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

Fang, Yanfeng; Liu, Zaichun; Han, Jingrui; Jin, Zhaoyong; Han, Yaqian; Wang, Faxing; Niu, Yaran; Wu, Yuping; Xu, Yuanhong

doi:10.1002/aenm.201803406

Cited by 379 publications

(93 citation statements)

References 74 publications

(128 reference statements)

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“…Low cost and earth abundance make them a great alternative to replace noble metal catalysts. [10][11][12][13][14][15][16][17][18] If combining transition metals with metal oxides and their stable composition, a perovskite structured material (ABO 3 ) can be taken into account, which offers a high possibility with a flexible and thermally stable material. [19] Chang et al reported that chromium was a promising catalytic material for NRR since Cr 3 + showed the capability to strongly adsorb the N 2 over CH 4 and O 2 .…”

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confidence: 99%

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

et al. 2019

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Electrochemical synthesis of ammonia through the nitrogen reduction reaction (NRR) has the possibility to revolutionize our production of ammonia and to save our planet from both emissions and large energy consumption. In this study, a perovskite structured lanthanum chromite catalyst (LaCrO 3 ) is synthesized, characterized as well as electrochemically evaluated for NRR. The highest ammonia yield is obtained at À 0.8 V vs. reversible hydrogen electrode with an ammonia formation rate of 24.8 μg h À 1 mg À 1 cat , and a Faradaic efficiency of 15 %. Material calculation further confirms the possible mechanism of ammonia formation with the aid of LaCrO 3 catalyst. The resulting conclusion offers a great alternative with the easily produced and low-cost perovskite structured electrocatalysts for ammonia production.

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confidence: 99%

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

et al. 2019

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“…[3] Benefiting from the advantages of N2 electroreduction reaction (NERR) such as its mild reaction condition, high energy efficiency, and functionality without CO2 emissions or fossil fuel consumption, exploring smart design to synthesize efficient catalysts toward NERR has attracted growing interest. [4,5] The overall NERR reaction can be depicted as 2 + 3 2 → 2 3 + 3 2 ⁄ 2 , [6] in which N2 reacts with H2O to produce NH3 and O2. NERR has a similar theoretical potential to that of hydrogen evolution reaction (HER), [7] which creates a fundamental problem for electrochemical ammonia synthesis.…”

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confidence: 99%

Single-atom catalysts boost nitrogen electroreduction reaction

Zhai

Zhu

et al. 2020

Materials Today

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Ammonia (NH3) is mainly produced through the traditional Haber-Bosch process under harsh conditions with huge energy consumption and massive carbon dioxide (CO2) emission. The nitrogen electroreduction reaction (NERR), as an energy-efficient and environment-friendly process of converting nitrogen (N2) to NH3 under ambient conditions, has been regarded as a promising alternative to the Haber-Bosch process and has received enormous interest in recent years. Although some exciting progress has been made, considerable scientific and technical challenges still exist in improving the NH3 yield rate and Faradic efficiency, understanding the mechanism of the reaction and promoting the wide commercialization of NERR. Single-atom catalysts (SACs) have emerged as promising catalysts because of its atomically dispersed activity sites and maximized atom efficiency, unsaturated coordination environment, and its unique electronic structure, which could significantly improve the rate of reaction and yield rate of NH3. In this review we briefly introduce the unique structural and electronic features of SACs, which contributes to comprehensively understand the reaction mechanism owing to their structural simplicity and diversity, and in turn expedite the rational design of fantastic catalysts at the atomic scale. Then, we summarize the most recent experimental and computational efforts on developing novel SACs with excellent NERR performance, including precious metal-, nonprecious metal-and nonmetal-based SACs. Finally, we present challenges and perspectives of SACs on NERR, as well as some potential means for advanced NERR catalyst.

