electrocatalytic Active Sites into Extended Frameworks

From Molecules to Porous Materials: Integrating Discrete Electrocatalytic Active Sites into Extended Frameworks

Operando Unraveling Photothermal-Promoted Dynamic Active Sites Generation in Spinel NiFe2O4 for Oxygen Evolution

Co-doped carbon materials synthesized with polymeric precursors as bifunctional electrocatalysts

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