Achieving reaction pathway separation for electrochemical nitrate fixation on triatomic catalysts: A new mechanism

Yang, Lei; Feng, Shenghua; Zhu, Weihua

doi:10.1016/j.jhazmat.2022.129972

Cited by 14 publications

(10 citation statements)

References 36 publications

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“…2(c), which is well-known as the "donorcontribution" view. 5,33,42,[46][47][48][49] To compensate, the partial density of states (PDOS) of the NO-p and FeMoMo-d orbitals before and aer the NO adsorption were analyzed to unveil the TM-NO interactions. As shown in Fig.…”

Section: Resultsmentioning

confidence: 99%

“…† Note that, with the assistance of ternary steric hindrance synergism and enhanced N-terminal collision probability, the NO monomer seems to prefer to bond with the TM sites using its N-terminal, consistent with previous works. 15,48,[52][53][54][55] To reach a comprehensive understanding of the NORR progress, a diagram of the free energy changes for Fe@MoS 2 in the distal mechanism was prepared and is presented in Fig. 4(a) with the key intermediates being available in Fig.…”

Section: Resultsmentioning

confidence: 99%

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Using ternary steric hindrance synergy of a defective MoS₂ monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study

2023

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Using ternary steric hindrance synergy of a defective MoS₂ monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study

2023

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“…For SACs, the TM active sites can accept the electrons of NO 3 -, and simultaneously donate d electrons to empty π* orbital according to the "acceptance-donation" mechanism. To maximize the activation potential, DACs can make use of d-orbitals of the bimetallic sites via "pull-pull" effect, [40] as shown in Figure 1b. It can also take advantage of the innate dual-site to increase the adjusted space.…”

Section: Structural Stability and No 3 -Adsorption Of The M 1 M 2 @G-...mentioning

confidence: 99%

High‐Throughput Screening of Heterogeneous Transition Metal Dual‐Atom Catalysts by Synergistic Effect for Nitrate Reduction to Ammonia

Shu¹,

Chen²,

Liu³

et al. 2023

Adv Funct Materials

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Nitrate reduction to ammonia has attracted much attention for nitrate (NO3‐) removal and ammonia (NH3) production. Identifying promising catalyst for active nitrate electroreduction reaction (NO3RR) is critical to realize efficient upscaling synthesis of NH3 under low‐temperature condition. For this purpose, by means of spin‐polarized first‐principles calculations, the NO3RR performance on a series of graphitic carbon nitride (g‐CN) supported double‐atom catalysts (denoted as M1M2@g‐CN) are systematically investigated. The synergistic effect of heterogeneous dual‐metal sites can bring out tunable activity and selectivity for NO3RR. Amongst 21 candidates examined, FeMo@g‐CN and CrMo@g‐CN possess a high performance with low limiting potentials of ‐0.34 and ‐0.39 V, respectively. The activities can be attributed to a synergistic effect of the M1M2 dimer d orbitals coupling with the anti‐bonding orbital of NO3‐. The dissociation of deposited FeMo and CrMo dimers into two separated monomers is proved to be difficult, ensuring the kinetic stability of M1M2@g‐CN. Furthermore, the dual‐metal decorated on g‐CN significantly reduces the bandgap of g‐CN and broadens the adsorption window of visible light, implying its great promise for photocatalysis. This work opens a new avenue for future theoretical and experimental design related to NO3RR photo‐/electrocatalysts.

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“…Ammonia (NH 3 ), one of the essential feedstocks, plays an important role in many fields including fertilizer, medicine, activity toward NRA, due to the unfavorably sluggish desorption of NRA intermediates. [19] Previous strategies of modifying the metal sites of SACs would meet a dilemma for simultaneous enhancement of NRA selectivity and activity. Since the NRA electrocatalysis also falls into the category of proton-coupled electron transfer reactions, insufficient proton supply would possibly limit the NRA activity while excessive proton supply could aggravate the competitive HER.…”

Section: Introductionmentioning

confidence: 99%

Conjugated Coordination Polymer as a New Platform for Efficient and Selective Electroreduction of Nitrate into Ammonia

et al. 2023

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Electroreduction of nitrate into ammonia (NRA) provides a sustainable route to convert the widespread nitrate pollutants into high‐value‐added products under ambient conditions, which unfortunately suffers from unsatisfactory selectivity due to the competitive hydrogen evolution reaction (HER). Previous strategies of modifying the metal sites of catalysts often met a dilemma for simultaneously promoting activity and selectivity toward NRA. Here, a general strategy is reported to enable an efficient and selective NRA process through coordination modulation of single‐atom catalysts to tailor the local proton concentration at the catalyst surface. By contrast, two analogous Ni‐single‐atom enriched conjugated coordination polymers (NiO4‐CCP and NiN4‐CCP) with different coordination motifs are investigated for the proof‐of‐concept study. The NiO4‐CCP catalyst exhibits an ammonia yield rate as high as 1.83 mmol h−1 mg−1 with a Faradaic efficiency of 94.7% under a current density of 125 mA cm−2, outperforming the NiN4‐CCP catalyst. These experimental and theoretical studies both suggest that the strategy of coordination modulation can not only accelerate the NRA by adjusting the adsorption energies of NRA intermediates on the metal sites but also inhibit the HER through regulating the proton migration with contributions from the metal‐hydrated cations adsorbed at the catalyst surface, thus achieving simultaneous enhancement of NRA selectivity and activity.

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Achieving reaction pathway separation for electrochemical nitrate fixation on triatomic catalysts: A new mechanism

Cited by 14 publications

References 36 publications

Using ternary steric hindrance synergy of a defective MoS₂ monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study

Using ternary steric hindrance synergy of a defective MoS₂ monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study

High‐Throughput Screening of Heterogeneous Transition Metal Dual‐Atom Catalysts by Synergistic Effect for Nitrate Reduction to Ammonia

Conjugated Coordination Polymer as a New Platform for Efficient and Selective Electroreduction of Nitrate into Ammonia

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Achieving reaction pathway separation for electrochemical nitrate fixation on triatomic catalysts: A new mechanism

Cited by 14 publications

References 36 publications

Using ternary steric hindrance synergy of a defective MoS2 monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study

Using ternary steric hindrance synergy of a defective MoS2 monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study

High‐Throughput Screening of Heterogeneous Transition Metal Dual‐Atom Catalysts by Synergistic Effect for Nitrate Reduction to Ammonia

Conjugated Coordination Polymer as a New Platform for Efficient and Selective Electroreduction of Nitrate into Ammonia

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Using ternary steric hindrance synergy of a defective MoS₂ monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study

Using ternary steric hindrance synergy of a defective MoS₂ monolayer to manipulate the electrocatalytic mechanism toward nitric oxide reduction: a first-principles and machine learning study