Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

Huang, Yiyin; Babu, Dickson D.; Peng, Zhen; Wang, Yaobing

doi:10.1002/advs.201902390

Cited by 81 publications

(54 citation statements)

References 183 publications

(273 reference statements)

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“…Through surface control, defect engineering, alloying, component regulation, and hybridization, and other strategies, increase the exposed active sites or adjust the electronic structure to improve catalytic performance. [154,[156][157][158][159][160] The promotion of selective absorption and activation of N 2 molecules on NRR electrocatalysts through alloying or composition adjustment has also been gradually studied. [160][161][162][163] Among them, HEAs may become potential electrocatalysts for NRR due to their adjustable components and high tolerance, improving the activity, selectivity, and stability of NRR.…”

Section: Multi-sites Electrocatalysis Of High-entropy Alloy Electrocatalyst In Nrrmentioning

confidence: 99%

“…[165] In addition, metals such as Ti, Y, and Zr have stronger bonding strength with N and can be developed appropriately. [157] After nitrogen activation, the next proton-electron transfer process depends on the nature of the active site. Through component adjustment, such as alloy engineering, the electronic structure and performance of various metals can be optimized, and the adsorption and activation of reactants on the catalyst surface can be promoted.…”

Section: Designing Efficient Heas Catalyst For Nrrmentioning

confidence: 99%

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Multi‐Sites Electrocatalysis in High‐Entropy Alloys

Lai

et al. 2021

Adv Funct Materials

187

135

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High‐entropy alloys (HEAs) have attracted widespread attention in electrocatalysis due to their unique advantages (adjustable composition, complex surface, high tolerance, etc.). They allow for the formation of new and tailorable active sites in multiple elements adjacent to each other, and the interaction can be tailored by rational selection of element configuration and composition. However, it needs to be further explored in catalyst design, the interaction of elements, and the determination of active sites. This review article focuses on the important progress for multi‐sites electrocatalysis in HEAs. The classification is done on the basis of catalytic reaction, including hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, alcohol oxidation reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction. Based on experiments and theories, a more in‐depth exploration of the high catalytic activity of HEAs will be conducted, including the selection of elements (the special role of each element in catalysis) and the multi‐sites effect. This review can provide the basis for the element selection and design of HEAs in some reactions, to adjust the compositions of HEAs to improve their intrinsic activity. Furthermore, the remaining challenges and future directions for promising research fields are also provided.

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Section: Multi-sites Electrocatalysis Of High-entropy Alloy Electrocatalyst In Nrrmentioning

confidence: 99%

Section: Designing Efficient Heas Catalyst For Nrrmentioning

confidence: 99%

Multi‐Sites Electrocatalysis in High‐Entropy Alloys

Lai

et al. 2021

Adv Funct Materials

187

135

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“…Electrochemical reduction of N 2 (NRR, N 2 + 6e − + 6H + → 2NH 3 ) is a promising nitrogenfixation system that can sustainably operate under mild conditions [3,4]. However, the efficient generation of NH 3 is difficult due to the sluggish cleavage of chemically inert N≡N bond [2,3,5,6]. Moreover, NRR involves multiple intermediates and needs to compete with the hydrogen evolution reaction (HER) in aqueous solution, which makes limited Faradaic efficiency (FE) for NH 3 [7][8][9][10][11][12][13][14].…”

Section: Mnmentioning

confidence: 99%

“…Moreover, NRR involves multiple intermediates and needs to compete with the hydrogen evolution reaction (HER) in aqueous solution, which makes limited Faradaic efficiency (FE) for NH 3 [7][8][9][10][11][12][13][14]. Electrocatalysts based on precious metals like Ru and Rh have been experimentally and theoretically explored to present favorable NRR activity [6,[15][16][17][18]. From practical standpoint, it is significant to develop robust and selective electrocatalysts for NRR from cost-effective metals.…”

Section: Mnmentioning

confidence: 99%

Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia

Wang

Liu

et al. 2021

Nano-Micro Lett.

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Efficient and robust single-atom catalysts (SACs) based on cheap and earth-abundant elements are highly desirable for electrochemical reduction of nitrogen to ammonia (NRR) under ambient conditions. Herein, for the first time, a Mn–N–C SAC consisting of isolated manganese atomic sites on ultrathin carbon nanosheets is developed via a template-free folic acid self-assembly strategy. The spontaneous molecular partial dissociation enables a facile fabrication process without being plagued by metal atom aggregation. Thanks to well-exposed atomic Mn active sites anchored on two-dimensional conductive carbon matrix, the catalyst exhibits excellent activity for NRR with high activity and selectivity, achieving a high Faradaic efficiency of 32.02% for ammonia synthesis at − 0.45 V versus reversible hydrogen electrode. Density functional theory calculations unveil the crucial role of atomic Mn sites in promoting N2 adsorption, activation and selective reduction to NH3 by the distal mechanism. This work provides a simple synthesis process for Mn–N–C SAC and a good platform for understanding the structure-activity relationship of atomic Mn sites. Graphic Abstract

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“…2) Numerous couples of different atomic centers and various substrates would extend the sample capacity for mechanism investigation of NERR. [15] Although some excellent review articles have been published about the synthesis of novel catalysts and their applications in NERR [5,[16][17][18][19][20][21]…”

Section: Introductionmentioning

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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Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

Cited by 81 publications

References 183 publications

Multi‐Sites Electrocatalysis in High‐Entropy Alloys

Multi‐Sites Electrocatalysis in High‐Entropy Alloys

Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia

Single-atom catalysts boost nitrogen electroreduction reaction

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