Electrochemical Ammonia Synthesis via Nitrogen Reduction Reaction on a MoS<sub>2</sub> Catalyst: Theoretical and Experimental Studies

Zhang, Ling; Ji, Xuqiang; Ren, Xiang; Ma, Yongjun; Shi, Xifeng; Tian, Ziqi; Asiri, Abdullah M.; Liang, Changhao; Tang, Bo; Sun, Xuping

doi:10.1002/adma.201800191

Cited by 760 publications

(572 citation statements)

References 47 publications

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“…MoS 2 , one of the layered sulfide materials with low‐cost and nontoxicity, also used as electrocatalysts for NRR . A study has demonstrated that a MoS 2 NS array is also active for NRR, but it suffers from relatively low electrical conductivity with an FE of 1.17% . However, Li et al demonstrated that greatly boosted electrocatalytic N 2 reduction to NH 3 by using MoS 2 NSs‐rGO hybrid under ambient conditions.…”

Section: Electrochemical N2 Reductionmentioning

confidence: 99%

Reduced graphene oxide‐based materials for electrochemical energy conversion reactions

et al. 2019

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There have been ever-growing demands to develop advanced electrocatalysts for renewable energy conversion over the past decade. As a promising platform for advanced electrocatalysts, reduced graphene oxide (rGO) has attracted substantial research interests in a variety of electrochemical energy conversion reactions. Its versatile utility is mainly attributed to unique physical and chemical properties, such as high specific surface area, tunable electronic structure, and the feasibility of structural modification and functionalization. Here, a comprehensive discussion is provided upon recent advances in the material preparation, characterization, and the catalytic activity of rGO-based electrocatalysts for various electrochemical energy conversion reactions (water splitting, CO 2 reduction reaction, N 2 reduction reaction, and O 2 reduction reaction). Major advantages of rGO and the related challenges for enhancing their catalytic performance are addressed. K E Y W O R D S

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Section: Electrochemical N2 Reductionmentioning

confidence: 99%

Reduced graphene oxide‐based materials for electrochemical energy conversion reactions

et al. 2019

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“…From the thermodynamics point of view, *NNH is usually deemed as a key intermediate during the NRR process. A number of simulation studies on NRR catalysts including NiO have substantiated that the first proton‐coupled electron transfer to generate *NNH (*N 2 →*NNH) is the potential determining step (PDS) of the overall NRR. Thus, an effective NRR catalyst should facilitate *NNH formation/stabilization.…”

Section: Figurementioning

confidence: 99%

Nitrogen‐Doped NiO Nanosheet Array for Boosted Electrocatalytic N₂ Reduction

Wang

et al. 2019

ChemCatChem

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Electrocatalytic N2 reduction reaction (NRR) provides a sustainable approach for ambient N2 fixation. Non‐noble transition metal‐based electrocatalysts (TMEs) are emerging as the most promising NRR catalysts, but commonly exhibited limited NRR activity. Heteroatom doping is an effective method to improve the electrocatalytic activity of TMEs by finely modulating the electronic structures. Herein, as a proof‐of‐concept, nitrogen‐doped NiO nanosheet array on carbon cloth (N‐NiO/CC) was investigated as model heteroatom‐doped TMEs for NRR. The N‐NiO/CC exhibited the considerably enhanced NRR performance with a NH3 yield of 22.7 μg h−1 mg−1 and an FE of 7.3 % in 0.1 M LiClO4 at −0.5 V (vs. RHE), far superior to those of undoped counterpart. Density functional theory (DFT) calculations revealed that the N‐doping could induce the enhanced surface conductivity and upraised d‐band center, leading to promoted *NNH stabilization, reduced reaction energy barrier and thus improved NRR performance.

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“…[58,59] The calibration curve for NH 3 assay was presented in Figure S6 in the Supporting Information. The NRR electrocatalytic activities of Ti 3 C 2 T x on the CP (Ti 3 C 2 T x -CP) were also studied for comparison.…”

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confidence: 99%

High‐Performance Electrocatalytic Conversion of N₂ to NH₃ Using Oxygen‐Vacancy‐Rich TiO₂ In Situ Grown on Ti₃C₂T_x MXene

Fang

Liu

Han

et al. 2019

Advanced Energy Materials

367

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To achieve the energy‐effective ammonia (NH3) production via the ambient‐condition electrochemical N2 reduction reaction (NRR), it is vital to ingeniously design an efficient electrocatalyst assembling the features of abundant surface deficiency, good dispersibility, high conductivity, and large surface specific area (SSA) via a simple way. Inspired by the fact that the MXene contains thermodynamically metastable marginal transition metal atoms, the oxygen‐vacancy‐rich TiO2 nanoparticles (NPs) in situ grown on the Ti3C2Tx nanosheets (TiO2/Ti3C2Tx) are prepared via a one‐step ethanol‐thermal treatment of the Ti3C2Tx MXene. The oxygen vacancies act as the main active sites for the NH3 synthesis. The highly conductive interior untreated Ti3C2Tx nanosheets could not only facilitate the electron transport but also avoid the self‐aggregation of the TiO2 NPs. Meanwhile, the TiO2 NPs generation could enhance the SSA of the Ti3C2Tx in return. Accordingly, the as‐prepared electrocatalyst exhibits an NH3 yield of 32.17 µg h−1 mg−1cat. at −0.55 V versus reversible hydrogen electrode (RHE) and a remarkable Faradaic efficiency of 16.07% at −0.45 V versus RHE in 0.1 m HCl, placing it as one of the most promising NRR electrocatalysts. Moreover, the density functional theory calculations confirm the lowest NRR energy barrier (0.40 eV) of TiO2 (101)/Ti3C2Tx compared with Ti3C2Tx or TiO2 (101) alone.

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Electrochemical Ammonia Synthesis via Nitrogen Reduction Reaction on a MoS₂ Catalyst: Theoretical and Experimental Studies

Cited by 760 publications

References 47 publications

Reduced graphene oxide‐based materials for electrochemical energy conversion reactions

Reduced graphene oxide‐based materials for electrochemical energy conversion reactions

Nitrogen‐Doped NiO Nanosheet Array for Boosted Electrocatalytic N₂ Reduction

High‐Performance Electrocatalytic Conversion of N₂ to NH₃ Using Oxygen‐Vacancy‐Rich TiO₂ In Situ Grown on Ti₃C₂T_x MXene

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Electrochemical Ammonia Synthesis via Nitrogen Reduction Reaction on a MoS2 Catalyst: Theoretical and Experimental Studies

Cited by 760 publications

References 47 publications

Reduced graphene oxide‐based materials for electrochemical energy conversion reactions

Reduced graphene oxide‐based materials for electrochemical energy conversion reactions

Nitrogen‐Doped NiO Nanosheet Array for Boosted Electrocatalytic N2 Reduction

High‐Performance Electrocatalytic Conversion of N2 to NH3 Using Oxygen‐Vacancy‐Rich TiO2 In Situ Grown on Ti3C2Tx MXene

Contact Info

Product

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About

Electrochemical Ammonia Synthesis via Nitrogen Reduction Reaction on a MoS₂ Catalyst: Theoretical and Experimental Studies

Nitrogen‐Doped NiO Nanosheet Array for Boosted Electrocatalytic N₂ Reduction

High‐Performance Electrocatalytic Conversion of N₂ to NH₃ Using Oxygen‐Vacancy‐Rich TiO₂ In Situ Grown on Ti₃C₂T_x MXene