Manipulating the interaction of Pt NPs with N-hollow carbon spheres by F-doping for boosting oxygen reduction/methanol oxidation reactions

Lv, Chaojie; Cheng, Jiarun; Yang, Yuquan; Wu, Jiwen; Wu, Kaili; Yang, Yunguo; Lau, Woon Ming; Wang, Ning; Pang, Dawei; Zheng, Jinlong

doi:10.1039/d2ta09416a

Cited by 34 publications

(18 citation statements)

References 63 publications

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“…In Figure 2g,h, the valence band maximum ( E v ) and cutoff level ( E cutoff ) were confirmed, and the work function ( Φ ) can be measured via Φ = hv (21.22 eV)− | E f − E cutoff | . [ 20 ] These results indicate that the E v of Fe and F co‐doping NiO catalyst is 3.04 eV, higher than that of NiO (2.69 eV), which also means that electrons are more likely to jump and excite to the conduction band, speeding up electron transport (Figure 2i). At the same time, the Φ of Fe, F‐NiO (3.66 eV) is also much smaller than that of NiO (4.11 eV), which further verifies that Fe and F dual‐doping optimizes the electronic structure of NiO catalyst, and makes the Fermi level of the system closer to the vacuum level, eventually effectively enhance the charge transfer ability, weaken the OER energy barrier, and accelerate reaction kinetics.…”

Section: Resultsmentioning

confidence: 97%

Dual Atoms (Fe, F) Co‐Doping Inducing Electronic Structure Modulation of NiO Hollow Flower‐Spheres for Enhanced Oxygen Evolution/Sulfion Oxidation Reaction Performance

Lyu

Cheng

et al. 2023

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Heteroatoms Fe, F co‐doped NiO hollow spheres (Fe, F‐NiO) are designed, which simultaneously integrate promoted thermodynamics by electronic structure modulation with boosted reaction kinetics by nano‐architectonics. Benefiting from the electronic structure co‐regulation of Ni sites by introducing Fe and F atoms in NiO , as the rate‐determined step (RDS), the Gibbs free energy of OH* intermediates (ΔGOH*) for Fe, F‐NiO catalyst is significantly decreased to 1.87 eV for oxygen evolution reaction (OER) compared with pristine NiO (2.23 eV), which reduces the energy barrier and improves the reaction activity. Besides, densities of states (DOS) result verifies the bandgap of Fe, F‐NiO(100) is significantly decreased compared with pristine NiO(100), which is beneficial to promote electrons transfer efficiency in electrochemical system. Profiting by the synergistic effect, the Fe, F‐NiO hollow spheres only require the overpotential of 215 mV for OER at 10 mA cm−2 and extraordinary durability under alkaline condition. The assembled Fe, F‐NiO||Fe‐Ni2P system only needs 1.51 V to reach 10 mA cm−2, also exhibits outstanding electrocatalytic durability for continuous operation. More importantly, replacing the sluggish OER by advanced sulfion oxidation reaction (SOR) not only can realize the energy saving H2 production and toxic substances degradation, but also bring additional economic benefits.

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Section: Resultsmentioning

confidence: 97%

Dual Atoms (Fe, F) Co‐Doping Inducing Electronic Structure Modulation of NiO Hollow Flower‐Spheres for Enhanced Oxygen Evolution/Sulfion Oxidation Reaction Performance

Lyu

Cheng

et al. 2023

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“…The Pt 4f spectra of Pt&Fe 2 O 3 /NC and Pt&CoO/NC are shown in Figure c. There are two Pt valence states, namely, Pt 0 and Pt 2+ , in these two catalysts: the peaks at 72.4 and 77.2 eV belong to Pt 2+ , and the other two peaks at 71.7 and 75.1 eV are assigned to Pt 0 . − Compared to Pt/NC, there is a negative shift (approximately 0.7 eV) in Pt owing to the change in the electronic structure of Pt in the presence of the metal oxides, which weakens the binding energy of oxygen and thereby enhances the catalytic activity of Pt. − …”

Section: Resultsmentioning

confidence: 99%

Collaborative Anchoring of Pt Nanoparticles and Metal Oxide Nanoparticles on N-Doped Carbon as Catalysts for Oxygen Reduction

Zhang

Zhou

et al. 2023

ACS Appl. Nano Mater.

