Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

Sun, Ying; Deng, Zizhao; Song, Xi‐Ming; Li, Hui; Huang, Zi‐Hang; Zhao, Qin; Feng, Daming; Zhang, Wei; Liu, Zhao‐Qing; Ma, Tianyi

doi:10.1007/s40820-020-00444-y

Cited by 55 publications

(36 citation statements)

References 52 publications

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“…Reproduced with permission. [ 245 ] Copyright 2020, Springer. h) N 2 absorption in a hydrophobic membrane using FAS modification on catalyst; i) d‐band center of np‐Mo 4 P 3 and FAS‐modification of np‐Mo 4 P 3 ; j) Schematic of d‐band center distance from fermi‐level; k) Lower d‐band of np‐Mo 4 P 3 to weaken H adsorption.…”

Section: Gas‐involved Single Function Electrocatalystsmentioning

confidence: 99%

“…Bi 2 O 3 /FEG manifests excellent catalytic performance (Figure 11f,g) and long‑term stability toward NRR because of its strong interaction of Bi 6p band with the N 2p orbitals, binder‑free framework, and excellent electrical conductivity. [ 245 ] We and co‐workers [ 250 ] successfully anchored gold nanoparticles on bismuth sulfide nanorods (Au(111)@Bi 2 S 3 NRs). The N‐philic nature of Bi and the unique mutual coordination components greatly promoted the nitrogen adsorption by facilitating the formation of the intermediate N 2 H*.…”

Section: Gas‐involved Single Function Electrocatalystsmentioning

confidence: 99%

“…e) Schematic of the synthesis of Bi 2 O 3 /FEG; f) FE and NH 3 yield rate determined by the Nessler's reagent; g) FE and NH 3 yield rate determined by ion-selective electrode meter. Reproduced with permission [245]. Copyright 2020, Springer.…”

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confidence: 99%

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Self‐Supporting Electrodes for Gas‐Involved Key Energy Reactions

Wang

Zang

Xuan

et al. 2021

Adv Funct Materials

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Self‐supporting materials are widely adopted in gas‐involved electrocatalysis during the past few decades because of their unique physical/electrochemical properties, especially the stabilized spatial framework and the large electrochemical interfaces. Reportedly, there is no clear definition to define “self‐supporting” materials, and also, no such comprehensive reviews have fully discussed the self‐supporting materials in gas‐involved electrochemical applications. Therefore, it is necessary to provide timely updates in this potential field. In this review, for the first time, a reasonable definition of self‐supporting materials and comprehensively review the recent research progress of related electrodes in gas‐involved electrocatalytic applications is given. Firstly, it is discussed their synthetic methodologies, including design principles, different types of substrates‐ and substrate‐free structures. Subsequently, the recent advances of self‐supporting electrodes for gas‐involved key energy related electrocatalysis (i.e., hydrogen evolution, oxygen reduction, oxygen evolution, nitrogen reduction, and carbon dioxide reduction reactions) and their practical applications in water‐splitting, fuel cells and metal‐air batteries are mainly presented. Finally, a summary of the progress of self‐supporting electrocatalysts, the remaining challenges, and the perspectives are given to instruct their future development. It is expected that this review will provide new research insights for the future development of renewable energy storage and conversion systems.

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Section: Gas‐involved Single Function Electrocatalystsmentioning

confidence: 99%

Section: Gas‐involved Single Function Electrocatalystsmentioning

confidence: 99%

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Self‐Supporting Electrodes for Gas‐Involved Key Energy Reactions

Wang

Zang

Xuan

et al. 2021

Adv Funct Materials

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“…[ 1–3 ] As matters stand, the industrial capital route of ammonia synthesis Haber–Bosch process has consumed exceed 1% of the world energy supply and discharged large amounts of greenhouse gas. [ 4 ] Different from the Haber–Bosch technology required high temperatures (400–500 °C) and pressures (200–300 atm), the mild approaches for nitrogen fixation such as homogeneous catalysis with organic or reductive agents, [ 5,6 ] electrocatalysis, [ 7–10 ] nitrogenase catalysis, [ 11,12 ] and photocatalysis [ 13–15 ] are promising alternatives. Amongst, the electrochemical nitrogen reduction reaction (eNRR) has gained much attention, since it takes water and air as the synthetic source and could be powered by renewable electricity.…”

