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Single-atom catalysts for electrochemical N2 reduction to NH3

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Abstract

The increasing demand for clean energy and growing concerns regarding environmental sustainability have led to greater attention devoted toward the production of clean fuels via green chemistry. In this respect, ammonia is a green alternative to fossil fuels and can serve as a clean energy source. There is now great interest in realizing the electrochemical reduction in atmospheric nitrogen (N2) for cheap, environmentally friendly and reliable ammonia (NH3) production worldwide. However, the robustness of the triple bond in N2 and the low efficiency of candidate catalysts limit the utility of this conversion. Single atom catalysts have been found to be more effective than nanoparticles due to their unique properties, and thus have been studied extensively for the nitrogen reduction reaction. In this review, we have covered the recent advances in design and synthesis of noble metal and non-noble metal single atom catalysts for the electrochemical reduction in nitrogen during the years 2018–2022. The catalyst efficiencies, with reference to coordination preferences and theoretical studies have been discussed. Moreover, we also provide insights into the current challenges and some considerations for further future studies.

摘要

随着人们对清洁能源需求的增加, 以及对环境可持续性的担忧日益加剧, 通过绿色化学生产清洁燃料受到越来越多的关注。氨是化石燃料的绿色替代品, 可以作为清洁能源。目前, 人们对实现大气中氮气 (N2) 的电化学还原以生产氨 (NH3), 从而在全球范围内实现廉价、环保和可靠的氨生产产生了浓厚兴趣。然而, N2中三键的稳定性以及催化剂的低效率限制了这一转化的实用性。单原子催化剂因其独特的性质而比纳米催化剂更高效, 并已被广泛应用于氮还原反应 (NRR) 。在这篇综述中, 我们介绍了2018 − 2022年以来用于电化学氮还原的贵金属和非贵金属基单原子催化剂 (SAC) 的设计和合成的最新进展。基于对配位环境和理论计算的研究, 对催化剂的效率进行了讨论。此外, 还在与NRR的进一步研究相关的当前挑战和未来前景方面提出了我们的见解。

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Fig. 1
Fig. 2

Reproduced with permission from Ref. [45]. Copyright 2019, the Royal Society of Chemistry

Fig. 3

Reproduced with permission from Ref. [47]. Copyright 2016, American Chemical Society

Fig. 4

Reproduced with permission from Ref. [60]. Copyright 2015, Elsevier. b Comparison of HER and NRR limiting-potential volcanoes. HER and NRR overpotentials (UL) as a function of *N binding-energy (ΔGN) descriptor are shown in blue and black, respectively, and individual metal points are labeled for (111) (left) and (211) (right) surfaces. Here from the graph, it is clear that HER limiting potentials are consistently less negative than those for NRR. Reproduced with permission from Ref. [61]. Copyright 2018, American Chemical Society

Fig. 5

Reproduced with permission from Ref. [69]. Copyright 2013, Springer Nature. b Schematic illustration of thermally stable Pd catalyst synthesized using ALD. Redrawn from Ref. [70]. Copyright 2016, the Royal Society of Chemistry. c Schematic illustration of metal SACs on graphene oxide (GO). Reproduced with permission from Ref. [71]. Copyright 2018, Springer Nature. d Schematic diagram of synthesis of Ni/graphdiyne and Fe/graphdiyne (GD). Reproduced with permission from Ref. [73]. Copyright 2018, Nature Publishing Group. e Deposition of iridium species. Panels (1) and (2) show cathodic and anodic electrochemical deposition mechanism, respectively; iridium mass loadings as a function of iridium concentration in 1 mol·L−1 KOH electrolyte for (3) cathodic and (4) anodic deposition. Cycle number of scanning was set at 10 and 3 for cathodic and anodic deposition, respectively. Reproduced with permission from Ref. [74]. Copyright 2020, Nature Publishing Group

Fig. 6
Fig. 7

Reproduced with permission from Ref. [27]. Copyright 2019, WILEY–VCH Verlag GmbH & Co. KGaA, Weinheim

Fig. 8

Reproduced with permission from Ref. [117]. Copyright 2019, American Chemical Society

Fig. 9

Reproduced with permission from Ref. [121]. Copyright 2019, WILEY–VCH Verlag GmbH & Co. KGaA, Weinheim

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 21972010) and Beijing Natural Science Foundation (No. 2192039).

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Authors and Affiliations

  1. Department of Chemical Engineering, COMSATS University Islamabad, Lahore, 54000, Pakistan

    Muhammad Saqlain Iqbal & Syed Muhammad Imran

  2. State Key Laboratory of Organic-Inorganic Composites, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, China

    Zhi-Bo Yao, Yu-Kun Ruan, Lei-Duan Hao & Zhen-Yu Sun

  3. Department of Chemistry, Government College University Faisalabad, Faisalabad, 38000, Pakistan

    Ramsha Iftikhar

  4. Department of Physics, University of Warwick, Coventry, CV4 7AL, UK

    Alex W. Robertson

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Iqbal, M.S., Yao, ZB., Ruan, YK. et al. Single-atom catalysts for electrochemical N2 reduction to NH3. Rare Met. 42, 1075–1097 (2023). https://doi.org/10.1007/s12598-022-02215-7

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