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Platinum (Pt)-based catalysts are the most widely used catalysts for the oxygen reduction reaction (ORR). However, there are still great challenges to overcome in improving catalyst activity and reducing the use of Pt. Herein, catalysts with Pt nanoparticles and metal oxide nanoparticles on N-doped carbon with ultralow Pt loading (<2 wt % Pt), namely, Pt&Fe 2 O 3 /NC and Pt&CoO/NC, are synthesized by a two-step pyrolysis method, in which N-doped carbon is first prepared by pyrolyzing carbon and melamine at 900 °C and Pt nanoparticles and metal oxide nanoparticles are then prepared by pyrolyzing a Pt salt and M(OH) x (M = Fe, Co) at 700 °C. The Pt and metal oxide are uniformly dispersed on the NC, resulting in ultrafine Pt nanoparticles (∼2 nm). Metal oxides regulate the electronic structure of Pt to weaken the binding energy of oxygen. Both Pt&Fe 2 O 3 /NC and Pt&CoO/NC show good ORR catalytic activities in alkaline solution. Pt&Fe 2 O 3 /NC shows the ORR catalytic performance, with the peak potential and half-wave potential at 0.883 and 0.862 V, better than those of Pt&CoO/NC (0.861 and 0.842 V) and Pt/NC (0.856 and 0.838 V) and comparable to that of commercial 20 wt % Pt/C. The ORR mechanism on these two catalysts involves a direct four-electron path. This provides a method for improving the ORR catalytic performance of catalysts with ultralow Pt loading via the joint anchoring of ultrafine Pt by metal oxides and NC, resulting in synergistic interactions.

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“…4,5 To reduce the utilization of Pt and still maintain its outstanding activity, Pt alloys have been extensively studied. [6][7][8] As electrochemical reactions usually take place on the surface of catalysts, it is important to study the surface Pt reactive sites of the Pt alloy. [9][10][11][12] X-ray absorption spectroscopy (XAFS) and spherical-aberrationcorrected transmission electron microscopy (SACTEM) have advanced in study of coordination environments and surface atomic structure, but it is still challenging to identify the practical active sites because of the lack of effective research tools to detect intermediate species.…”

Section: Introductionmentioning

confidence: 99%

Revealing surface fine structure on PtAu catalysts by an in situ ATR-SEIRAS CO-probe method

Li¹,

An²,

Yang³

et al. 2023

J. Mater. Chem. A

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Manipulating the interaction of Pt NPs with N-hollow carbon spheres by F-doping for boosting oxygen reduction/methanol oxidation reactions

Abstract: The highly dispersed Pt NPs anchored in hierarchically N, F co-doped hollow carbon spheres (Pt@N, F-HCS) was synthesized through a template-assisted strategy followed by fluorination and wet chemical reduction. Attributing...

Cited by 34 publications

References 63 publications

Dual Atoms (Fe, F) Co‐Doping Inducing Electronic Structure Modulation of NiO Hollow Flower‐Spheres for Enhanced Oxygen Evolution/Sulfion Oxidation Reaction Performance

Dual Atoms (Fe, F) Co‐Doping Inducing Electronic Structure Modulation of NiO Hollow Flower‐Spheres for Enhanced Oxygen Evolution/Sulfion Oxidation Reaction Performance

Collaborative Anchoring of Pt Nanoparticles and Metal Oxide Nanoparticles on N-Doped Carbon as Catalysts for Oxygen Reduction

Revealing surface fine structure on PtAu catalysts by an in situ ATR-SEIRAS CO-probe method

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