Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts

Jiao, Long; Zhang, Rui; Wan, Gang; Yang, Weijie; Wan, Xin; Zhou, Hua; Shui, Jianglan; Yu, Shu‐Hong; Jiang, Hai‐Long

doi:10.1038/s41467-020-16715-6

Cited by 390 publications

(174 citation statements)

References 52 publications

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“…[42] In order to increase the loading mass of metal SACs, they utilized a SiO 2 nanocoating strategy to avoid the formation of Fe agglomeration, and asdesigned SiO 2 @PCN-222 structure could obtain a high Fe loading mass of 3.46%. [43] Similarly, Xu's group has modified the synthetic process to fabricate overhang-eave structures with a silica-mediated strategy, which could maximize the exposure of active Fe SACs sites because more stretched edges could significantly promote the mass transport of ORR species. [18e] However, both ZIF-8 and PCN-222 require the ultrahigh temperature to reach the carbonization to immobilize the SACs.…”

Section: Metal Organic Framework-derived Carbon Supportsmentioning

confidence: 99%

“…[28] Recently, many researchers have found that SiO 2 could stabilize the metal NPs, clusters, or SACs by reducing the surface energy of metal atoms. [18e], [43] Therefore, SiO 2 protection method was widely used to increase the density of metal SACs. [18b], [33,34][43] For example, Jiang's group put forward a SiO 2 nanocasting strategy method for the preparation of PCN-222 MOF (a porphyrinic MOF with mesopores).…”

Section: Improve the Density Of Metal Sacsmentioning

confidence: 99%

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Carbon‐Supported Single‐Atom Catalysts for Formic Acid Oxidation and Oxygen Reduction Reactions

Han

Zhang

Yang

et al. 2021

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Pt-based alloys to accelerate the kinetic activity and improve the intermediates poisoning resistance. [2] Meanwhile, at the cathode side of DFAFCs and PEMFCs, oxygen is reduced into water through a four electron oxygen reduction reaction (ORR) route. Despite the high-cost and limited supply, costly Pt-based electrocatalysts remain the widely investigated materials for efficient ORR activity. Although the kinetics of FAOR and ORR have been enhanced by applying these modified platinum group metals (PGMs), [3] the higher cost and poorer-stability have significantly held back the commercialization of DFAFCs. Therefore, it is highly imperative to explore PGM-free electrocatalysts with high activity and robust stability for both FAOR and ORR.Recently, numerous efforts have been made to theoretically and experimentally employ single-atom catalysts (SACs) that were dispersed in different supports for promising catalysis with high selectivity and maximized metal usage. [4] The synthesis methods have been summarized to prepare SACs with diverse strategies, [5] including atomic layer deposition (ALD), [6] host-guest strategy, [1] wetness impregnation, [7] polymer derived pyrolysis, [8] and so on. Particularly, these isolated SACs have been identified by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy. These synthesized SACs with different metals have been utilized for various catalytic reactions: carbon monoxide (CO) oxidation, [9] organic catalysis, [10] water splitting, [11] hydrogen oxidation reaction, [12] CO 2 reduction, [13] ORR, [14] FAOR, [1] nitrogen reduction reaction (NRR), [15] and lithium-sulfur batteries. [16] Integrated with numerous merits, metal SACs have been considered as an ideal platform to bridge the gap between high-efficiency and low PGMs usage toward fuel cells applications. 1) The highly stable SACs are dominantly determined by the strong chemical bonding between single metal atoms and the substrates.2) The sufficient and uniform electronic and geometric structures make SACs highly specific selectivity in many chemical applications. 3) The high utilization of SACs could significantly minimize the cost of metals, especially for precious metals. 4) The accessibility to regulate the coordination of SACs could trigger intriguingly active properties for catalysis. Hence, the rational combination of single metal sites and supports couldThe commercialization of fuel cells, especially for direct formic acid fuel cells (DFAFCs) and proton-exchange membrane fuel cells (PEMFCs), is significantly restrained by the high cost, poor stability, and sluggish kinetics of platinum group metals (PGM) catalysts for both the anodic formic acid oxidation reaction (FAOR) and the cathodic oxygen reduction reaction (ORR). Currently, it has confronted with challenges, including exploring highly active, cost-effective, and stable catalysts to replace PGM for DFAFCs and PEMFCs. Recently, the increasing investigation has been focused ...

