Sulfur defect-rich WS2−x nanosheet electrocatalysts for N2 reduction

Ma, Liangyu; Kong, Wenhan; Liu, Mengli; Jin, Zhaoyong; Han, Yaqian; Sun, Jie; Liu, Jie; Xu, Yuanhong; Li, Jinghong

doi:10.1007/s40843-020-1572-3

Cited by 17 publications

(5 citation statements)

References 44 publications

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“…The NO adsorption configurations over both pristine and defective (with chalcogen vacancy) TMD surfaces and the corresponding adsorption energies are shown in Figure S1 and Table S1 (see ESI), respectively. For all the five TMD monolayers, the reported most stable vacancies are chalcogen vacancy [22h–j,l,m,24,40] . The most stable NO adsorption at a vacancy site is always through the N end and is much stronger than on the perfect surface.…”

Section: Resultsmentioning

confidence: 93%

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

Tursun

2021

ChemElectroChem

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Nitric oxide electroreduction reaction (NOER) is one of the most attractive routes for ammonia synthesis and NOx‐related pollutant treatment. However, current research on NOER catalysts mainly focus on noble metals and single atom catalysts, while low‐cost transition metal dichalcogenides (TMDs) are rarely considered, let alone their product selectivity. Herein, using first‐principles calculations, we systematically investigate the performance of a series of single‐layer TMDs (MoS2, MoSe2, MoTe2, TaTe2 and WTe2) in the 1T’ phase as electrocatalysts for NOER. Our results reveal that defective 1T’‐MoS2 and 1T’‐MoSe2 monolayers (with the most common sulphur and selenium vacancies, respectively) exhibit excellent activity for NOER as well as high selectivity for ammonia, which can be correspondingly yielded at 0 and −0.06 V potentials, comparable to the best Pt‐based and single atom catalysts. Furthermore, these two catalysts efficiently suppress the competing hydrogen evolution reaction (HER). Thus, single‐layer TMDs synthesized with chalcogen vacancies may serve as efficient catalysts for electrochemical ammonia synthesis from pollutants and electrocatalytic denitrification.

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Section: Resultsmentioning

confidence: 93%

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

Tursun

2021

ChemElectroChem

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“…This was determined by analyzing the CV curves within the range of ∼0.26–0.36 V vs RHE, as depicted in Figure d,e. Furthermore, the high C dl value of 31.75 mF cm –2 (Figure e) indicates that Fe SAC -N-C possesses a high ECSA, which is beneficial for the NRR process. − To further investigate the origin of the observed NRR activity of the Fe SAC -N-C catalyst, its Nyquist plot (Figure f) unraveled a narrower capacitance arc at −0.1 V vs RHE than that of the C–N, verifying the rapid charge transfer, and thus the better catalytic efficacy. Notably, the Fe SAC -N-C electrocatalyst exhibited a higher angle for the linear curve in the low frequency region when compared to that of the C–N counterpart.…”

Section: Resultsmentioning

confidence: 92%

Fe-Single-Atom Catalysts on Nitrogen-Doped Carbon Nanosheets for Electrochemical Conversion of Nitrogen to Ammonia

Agour,

Elkersh,

Khedr

et al. 2023

ACS Appl. Nano Mater.

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Electrochemical nitrogen reduction reaction (NRR) has been established as a promising and sustainable alternative to the Haber−Bosch process, which requires intensive energy to produce ammonia. Unfortunately, NRR is constrained by the high adsorption/activation of the N 2 energy barrier and the competing hydrogen evolution reaction, resulting in low faradic efficiency. Herein, a well-dispersed iron single-atom catalyst was successfully immobilized on nitrogen-doped carbon nanosheets (Fe SAC -N-C) synthesized from pre-hydrothermally derived Fe-doped carbon quantum dots with an average particle size of 2.36 nm and used for efficient electrochemical N 2 fixation at ambient conditions. The as-synthesized Fe SAC -N-C catalyst records an onset potential of 0.12 V RHE , exhibiting a considerable faradic efficiency of 23.7% and an NH 3 yield rate of 3.47 μg h −1 cm −2 in aqueous 0.1 M KOH electrolyte at a potential of −0.1 V RHE under continuous N 2 feeding conditions. The control experiments assert that the produced NH 3 molecules only emerge from the dissolved N 2 -gas, reflecting the remarkable stability of the nitrogen−carbon framework during electrolysis. The DFT calculations showed the Fe SAC -N-C catalyst to demonstrate a lower energy barrier during the rate-limiting step of the NRR process, consistent with the observed high activity of the catalyst. This study highlights the exceptional potential of single-atom catalysts for electrochemical NRR and offers a comprehensive understanding of the catalytic mechanisms involved. Ultimately, this work provides a facile synthesis strategy of Fe SAC -N-C nanosheets with high atomic-dispersion, creating a novel design avenue of Fe SAC -N-C that can vividly have a potential applicability in the large spectrum of electrocatalytic applications.

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“…S16 in the ESM) After the stability test, Ni maintained its valence state. For the S 2p spectra, the peak at 163.5 eV is assigned to the S-Ni species, and the peaks at 169.0 eV were assigned to the oxidized S [62]. It is found that Ni 3 S 2 NWs have a large portion of oxidized S species, which may cause by the rich defects in the NWs.…”

Section: The Ethanol Upgrading Activities Of the Ni 3 S 2 Nwsmentioning

confidence: 97%

“…It is found that Ni 3 S 2 NWs have a large portion of oxidized S species, which may cause by the rich defects in the NWs. The defect sites are easier to be oxides and thus lead to higher ethanol upgrading activity [62,63].…”

Section: The Ethanol Upgrading Activities Of the Ni 3 S 2 Nwsmentioning

confidence: 99%

Defective Ni3S2 nanowires as highly active electrocatalysts for ethanol oxidative upgrading

et al. 2021

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Electrochemical upgrading of biomass ethanol to value-added chemicals is promising for sustainable society. Here, we synthesize defective Ni 3 S 2 nanowires (NWs), which show high activity towards electrochemical oxidation of ethanol to acetate. The Ni 3 S 2 NWs are formed by the oriented attachment mechanism, and rich defects are introduced during the growth. A low onset potential of 1.31 V and high mass activity of 8,716 mA•mg Ni −1 at 1.5 V are achieved using the synthesized Ni 3 S 2 NWs toward the ethanol electro-oxidation, which are better than the Ni(OH) 2 NWs and the Ni 3 S 2 nanoparticles (NPs). And the selectivity for the acetate generation is ca. 99%. The high activity of Ni 3 S 2 NWs is attributed to the easier oxidation of Ni(II) to the catalytically active Ni(III) species with the promotion from S component and rich defects. These results demonstrate that the defective NWs can be synthesized by the oriented attachment method and the defective Ni 3 S 2 NWs structure as the efficient nonnoble metal electrocatalysts for oxidative upgrading of ethanol.

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Sulfur defect-rich WS2−x nanosheet electrocatalysts for N2 reduction

Cited by 17 publications

References 44 publications

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

NO Electroreduction by Transition Metal Dichalcogenides with Chalcogen Vacancies

Fe-Single-Atom Catalysts on Nitrogen-Doped Carbon Nanosheets for Electrochemical Conversion of Nitrogen to Ammonia

Defective Ni3S2 nanowires as highly active electrocatalysts for ethanol oxidative upgrading

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