Highly accessible and dense surface single metal FeN<sub>4</sub> active sites for promoting the oxygen reduction reaction

Chen, Guangbo; An, Yun; Liu, Shengwen; Sun, Fanfei; Qi, Haoyuan; Wu, Haofei; He, Yanghua; Chen, Mingwei; Shi, Run; Zhang, Jian; Kuc, Agnieszka; Kaiser, Ute; Zhang, Tierui; Heine, Thomas; Wu, Gang; Feng, Xinliang

doi:10.1039/d2ee00542e

Cited by 98 publications

(53 citation statements)

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“…29 Increasing the surface area of the materials to increase the abundant surface metal anchoring sites is another strategy. 30 In this work, the content of Co−N x active sites increases upon the increase of Au addition, and we believe that this is because that the Au component addition can change the Co coordination environment and promote the dispersion of Co atoms. A similar result was also observed in the Pt single atom (SA)-modified Pd cluster catalyst, and it was found that the addition of trace amounts of Pt SAs in fully exposed Pd clusters could reduce the coordination numbers of Pd−O and Pd−Pd shells, indicating that the addition of trace Pt SAs could change the coordination environment of Pd atoms.…”

Section: Active Center Identificationmentioning

confidence: 65%

“…A strategy such as adding an additional nitrogen source such as melamine in the high-temperature pyrolysis process is usually used . Increasing the surface area of the materials to increase the abundant surface metal anchoring sites is another strategy . In this work, the content of Co–N x active sites increases upon the increase of Au addition, and we believe that this is because that the Au component addition can change the Co coordination environment and promote the dispersion of Co atoms.…”

Section: Resultsmentioning

confidence: 85%

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Regulation of the Co–N_x Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Wang

Zhang

et al. 2022

ACS Catal.

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The Co–N x active sites play a critical role over the Co@NC catalyst in the heterogeneous catalysis. However, the effective methods for the regulation of the content and electronic structure of Co–N x active sites to enhance the catalytic efficiency of heterogeneous catalysts are still insufficient. Herein, a nitrogen-doped porous carbon-encapsulated Au-doped Co nanoparticle catalysts with abundant and electron-rich Co–N x sites in the outer carbon layer was designed by a Au doping strategy through pyrolysis of the HAuCl4-modified ZIF-67 metal organic framework precursor. The optimal catalyst exhibits improved catalytic performance in alcohol selective oxidative esterification. The linear relationship between the ester yield and Co–N x species content, combined with a series of control experiments, indicated that the Co–N x active sites are crucial for achieving the excellent catalytic activity (yield: 99.9%). In situ diffuse reflectance infrared Fourier transform spectroscopy, O2-temperature-programed desorption characterizations, active oxygen species quenching experiments together with density functional theory calculations results indicate that Au doping in the Co nanoparticle core increases the content and the electron density of Co–N x species on the outer carbon shell, which enhanced the chemical adsorption and activation of molecular O2 for producing reactive O2 •– species. This study demonstrated a novel Co–N x active site regulation strategy for the efficient selective oxidative esterification of alcohols under mild reaction conditions.

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Section: Active Center Identificationmentioning

confidence: 65%

Section: Resultsmentioning

confidence: 85%

Regulation of the Co–N_x Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Wang

Zhang

et al. 2022

ACS Catal.

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“…S10 †) of CoSA@NPC, NS-NPC and NI-NPC, they can be resolved as C]C (sp 2 ), C-C (sp 3 ), C-N/C-O, and C]O. 35 It is worth mentioning that the sp 3 /sp 2 ratio of CoSA@NPC is 0.603, which is larger than that of NI-NPC (0.495) and NS-NPC (0.482) (Fig. S11 and Table S3 †), verifying the higher defect/edge level 36 in CoSA@NPC.…”

Section: †)mentioning

confidence: 99%

Atomically dispersed Co in a cross-channel hierarchical carbon-based electrocatalyst for high-performance oxygen reduction in Zn–air batteries