Section: Introductionmentioning

confidence: 99%

Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance

Liao

Wang

et al. 2021

Adv Funct Materials

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Electrochemical nitrogen reduction reaction (eNRR) is recognized as a promising approach for ammonia synthesis, which is, however, impeded by the inert nitrogen and the unavoidable competing hydrogen evolution reaction (HER). Here, a Mo-PTA@CNT electrocatalyst in which Mo species are anchored on the fourfold hollow sites of phosphotungstic acid (PTA) and closely embedded in multi-walled carbon nanotubes (CNT) for immobilization is designed and synthesized. Interestingly, the catalyst presents a high ammonia yield rate of 51 ± 1 µg h −1 mg cat.−1 and an excellent Faradaic efficiency of 83 ± 1% at −0.1 V versus RHE under ambient conditions. The concentrations of NH 4 + are also quantitatively calculated by 1 H NMR spectra and ion chromatography. Isotopic labeling identifies that the N atom of the formed NH 3 originates from N 2 . The controlled experiments confirm a strong interaction between Mo-PTA and N 2 with an adsorption energy of 50.46 kJ mol −1 and activation energy of 21.36 kJ mol −1 . More importantly, due to CNT's gas storage and hydrophobicity properties, there is a fourfold increase in N 2 content. The concentration of H 2 O is reduced by more than half at the interface of the electrode. Thus, the activity of eNRR can be significantly improved with ultrahigh electron selectivity.

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“…Extensive efforts have been made to advance the electrochemical ammonia synthesis (

N_{2} + 3 H_{2} normalO \to 2 {NH}_{3} + 3 / 2 O_{2}

) 6‐14 . Water splitting is a key step to provide hydrogen for nitrogen protonation (

* N_{2} + 6 H^{+} + 6 e^{-} \to * + 2 {NH}_{3}

).…”

Section: Introductionmentioning

confidence: 99%

Boosting electrocatalytic nitrogen reduction to ammonia in alkaline media

Lin

Pan

et al. 2021

Int J Energy Res

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Summary Electrochemical ammonia synthesis is a promising alternative technique to traditional Haber‐Bosch process, capable of converting nitrogen to ammonia at ambient conditions and can be driven by intermittent energy. However, it generally requires high overpotential for nitrogen dissociation due to the stable triple bonds of nitrogen molecules, resulting in a poor ammonia yield rate. Tailoring the electrolyte‐ion composition is a promising approach to facilitate nitrogen dissociation by optimizing the local reaction environment near the electrode toward ammonia production. In this study, the effect of anions in the electrolyte composition on electrocatalytic nitrogen reduction to ammonia is investigated. It is found that a lower onset potential for nitrogen reduction (−0.2 V vs RHE) and a higher ammonia yield rate (6.69 × 10−11 mol cm−2 s−1) are achieved in the electrolyte containing OH− anions, compared to singly charged anions of Cl− and SCN− when using an electrode made of commercial Au/C electrocatalysts. In addition, current density contributed by nitrogen reduction achieved in the high‐pH electrolyte (pH ≥ 13) shows around 3‐fold increase compared to that in low‐pH electrolyte (11 ≤ pH ≤ 12). Such performance enhancement is possibly attributed to the appearance of hydronium ions (H3O+) in high‐pH electrolyte, which facilitates nitrogen dissociation by strengthening protonation(*N2+6H3O++6e−→*+2NH3·H2normalO+4H2normalO).

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Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

Cited by 55 publications

References 52 publications

Self‐Supporting Electrodes for Gas‐Involved Key Energy Reactions

Self‐Supporting Electrodes for Gas‐Involved Key Energy Reactions

Interfacial Engineering Promoting Electrosynthesis of Ammonia over Mo/Phosphotungstic Acid with High Performance

Boosting electrocatalytic nitrogen reduction to ammonia in alkaline media

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