N, O trans-coordinating silver single-atom catalyst for robust and efficient ammonia electrosynthesis from nitrate

Shen, Zhen; Yu, Yingsong; Zhao, Zhiwei; Mushtaq, Muhammad; Ji, Qianqian; Yasin, Ghulam; Rehman, Lashari Najeeb Ur; Liu, Xiaochun; Cai, Xingke; Tsiakaras, Panagiotis; Zhao, Jie

doi:10.1016/j.apcatb.2023.122687

Cited by 30 publications

(10 citation statements)

References 57 publications

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“…Moreover, Table S1 compares the NO3 − RR performa of Mo/TiO2−M with other previously reported electrodes. The FE and NH3 yields of Mo/TiO2−M electrode are comparable to most of the previous cathodes, further indicat the good activity of the as−prepared Mo/TiO2−M electrode [27,[54][55][56][57][58][59].…”

Section: Electrocatalytic Performance Of Electrodes For Mo/tiomentioning

confidence: 66%

Molybdenum-Modified Titanium Dioxide Nanotube Arrays as an Efficient Electrode for the Electroreduction of Nitrate to Ammonia

Chen,

Hu,

et al. 2024

Molecules

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Electrochemical nitrate reduction (NO3−RR) has been recognized as a promising strategy for sustainable ammonia (NH3) production due to its environmental friendliness and economical nature. However, the NO3−RR reaction involves an eight-electron coupled proton transfer process with many by-products and low Faraday efficiency. In this work, a molybdenum oxide (MoOx)-decorated titanium dioxide nanotube on Ti foil (Mo/TiO2) was prepared by means of an electrodeposition and calcination process. The structure of MoOx can be controlled by regulating the concentration of molybdate during the electrodeposition process, which can further influence the electron transfer from Ti to Mo atoms, and enhance the binding energy of intermediate species in NO3−RR. The optimized Mo/TiO2-M with more Mo(IV) sites exhibited a better activity for NO3−RR. The Mo/TiO2-M electrode delivered a NH3 yield of 5.18 mg h−1 cm−2 at −1.7 V vs. Ag/AgCl, and exhibited a Faraday efficiency of 88.05% at −1.4 V vs. Ag/AgCl. In addition, the cycling test demonstrated that the Mo/TiO2-M electrode possessed a good stability. This work not only provides an attractive electrode material, but also offers new insights into the rational design of catalysts for NO3−RR.

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Section: Electrocatalytic Performance Of Electrodes For Mo/tiomentioning

confidence: 66%

Molybdenum-Modified Titanium Dioxide Nanotube Arrays as an Efficient Electrode for the Electroreduction of Nitrate to Ammonia

Chen,

Hu,

et al. 2024

Molecules

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“…And, the possible liquid by-products, including N 2 H 4 , NO 2 − , and NO 3 − , were quantified by ultraviolet–visible (UV–Vis) spectrophotometry (Figs. S13-S15) [ 43 ]. More importantly, the potential by-product of N 2 H 4 , NO 2 − and NO 3 − was not detected in the solution that had been reacted for 2 h in the N 2 + CO 2 saturated 0.1 M KHCO 3 electrolyte at each potential (Figs.…”

Section: Resultsmentioning

confidence: 99%

Engineering Spin States of Isolated Copper Species in a Metal–Organic Framework Improves Urea Electrosynthesis

et al. 2023

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The catalytic activities are generally believed to be relevant to the electronic states of their active center, but understanding this relationship is usually difficult. Here, we design two types of catalysts for electrocatalytic urea via a coordination strategy in a metal–organic frameworks: CuIII-HHTP and CuII-HHTP. CuIII-HHTP exhibits an improved urea production rate of 7.78 mmol h−1 g−1 and an enhanced Faradaic efficiency of 23.09% at − 0.6 V vs. reversible hydrogen electrode, in sharp contrast to CuII-HHTP. Isolated CuIII species with S = 0 spin ground state are demonstrated as the active center in CuIII-HHTP, different from CuII with S = 1/2 in CuII-HHTP. We further demonstrate that isolated CuIII with an empty $${d}_{{{\text{x}}^{2}\text{-y}}^{2}}^{0}$$ d x 2 -y 2 0 orbital in CuIII-HHTP experiences a single-electron migration path with a lower energy barrier in the C–N coupling process, while CuII with a single-spin state ($${d}_{{{\text{x}}^{2}\text{-y}}^{2}}^{1}$$ d x 2 -y 2 1 ) in CuII-HHTP undergoes a two-electron migration pathway.

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“…94 Zhao et al synthesized trans -N,O-coordinated Ag SACs with a novel configuration of trans Ag–N 2 O 2 (Fig. 5d), 95 which inhibited the hydrogen evolution reaction (HER) (Fig. 5e) and optimized the adsorption of intermediates, thereby promoting the potential-determining step in the eNO 3 RR.…”

Section: Metal–inorganic Interfacementioning

confidence: 99%

Engineering interfacial architectures toward nitrate electrocatalysis and nitrogen neutral cycle

Gu,

Luo,

Zhang

et al. 2024

Mater. Chem. Front.

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N, O trans-coordinating silver single-atom catalyst for robust and efficient ammonia electrosynthesis from nitrate

Cited by 30 publications

References 57 publications

Molybdenum-Modified Titanium Dioxide Nanotube Arrays as an Efficient Electrode for the Electroreduction of Nitrate to Ammonia

Molybdenum-Modified Titanium Dioxide Nanotube Arrays as an Efficient Electrode for the Electroreduction of Nitrate to Ammonia

Engineering Spin States of Isolated Copper Species in a Metal–Organic Framework Improves Urea Electrosynthesis

Engineering interfacial architectures toward nitrate electrocatalysis and nitrogen neutral cycle

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