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“…Therefore, substantial efforts have been devoted to nonprecious metal electrocatalysts which are abundant in earth as an extremely promising alternative for the electrochemical synthesis of NH 3 . [10][11][12][13][14][15][16][17][18] Metal-organic frameworks (MOFs) have ultra-high specific surface area, unsaturated metal sites, extended frame structure, and adjustable functions. [19] Based on these unique characteristics, MOFs have been used widely in the field of hydrogen storage, [20,21] gas adsorption and separation, [22][23][24][25][26] light, [27] electricity, [28,29] and magnetic.…”

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Electrocatalysis of N₂to NH₃by HKUST‐1 with High NH₃Yield

Cao

et al. 2020

Chemistry An Asian Journal

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Electrolytic ammonia synthesis from nitrogen at ambient conditions is appearing as a promising alternative to the Haber-Bosch process which is consuming high energy and emitting CO 2 . Here, a typical MOF material, HKUST-1 (CuÀ BTC, BTC = benzene-1,3,5-tricarboxylate), was selected as an electrocatalyst for the reaction of converting N 2 to NH 3 under ambient conditions. At À 0.75 V vs. reversible hydrogen electrode, it achieves excellent catalytic performance in the electrochemical synthesis of ammonia with high NH 3 yield (46.63 μg h À 1 mg À 1 cat. or 4.66 μg h À 1 cm À 2 ) and good Faraday efficiency (2.45%). It is indicated that the good performance of the HKUST-1 catalyst may originate from the formation of Cu(I). In addition, the catalyst also has good selectivity for N 2 to NH 3 . NH 3 plays an important role in the manufacture of inorganic fertilizers, pharmaceuticals, and explosives. [1] Although the atmosphere contains about 78% of nitrogen gas, most organisms must utilize diverse methods to convert free nitrogen from the air into nitrogen-containing compounds before digesting and absorbing because of the inertness of nitrogen itself, which is known as "nitrogen fixation". [2][3][4] Compared with the traditional high energy-intensive Haber-Bosch method, electrochemical NH 3 synthesis can be operated at normal temperature and pressure with the advantages of simple equipments and without releasing a large amount of CO 2 . [5] However, the slow kinetics of N 2 adsorption and the strong N � N bond energy lead to a low efficiency of the NH 3 yields. Hence, stable and efficient electrocatalysts are needed to run the N 2 reduction reaction (NRR) at ambient conditions. Although noble metal materials exhibit high catalytic activity in the electrochemical synthesis of NH 3 , [6][7][8][9] the defects of high cost and low storage are the biggest obstacles for large scale usage. Therefore, substantial efforts have been devoted to nonprecious metal electrocatalysts which are abundant in earth as an extremely promising alternative for the electrochemical synthesis of NH 3 . [10][11][12][13][14][15][16][17][18] Metal-organic frameworks (MOFs) have ultra-high specific surface area, unsaturated metal sites, extended frame structure, and adjustable functions. [19] Based on these unique characteristics, MOFs have been used widely in the field of hydrogen storage, [20,21] gas adsorption and separation, [22][23][24][25][26] light, [27] electricity, [28,29] and magnetic. [30] HKUST-1 (CuÀ BTC, BTC = benzene-1,3,5-tricarboxylate) with Cu(II) nodes coordinated by negatively charged BTC linkers exhibits a octahedral cages structure with large cavities, and unsaturated Cu sites act as strong adsorption part of various molecules or water vapor. [31][32][33][34] During the electrochemical reduction, Cu(II) can be transformed into to Cu 2 O/Cu(0) induced by the potential, which increases the electro-conductivity and is likely to be the catalytically active species. [35,36] Inspired by this, we studied the N 2 to NH 3 catalytic acti...

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

Cited by 379 publications

References 74 publications

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Single-atom catalysts boost nitrogen electroreduction reaction

Electrocatalysis of N₂to NH₃by HKUST‐1 with High NH₃Yield

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

Cited by 379 publications

References 74 publications

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO3 Catalyst

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO3 Catalyst

Single-atom catalysts boost nitrogen electroreduction reaction

Electrocatalysis of N2to NH3by HKUST‐1 with High NH3Yield

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

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Electrocatalysis of N₂to NH₃by HKUST‐1 with High NH₃Yield