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Section: Metal Organic Framework-derived Carbon Supportsmentioning

confidence: 99%

Section: Improve the Density Of Metal Sacsmentioning

confidence: 99%

Carbon‐Supported Single‐Atom Catalysts for Formic Acid Oxidation and Oxygen Reduction Reactions

Han

Zhang

Yang

et al. 2021

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“…To overcome these issues, the nanocasting of a stabilizer to reduce the surface energy of the metal atoms is a promising synthesis method. For example, the insertion of silicon oxide into the porphyritic metal organic frameworks (MOF) exhibits effectiveness to synthesized SACs 129 . The addition of the protective SiO 2 remarkably increases migration energy gap and consequently prevents the atoms from agglomeration, leading to highly metal loading in the catalyst.…”

Section: Tm/carbon Hybrids For Oxygen Electrocatalystsmentioning

confidence: 99%

Transition metal/carbon hybrids for oxygen electrocatalysis in rechargeable zinc‐air batteries

Douka

Yang

Huang

et al. 2020

EcoMat

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Zinc‐air batteries (ZABs) could be an ideal candidate for challenging energy conversion and storage technology. Usually, the crucial oxygen reduction reaction and oxygen evolution reaction are naturally lethargic and require efficient catalysts to kinetically boost the energy conversion processes to achieve the practicable ZABs application. Transition‐metal/carbon hybrid catalysts show excellent potentials in electrocatalysis, and they have been developed into cost‐effective and scalable oxygen electrocatalyst alternatives for expensive and scarcer noble metal ones in rechargeable ZABs. Herein we summarize recent achievements in transition metal/carbon hybrids for oxygen electrocatalysis. These catalysts mainly fall into two categories by the integrated metal/metal oxides nanoparticles and atomically dispersed transition metal/carbon matrix. We focus on the relationship between structure and performance with their synthesis strategies. Their application in rechargeable ZABs are also comprehensively discussed. Finally, the perspectives on transition metal/carbon hybrids for oxygen electrocatalysis are presented for the future challenges in rechargeable ZABs.

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“…In 2020, the same group reported a similar material, in which SiO 2 was incorporated into the mesopores of PCN-222 [ 86 ]. The above MOF was synthesized as described in ref.…”

Section: Mof-based Orr Electrocatalystsmentioning

confidence: 99%

Synthesis and Performance of MOF-Based Non-Noble Metal Catalysts for the Oxygen Reduction Reaction in Proton-Exchange Membrane Fuel Cells: A Review

et al. 2020

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Hydrogen is widely regarded as a prime energy carrier for bridging the gap between renewable energy supply and demand. As the energy-generating component of the hydrogen cycle, affordable and reliable fuel cells are of key importance to the growth of the hydrogen economy. However, the use of scarce and costly Pt as an electrocatalyst for the oxygen reduction reaction (ORR) remains an issue to be addressed, and in this regard, metal–organic frameworks (MOFs) are viewed as promising non-noble alternatives because of their self-assembly capability and tunable properties. Herein, recent (2018–2020) works on MOF-based electrocatalysts containing N-doped C, Mn, Fe, Co, multiple metals, and multiple sites are reviewed and summarized with a focus on ORR activity, and the principal physicochemical properties and electrochemical performance of these catalysts realized using rotating electrodes are compared.

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Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts

Cited by 390 publications

References 52 publications

Carbon‐Supported Single‐Atom Catalysts for Formic Acid Oxidation and Oxygen Reduction Reactions

Carbon‐Supported Single‐Atom Catalysts for Formic Acid Oxidation and Oxygen Reduction Reactions

Transition metal/carbon hybrids for oxygen electrocatalysis in rechargeable zinc‐air batteries

Synthesis and Performance of MOF-Based Non-Noble Metal Catalysts for the Oxygen Reduction Reaction in Proton-Exchange Membrane Fuel Cells: A Review

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