MXene Materials for the Electrochemical Nitrogen Reduction—Functionalized or Not?

Johnson, Luke R.; Sridhar, Sudiksha; Zhang, Liang; Fredrickson, Kurt D.; Raman, Abhinav S.; Jang, Joonbaek; Leach, Connor T.; Padmanabhan, Ashwin; Price, Christopher C.; Frey, Nathan C.; Raizada, Abhishek; Rajaraman, Vishwanathan; Saiprasad, Sai Aparna; Tang, Xin; Vojvodić, Aleksandra

doi:10.1021/acscatal.9b01925

Cited by 142 publications

(133 citation statements)

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“…[ 6 ] Furthermore, such production method is energy‐intensive that consumes 1–3% of the global energy annually and emit tons of CO 2 correspondingly. [ 7 ] Over the last decades, electrochemical NRR has attracted global attention due to its renewable raw materials of N 2 and water as well as ambient synthesis condition. [ 8 ] With recent booming development, the study of NRR electrocatalysts has moved from precious metals to cheap and abundant transition metal oxides and metal‐free materials, etc.…”

Section: Figurementioning

confidence: 99%

Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction

Jin

Liu

et al. 2020

Advanced Energy Materials

177

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Ammonia (NH 3 ) is essential to human life due to its vital roles in fuel production, agricultural cultivation and industrial manufacture. [1,2] The abundant nitrogen (N 2 ) in the earth's atmosphere is the main raw material for the synthesis of NH 3 , [3] but the large bond energy (940.95 kJ mol −1 ) of NN bond [1,4] makes N 2 reduction reaction (NRR) extremely difficult. [5] At present, the traditionally industrial NH 3 synthesis strongly relies on the Haber-Bosch process, which has to be conducted at high pressures at 200-300 atm and high temperature of ≈500 °C. [6] Furthermore, such production method is energy-intensive that consumes 1-3% of the global energy annually and emit tons of CO 2 correspondingly. [7] Over the last decades, electrochemical NRR has attracted global attention due to its renewable raw materials of N 2 and water as well as ambient synthesis condition. [8] With recent booming development, the study of NRR electrocatalysts has moved from precious metals to cheap and abundant transition metal oxides and metal-free materials, etc. [9] However, due to the lack of rational and target-specific design of the NRR electrocatalyst, it is still a difficult task to reach an ideal electrocatalyst fulfilling with the requirements of high NH 3 yield, excellent selectivity and cost-effectiveness simultaneously. To meet these requirements, it is expected that catalysts contain abundant active sites. [10] Under this context, various low-dimensional catalysts have been extensively investigated, such as 2D nanosheets and 0D quantum dots (QDs) due to their ultrahigh ratio of active sites and defects exposed on the surfaces.QDs, especially derived from 2D materials (2D-QDs), are often with small size of less than 10 nm, enhanced surface defects and large surface specific area, thus offering abundantactive basal and edge sites, together with various functional groups. [8,11,12] As a result, a large space has been generated for advanced rational design for N 2 adsorption and full reduction. [13,17] So far, however, the effect of edge sites and their functional groups on NRR performance of 2D-QDs is poorly known. MXene, an emerging typical 2D material, can be expressed by the chemical formula of M n+1 X n T x (n = 1, 2 and 3), [18,20] where M stands for the transition metal (e.g., Ti, Ta, Nb, V, Mo), the X represents the nitrogen or carbon or carbonitride, while T x represents a large number of surface functional groups (e.g., OH, F). [21,22] Due to the excellent conductivity and stability, To enable an efficient and cost-effective electrocatalytic N 2 reduction reaction (NRR) the development of an electrocatalyst with a high NH 3 yield and good selectivity is required. In this work, Ti 3 C 2 T x MXene-derived quantum dots (Ti 3 C 2 T x QDs) with abundant active sites enable the development of efficient NRR electrocatalysts. Given surface functional groups play a key role on the electrocatalytic performance, density functional theory calculations are first conducted, clarifying that hydroxyl groups on Ti 3 C 2...

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Section: Figurementioning

confidence: 99%

Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction

Jin

Liu

et al. 2020

Advanced Energy Materials

177

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“…Specifically, H‐terminated M 2 CT x MXenes exhibit higher stability at a higher potential compared with O‐terminated and N‐terminated M 2 CT x MXenes. [ 18 ] F‐terminated Mo 2 CT x MXene also shows better N 2 RR activity compared with O‐terminated MXene. [ 52 ] The Ti 3 C 2 T x (T = F, OH) catalysts also show high structural stability and selectivity towards N 2 RR.…”

