Electrocatalytic NO Reduction to NH<sub>3</sub> on Mo<sub>2</sub>C Nanosheets

Chen, Kai; Shen, Peng; Zhang, Nana; Ma, Dongwei; Chu, Ke

doi:10.1021/acs.inorgchem.2c03714

Cited by 38 publications

(33 citation statements)

References 69 publications

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“…In light of the LSV results, the initial electrolysis potential of 0.0 V is chosen to quantitatively evaluate the NO 3 RR performance of RuO x /Pd through combined chronoamperometric (1 h electrolysis) and colorimetric measurements. − Figure a shows that RuO x /Pd delivers a maximum NH 3 -Faradaic efficiency of 98.6% with a corresponding NH 3 yield rate of 23.5 mg h –1 cm –2 and a partial current density of 296.3 mA cm –2 (Figure S13) at −0.5 V vs RHE, surpassing those of almost all state-of-the-art NO 3 RR catalysts ever reported (Table S1). The controlled UV–vis tests (Figure S14) and qualitative/quantitative 14 NO 3 – / 15 NO 3 – isotope labeling nuclear magnetic resonance (NMR) experiments (Figure b and Figure S15) forcefully affirm that the generated NH 3 stems from the NO 3 RR on RuO x /Pd. − …”

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confidence: 99%

Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

et al. 2023

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The electrochemical nitrate reduction to ammonia reaction (NO3RR) has emerged as an appealing route for achieving both wastewater treatment and ammonia production. Herein, sub-nm RuO x clusters anchored on a Pd metallene (RuO x /Pd) are reported as a highly effective NO3RR catalyst, delivering a maximum NH3-Faradaic efficiency of 98.6% with a corresponding NH3 yield rate of 23.5 mg h–1 cm–2 and partial a current density of 296.3 mA cm–2 at −0.5 V vs RHE. Operando spectroscopic characterizations combined with theoretical computations unveil the synergy of RuO x and Pd to enhance the NO3RR energetics through a mechanism of hydrogen spillover and hydrogen-bond interactions. In detail, RuO x activates NO3 – to form intermediates, while Pd dissociates H2O to generate *H, which spontaneously migrates to the RuO x /Pd interface via a hydrogen spillover process. Further hydrogen-bond interactions between spillovered *H and intermediates makes spillovered *H desorb from the RuO x /Pd interface and participate in the intermediate hydrogenation, contributing to the enhanced activity of RuO x /Pd for NO3 –-to-NH3 conversion.

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Section: Resultsmentioning

confidence: 99%

Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

et al. 2023

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“…Electrocatalytic reduction of NO to NH 3 (NORR) offers a prospective approach to attain both harmful NO removal and efficient NH 3 electrosynthesis, − while a high-efficiency NORR process relies on active and selective electrocatalysts to expedite the NORR process while inhibiting the major competitive hydrogen evolution reaction (HER). − By far, a variety of d-block transition metal materials are developed as the efficient catalysts for the NORR, − attributed to their partially filled d-orbital electrons to effectively activate NO molecules. However, d-orbital electrons of transition metals are also beneficial for binding *H to facilitate the competing HER and compromise the NO-to-NH 3 Faradaic efficiency (FE NH3 ) .…”

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p-Block Antimony Single-Atom Catalysts for Nitric Oxide Electroreduction to Ammonia

et al. 2023

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Electrocatalytic NO reduction to NH3 (NORR) offers a prospective approach to attain both harmful NO removal and efficient NH3 electrosynthesis. Main-group p-block metals are promising NORR candidates but still lack adequate exploration. Herein, p-block Sb single atoms confined in amorphous MoO3 (Sb1/a-MoO3) are designed as an efficient NORR catalyst, exhibiting the highest NH3 yield rate of 273.5 μmol h–1 cm–2 and a NO-to-NH3 Faradaic efficiency of 91.7% at −0.6 V vs RHE. In situ spectroscopic characterizations and theoretical computations reason that the outstanding NORR performance of Sb1/a-MoO3 arises from the isolated Sb1 sites, which can optimize the adsorption of *NO/*NHO to lower the reaction energy barriers and simultaneously exhibit a higher affinity to NO than to H2O/H species. Moreover, our strategy can be extended to prepare Bi1/a-MoO3, showing a high NORR property, demonstrating the immense potential of p-block metal single-atom catalysts toward the high-performing NORR electrocatalysis.

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“…Electrocatalytic NO reduction to NH 3 (NORR) emerges as a promising solution to realize both harmful NO mitigation and green NH 3 synthesis. − However, the complex five-electron NORR process still suffers from sluggish kinetics and unwanted side reactions including the hydrogen evolution reaction (HER) . Therefore, it is highly required to develop efficient NORR catalysts to enhance the NO-to-NH 3 conversion efficiency. − …”

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Self-Tandem Electrocatalytic NO Reduction to NH₃ on a W Single-Atom Catalyst

et al. 2023

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We design single-atom W confined in MoO 3−x amorphous nanosheets (W 1 /MoO 3−x ) comprising W 1 −O 5 motifs as a highly active and durable NORR catalyst. Theoretical and operando spectroscopic investigations reveal the dual functions of W 1 −O 5 motifs to (1) facilitate the activation and protonation of NO molecules and (2) promote H 2 O dissociation while suppressing *H dimerization to increase the proton supply, eventually resulting in a self-tandem NORR mechanism of W 1 / MoO 3−x to greatly accelerate the protonation energetics of the NOto-NH 3 pathway. As a result, W 1 /MoO 3−x exhibits the highest NH 3 −Faradaic efficiency of 91.2% and NH 3 yield rate of 308.6 μmol h −1 cm −2 , surpassing that of most previously reported NORR catalysts.

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Electrocatalytic NO Reduction to NH₃ on Mo₂C Nanosheets

Cited by 38 publications

References 69 publications

Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

p-Block Antimony Single-Atom Catalysts for Nitric Oxide Electroreduction to Ammonia

Self-Tandem Electrocatalytic NO Reduction to NH₃ on a W Single-Atom Catalyst

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Electrocatalytic NO Reduction to NH3 on Mo2C Nanosheets

Cited by 38 publications

References 69 publications

Sub-nm RuOx Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

Sub-nm RuOx Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

p-Block Antimony Single-Atom Catalysts for Nitric Oxide Electroreduction to Ammonia

Self-Tandem Electrocatalytic NO Reduction to NH3 on a W Single-Atom Catalyst

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Electrocatalytic NO Reduction to NH₃ on Mo₂C Nanosheets

Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

Sub-nm RuO_x Clusters on Pd Metallene for Synergistically Enhanced Nitrate Electroreduction to Ammonia

Self-Tandem Electrocatalytic NO Reduction to NH₃ on a W Single-Atom Catalyst