Phytic acid-guided ultra-thin N,P co-doped carbon coated carbon nanotubes for efficient all-pH electrocatalytic hydrogen evolution

Xiao, Fei; Chen, Zhimin; Wu, Hao; Wang, Ying; Cao, Enhong; Lu, Xiaodong; Wu, Yiqun; Ren, Zhiyu

doi:10.1039/c9nr07362k

Cited by 38 publications

(20 citation statements)

References 69 publications

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“…Currently, the development of superior electrocatalysts with earth-abundant elements for the HER has become a research priority. Among these studies, due to admirable electronic conductivity, vigorous stability, and environmental friendliness 4 , many works are centralized on carbon-based materials with various nanostructures, such as carbon nanotubes (CNTs) 5 , carbon nanosheets 6 , hollow carbons 7 , and g-C 3 N 4 -based materials 8 . Commonly, heteroatoms such as N, P, B, and S are doped into carbonbased materials to optimize their electrocatalytic performances 9 .…”

Section: Introductionmentioning

confidence: 99%

Tailoring the d-band center of N-doped carbon nanotube arrays with Co4N nanoparticles and single-atom Co for a superior hydrogen evolution reaction

et al. 2021

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A 3D self-supported integrated electrode, consisting of heteroatomic nitrogen-doped carbon nanotube arrays on carbon cloth with confined ultrafine Co4N nanoparticles and a distribution of anchored single-atom Co, is fabricated via a cobalt-catalyzed growth strategy using dicyandiamide as the nitrogen and carbon source and a layered cobalt hydroxide-nitrate salt as the precursor. The abundance of exposed active sites, namely, the Co4N nanoparticles, single-atom Co, and heteroatomic N-doped carbon nanotubes, and multiple synergistic effects among these components provide suitable tailoring of the d-band center for facilitating vectorial electron transfer and efficient electrocatalysis. Benefiting from the merits of its structural features and electronic configuration, the prepared electrode exhibits robust performance toward the hydrogen evolution reaction with overpotentials of only 78 and 86 mV at 10 mA cm−2 in acidic and basic electrolytes, respectively. Density functional theory calculations and X-ray photoelectron spectroscopy valence band measurements reveal that the effective tailoring of the d-band center by Co4N nanoparticles plays a crucial role in optimizing the hydrogen adsorption free energy to a more thermoneutral value for efficient electrocatalysis.

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Section: Introductionmentioning

confidence: 99%

Tailoring the d-band center of N-doped carbon nanotube arrays with Co4N nanoparticles and single-atom Co for a superior hydrogen evolution reaction

et al. 2021

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“…The comparison between the control material PANI-TS-TC ( Figure 5 a1,a2) and those containing the metallic species PANI-Ni-TS-TC ( Figure 5 b1,b2) and PANI-Co-TS-TC ( Figure 5 c1,c2) shows the presence of micro-structured particles of different shape and size. For polyaniline-based materials, it is known that the thermal treatment under an inert atmosphere of argon or nitrogen at 600–1200 °C will trigger the rearrangement of the different atoms to create new bonds of carbon–carbon (C-C, C=C, C-H) and carbon–nitrogen (pyridinic-N, pyrrolic-N, and graphitic-N) in a nanostructured network that has different levels of electrical conductivity, number of active sites and electrocatalytic kinetics [ 18 , 20 , 54 , 55 , 56 , 57 , 58 ]. In order to obtain a qualitative analysis of the nature of the structures formed with metallic species, in-depth analysis was conducted by EDX.…”

Section: Resultsmentioning

confidence: 99%

Probing Oxygen-to-Hydrogen Peroxide Electro-Conversion at Electrocatalysts Derived from Polyaniline