Liu

Wang

et al. 2022

J. Mater. Chem. A

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“…). , In addition, compared with traditional precursors of M–N/C catalysts, zeolitic imidazolate frameworks (ZIFs) are ideal precursors for preparation of single-atom catalysts due to their multiple advantages, such as periodicity, high uniformity, and single-atomic dispersion of metal centers in ZIFs. , Atomically dispersed transition metal/nitrogen-doped carbon materials derived from MOFs have been a research hotspot in electrocatalysis . Besides, silica is usually regarded as one kind of potential template for preparation of Fe–N/C catalysts. − …”

Section: Introductionmentioning

confidence: 99%

Atomically Dispersed FeN₂ at Silica Interfaces Coupled with Rich Nitrogen Doping-Hollow Carbon Nanospheres as Excellent Oxygen Reduction Reaction Catalysts

Zhao

et al. 2022

ACS Appl. Energy Mater.

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A SiO2-assisted strategy is a promising approach to prepare high-performance oxygen reduction reaction (ORR) catalysts. In this work, atomically dispersed FeN2 on rich nitrogen doping-hollow carbon nanosphere catalysts were prepared by silica interface assists. The Fe–N/C@SiO2 catalysts with an ultrathin SiO2 layer (∼3 nm) were derived from ZIF-8@Fe/SiO2 composites. A porous SiO2 thin layer was wrapped on a ZIF-8 surface while loading Fe atoms inside silica by one-step synthesis. Different from the conventional synthetic strategy, no additional post-treatments such as etching of SiO2 coatings and second pyrolysis are required. The ORR activity and stability are highly dependent on the thickness of the SiO2 layer. The rigid SiO2 layer not only traps the volatile nitrogen species on the surface to achieve a high nitrogen doping (11.14%) but also prevents the ZIF framework from collapse, forming hierarchical porous structures. Also more importantly, single Fe atoms are anchored in situ on the outer surface of the catalysts in the form of FeN2 configuration, thus greatly boosting the ORR activities. Remarkable stability (only 1% activity attenuation after 14 h of operation) is achieved in alkaline media due to the assist of inactive silica layers.

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Highly accessible and dense surface single metal FeN₄ active sites for promoting the oxygen reduction reaction

Abstract: Single iron atom and nitrogen-codoped carbon (Fe-N-C) electrocatalysts, which have great potential to catalyze the kinetically sluggish oxygen reduction reaction (ORR), have been recognized to be the most promising replacements...

Cited by 98 publications

References 58 publications

Regulation of the Co–N_x Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Regulation of the Co–N_x Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Atomically dispersed Co in a cross-channel hierarchical carbon-based electrocatalyst for high-performance oxygen reduction in Zn–air batteries

Atomically Dispersed FeN₂ at Silica Interfaces Coupled with Rich Nitrogen Doping-Hollow Carbon Nanospheres as Excellent Oxygen Reduction Reaction Catalysts

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Highly accessible and dense surface single metal FeN4 active sites for promoting the oxygen reduction reaction

Abstract: Single iron atom and nitrogen-codoped carbon (Fe-N-C) electrocatalysts, which have great potential to catalyze the kinetically sluggish oxygen reduction reaction (ORR), have been recognized to be the most promising replacements...

Cited by 98 publications

References 58 publications

Regulation of the Co–Nx Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Regulation of the Co–Nx Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Atomically dispersed Co in a cross-channel hierarchical carbon-based electrocatalyst for high-performance oxygen reduction in Zn–air batteries

Atomically Dispersed FeN2 at Silica Interfaces Coupled with Rich Nitrogen Doping-Hollow Carbon Nanospheres as Excellent Oxygen Reduction Reaction Catalysts

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Highly accessible and dense surface single metal FeN₄ active sites for promoting the oxygen reduction reaction

Regulation of the Co–N_x Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Regulation of the Co–N_x Active Sites of MOF-Templated Co@NC Catalysts via Au Doping for Boosting Oxidative Esterification of Alcohols

Atomically Dispersed FeN₂ at Silica Interfaces Coupled with Rich Nitrogen Doping-Hollow Carbon Nanospheres as Excellent Oxygen Reduction Reaction Catalysts