Section: Applications In Electrocatalysismentioning

confidence: 99%

“…For example, by tuning the type and stoichiometry of surface functional groups, the hydrogen evolution reaction (HER) activity can be enhanced with more O functional groups on the surface of MXenes, while more F functional groups are desirable for nitrogen reduction reaction (N 2 RR). [18,19] Furthermore MXenes can be conveniently incorporated with TMs, metal oxides, metal-free substrates, and other 2D materials, which often display synergistic effects on electrocatalytic performance. [15,20,21] Although MXene materials show promise in a variety of electrocatalytic reactions, this research field is still in an early stage.…”

Section: Introductionmentioning

confidence: 99%

Challenges and Opportunities in Utilizing MXenes of Carbides and Nitrides as Electrocatalysts

Wang

Nian

Biswas

et al. 2020

Advanced Energy Materials

120

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Sustainable energy conversion processes often require electrochemical reactions powered by renewable energy sources. 2D transition metal carbides and nitrides (MXenes), an important and growing class of 2D materials, have been demonstrated to be promising candidates for heterogeneous electrocatalysis due to their unique electronic, physical, chemical, and mechanical properties. Significant efforts have been made in the development of MXenes and MXene‐derived electrocatalysts for various electrochemical reactions, including the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, carbon dioxide reduction reaction, nitrogen reduction reaction, and methanol oxidation reaction. MXenes from earth‐abundant metals provide the potential for large‐scale applications, and their well‐defined structures allow for the identification of active sites and catalytic mechanisms. Herein, recent studies of MXenes in electrocatalysis are reviewed, and the challenges and opportunities for the design and fabrication of MXenes and MXene‐based materials with desired electrocatalytic properties are discussed.

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“…However, most of them focused on theoretical calculation. [80][81][82] Luo et al first reported that MXene (Ti 3 C 2 T x ) nanosheets attached to a vertically aligned metal host could achieve a high FE (5.78%) and an NH 3 yield rate of 4.72 μg h À 1 cm À 2 at À 0.1 V. [83] Then, Zhang et al reported the utilization of a Ti 3 C 2 T x MXene nanosheet as both the precursor and conductive substrate toward the in situ hydrothermal growth of TiO 2 nanoparticles. The combination of TiO 2 and Ti 3 C 2 T x led to a synergistically active Tibased nanohybrid catalyst that could strengthen N 2 reduction electrocatalysis.…”

Section: Mxene Based Catalystsmentioning

confidence: 99%

“…A large number of studies have investigated MXenes for nitrogen reduction. However, most of them focused on theoretical calculation . Luo et al.…”

Section: Advances In Noble‐metal‐free Catalysts For Electrocatalytic mentioning

confidence: 99%

Recent Advances in Noble‐Metal‐Free Catalysts for Electrocatalytic Synthesis of Ammonia under Ambient Conditions

Xiang

Wang

et al. 2020

Chemistry An Asian Journal

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Ammonia is an essential chemical for producing fertilizers and energy carriers. However, the industrial Haber-Bosch process causes huge CO 2 emissions and energy waste. As a promising alternative for Haber-Bosch process, electrochemical synthesis of ammonia has drawn much attention. Catalysts, as a vital part of electrochemical nitrogen reduction reaction (NRR), have developed rapidly in recent years. Compared to noble-metal catalysts, noble-metal-free catalysts possess a low-cost advantage. In this review, noble-metalfree catalysts, including metal-based materials, metal organic frameworks (MOFs), MXenes, and metal-free materials, are summarized. In addition, effective design strategies are discussed, along with the main problems and some potential directions of noble-metal-free NRR catalysts. 2. Advances in Noble-Metal-Free Catalysts for Electrocatalytic N 2 Reduction Recently, although noble metal catalysts have better catalytic performance in NRR, researchers have paid more attention to the utilization of resource-rich elements in the earth, including iron, molybdenum, carbon, nitrogen, boron and other nonnoble elements, in order to reduce costs and improve the [a

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MXene Materials for the Electrochemical Nitrogen Reduction—Functionalized or Not?

Cited by 142 publications

References 75 publications

Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction

Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction

Challenges and Opportunities in Utilizing MXenes of Carbides and Nitrides as Electrocatalysts

Recent Advances in Noble‐Metal‐Free Catalysts for Electrocatalytic Synthesis of Ammonia under Ambient Conditions

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MXene Materials for the Electrochemical Nitrogen Reduction—Functionalized or Not?

Cited by 142 publications

References 75 publications

Rational Design of Hydroxyl‐Rich Ti3C2Tx MXene Quantum Dots for High‐Performance Electrochemical N2 Reduction

Rational Design of Hydroxyl‐Rich Ti3C2Tx MXene Quantum Dots for High‐Performance Electrochemical N2 Reduction

Challenges and Opportunities in Utilizing MXenes of Carbides and Nitrides as Electrocatalysts

Recent Advances in Noble‐Metal‐Free Catalysts for Electrocatalytic Synthesis of Ammonia under Ambient Conditions

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Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction

Rational Design of Hydroxyl‐Rich Ti₃C₂T_x MXene Quantum Dots for High‐Performance Electrochemical N₂ Reduction