Synergistic modulation of local environment for electrochemical nitrate reduction via asymmetric vacancies and adjacent ion clusters

Chen, Dong; Zhang, Shaoce; Bu, Xiuming; Zhang, Rong; Quan, Quan; Lai, Zhengxun; Wang, Wei; Meng, You; Yin, Di; Yip, SenPo; Liu, Chuntai; Zhi, Chunyi; Ho, Johnny C.

doi:10.1016/j.nanoen.2022.107338

Cited by 30 publications

(14 citation statements)

References 43 publications

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“…Additionally, to verify the origin of N and eliminate the influence of the environment or electrodes on the test results, 15 N isotope labeling experiments were further carried out by using K 15 NO 3 as the source of nitrogen. As displayed in Figure c, 1 H NMR spectra of the electrolyte after electrolysis demonstrate that the typical double peaks of 15 N appear, which are clearly different from the three peaks of 14 N. The triple and double peak patterns with coupling constants of 52.2 and 73.2 Hz correspond to 14 NH 4 + and 15 NH 4 + signals, respectively, which the 1 H NMR measurements confirm that the production of NH 3 originates from the electroreduction of NO 3 – rather than from the contamination. To further demonstrate the durability of the catalyst, a long electrolysis process of 24 h was also performed.…”

Section: Resultsmentioning

confidence: 99%

Cu₂₊₁O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

et al. 2023

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Electrocatalytic nitrate reduction reaction (ENO 3 RR) is an alternative, sustainable, and environmentally friendly value-added NH 3 synthesis method under ambient conditions relative to the traditional Haber−Bosch process; however, its low NH 3 yield, low Faradaic efficiency (FE), low selectivity, and low conversion rate severely restrict the development. In this work, a Cu 2+1 O/Ag-CC heterostructured electrocatalyst was successfully fabricated by constructing a heterogeneous interface between Cu 2+1 O and Ag for selective electrochemical nitrate-to-ammonia conversion. The construction of the heterogeneous interface effectively promotes the synergistic effect of the catalytically active components Cu 2+1 O and Ag, which enhances the material conductivity, accelerates the interfacial electron transfer, and exposes more active sites, thus improving the performance of ENO 3 RR. Such Cu 2+1 O/Ag-CC manifests a high NH 3 yield of 2.2 mg h −1 cm −2 and a notable ammonia FE of 85.03% at the optimal applied potential of −0.74 V vs RHE in a relatively low concentration of 0.01 M NO 3 − -containing 0.1 M KOH. Moreover, it shows excellent electrochemical stability during the cycle tests. Our study not only provides an efficient catalyst for ammonia electro-synthesis from ENO 3 RR but also an effective strategy for the construction of ENO 3 RR electrocatalysts for electrocatalytic applications.

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Section: Resultsmentioning

confidence: 99%

Cu₂₊₁O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

et al. 2023

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“…Chen et al 221 developed a Cu-based electrocatalyst called Cu-Ov-W, which incorporates neighboring Mo clusters (Fig. 26a).…”

Section: Perovskite-based Electrocatalystsmentioning

confidence: 99%

“…Although the role of OV and ion clusters has been studied in electrochemical catalysis, the synergistic interaction between these two species has received limited attention. Chen et al 221 developed a Cu-based electrocatalyst called Cu-Ov-W, which incorporates neighboring Mo clusters (Fig. 26a).…”

Section: Recent Progress In Ov-based Electrocatalysts In Electrochemi...mentioning

confidence: 99%

Investigating the role of oxygen vacancies in metal oxide for enhanced electrochemical reduction of NO₃⁻ to NH₃: mechanistic insights

Ullah,

Wang,

Ahmad

et al. 2023

Inorg. Chem. Front.

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“…[57] Additional electron/chemical transfer through the interface could modulate thermodynamic reaction barrier of intermediates and inhibited the competitive hydrogen evolution reaction. [58] The Cu-Mn 3 O 4 heterostructure ultra-thin nano chip array with rich active sites, regulated electronic structure and interface synergy, promoted the adsorption and activation of nitrate, realized 95.8 % nitrate conversion (Figure 9a). [59] For Pd/ Cu 2 O hybrid with mesoporous hollow sphere structure, Pd formed part of PdCu alloy to transfer electrons, and polarized Cu 3d orbit instead of Cu 2 O as a new adsorption site.…”

Section: Defect and Interface Engineeringmentioning

confidence: 99%

Electrochemical Nitrate Reduction to Ammonia – Recent Progress

Niu,

Yang,

Qian

et al. 2023

ChemElectroChem

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The presence of nitrate in industrial, domestic and agricultural wastewater has a detrimental impact on both ecosystem and human health, as remediation and purification efforts are slow, challenging and difficult, given the high solubility and stability of this pollutant. Taking nitrate into high value‐added ammonia by electrochemical reduction can overcome high pollution and energy consumption limit of Haber‐Bosch process with long‐term significance of environmental protection and energy saving. This review summarized the research progress on the electrocatalytic reduction of nitrate to ammonia, with a focus on the reaction mechanisms, influencing factors, product detection methods, performance evaluation methods and the research status of electrocatalysts up to now. The review reported the latest strategies employed to design efficient electrocatalysts, such as pore structure regulation, alloying, heterostructure construction, defect and interface engineering, crystal surface regulation and microenvironment modulation of single‐atom catalysts. It highlights critical factors that determin the performance in terms of nitrate adsorption, exposed active sites, mass transfer rate, intermediates barrier and side reactions, as well as the stability of electrocatalysts and recovery of ammonia. In addition, the future direction of technology for electrocatalytic reduction of nitrate to ammonia has also been proposed.

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Synergistic modulation of local environment for electrochemical nitrate reduction via asymmetric vacancies and adjacent ion clusters

Cited by 30 publications

References 43 publications

Cu₂₊₁O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

Cu₂₊₁O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

Investigating the role of oxygen vacancies in metal oxide for enhanced electrochemical reduction of NO₃⁻ to NH₃: mechanistic insights

Electrochemical Nitrate Reduction to Ammonia – Recent Progress

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Synergistic modulation of local environment for electrochemical nitrate reduction via asymmetric vacancies and adjacent ion clusters

Cited by 30 publications

References 43 publications

Cu2+1O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

Cu2+1O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

Investigating the role of oxygen vacancies in metal oxide for enhanced electrochemical reduction of NO3− to NH3: mechanistic insights

Electrochemical Nitrate Reduction to Ammonia – Recent Progress

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Cu₂₊₁O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

Cu₂₊₁O/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance

Investigating the role of oxygen vacancies in metal oxide for enhanced electrochemical reduction of NO₃⁻ to NH₃: mechanistic insights