et al. 2022

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Hydrogen peroxide (H2O2) is a key chemical for many industrial applications, yet it is primarily produced by the energy-intensive anthraquinone process. As part of the Power-to-X scenario of electrosynthesis, the controlled oxygen reduction reaction (ORR) can enable the decentralized and renewable production of H2O2. We have previously demonstrated that self-supported electrocatalytic materials derived from polyaniline by chemical oxidative polymerization have shown promising activity for the reduction of H2O to H2 in alkaline media. Herein, we interrogate whether such materials could also catalyze the electro-conversion of O2-to-H2O2 in an alkaline medium by means of a selective two-electron pathway of ORR. To probe such a hypothesis, nine sets of polyaniline-based materials were synthesized by controlling the polymerization of aniline in the presence or not of nickel (+II) and cobalt (+II), which was followed by thermal treatment under air and inert gas. The selectivity and faradaic efficiency were evaluated by complementary electroanalytical methods of rotating ring-disk electrode (RRDE) and electrolysis combined with spectrophotometry. It was found that the presence of cobalt species inhibits the performance. The selectivity towards H2O2 was 65–80% for polyaniline and nickel-modified polyaniline. The production rate was 974 ± 83, 1057 ± 64 and 1042 ± 74 µmolH2O2 h−1 for calcined polyaniline, calcined nickel-modified polyaniline and Vulcan XC 72R (state-of-the-art electrocatalyst), respectively, which corresponds to 487 ± 42, 529 ± 32 and 521 ± 37 mol kg−1cat h−1 (122 ± 10, 132 ± 8 and 130 ± 9 mol kg−1cat cm−2) for faradaic efficiencies of 58–78%.

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“…Finally, the metal content of about 30 wt % is in agreement with the theoretical expectation by considering the mineralization yield of our protocol. It is known that during the calcination, the rearrangement of the different atoms from the starting materials produces the bonds such as carbon-carbon (C-C, C=C, C-H) and carbon-nitrogen (pyridinic-N, pyrrolic-N, and graphitic-N) within a porous-like structure that contribute to the performance by the electrical conductivity, the electrocatalytic kinetics and the high number of active sites [ 42 , 49 , 50 , 51 , 52 , 53 , 54 ]. Our previous and extensive study (SEM, EDX, TGA-DSC, XPS, BET, XRD, etc.)…”

Section: Resultsmentioning

confidence: 99%

Insights on the Electrocatalytic Seawater Splitting at Heterogeneous Nickel-Cobalt Based Electrocatalysts Engineered from Oxidative Aniline Polymerization and Calcination

et al. 2021

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Given the limited access to freshwater compared to seawater, a growing interest surrounds the direct seawater electrolysis to produce hydrogen. However, we currently lack efficient electrocatalysts to selectively perform the oxygen evolution reaction (OER) over the oxidation of the chloride ions that are the main components of seawater. In this contribution, we report an engineering strategy to synthesize heterogeneous electrocatalysts by the simultaneous formation of separate chalcogenides of nickel (NiSx, x = 0, 2/3, 8/9, and 4/3) and cobalt (CoSx, x = 0 and 8/9) onto a carbon-nitrogen-sulfur nanostructured network. Specifically, the oxidative aniline polymerization in the presence of metallic cations was combined with the calcination to regulate the separate formation of various self-supported phases in order to target the multifunctional applicability as both hydrogen evolution reaction (HER) and OER in a simulated alkaline seawater. The OER’s metric current densities of 10 and 100 mA cm−2 were achieved at the bimetallic for only 1.60 and 1.63 VRHE, respectively. This high-performance was maintained in the electrolysis with a starting voltage of 1.6 V and satisfactory stability at 100 mA over 17 h. Our findings validate a high selectivity for OER of ~100%, which outperforms the previously reported data of 87–95%.

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Phytic acid-guided ultra-thin N,P co-doped carbon coated carbon nanotubes for efficient all-pH electrocatalytic hydrogen evolution

Abstract: An ultra-thin N, P co-doped carbon (NPC) was constructed on CNT by selecting phytic acid as a “guide”. The obtained CNT@NPC performs as an efficient and robust metal-free electrocatalyst for pH-universal hydrogen evolution reaction.

Cited by 38 publications

References 69 publications

Tailoring the d-band center of N-doped carbon nanotube arrays with Co4N nanoparticles and single-atom Co for a superior hydrogen evolution reaction

Tailoring the d-band center of N-doped carbon nanotube arrays with Co4N nanoparticles and single-atom Co for a superior hydrogen evolution reaction

Probing Oxygen-to-Hydrogen Peroxide Electro-Conversion at Electrocatalysts Derived from Polyaniline

Insights on the Electrocatalytic Seawater Splitting at Heterogeneous Nickel-Cobalt Based Electrocatalysts Engineered from Oxidative Aniline Polymerization and Calcination

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