Construction of Reaction System and Regulation of Catalyst Active Sites for Sustainable Ammonia Production

IF 14 Q1 CHEMISTRY, MULTIDISCIPLINARY Accounts of materials research Pub Date : 2024-10-28 DOI:10.1021/accountsmr.4c00103
Zhe Meng, Miao-Miao Shi, Jun-Min Yan
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Abstract

Ammonia (NH3) is widely used for human life and considered a green energy carrier without CO2 emissions; thus, green and sustainable NH3 synthesis is of great importance. The traditional Haber-Bosch process requires harsh conditions with serious environmental implications. Therefore, numerous research is focused on the efficient synthesis of NH3 from abundant N2/air and water under ambient conditions, utilizing renewable energy sources. Despite the fact that the electrocatalytic N2 reduction reaction (eNRR) is an ideal method for NH3 synthesis, the NH3 yield and Faradaic efficiency (FE) are severally hampered by the inertness of N2, impeding its industrial application. Various strategies have been proposed to synthesize highly efficient heterogeneous catalysts for N2 adsorption and dissociation to improve NH3 yield and FE. Besides, benefiting from the nonthermal plasma N2 oxidation reaction (pNOR) and electrocatalytic nitrate/nitrite reduction reaction (eNOxRR), the two-step approach overcomes the limitations of eNRR, attracting significant interest. This strategy facilitates N2 splitting, which is a crucial step in the synthesis of NH3. Additionally, eNOxRR involves complex intermediates, making it essential to investigate catalysts with high selectivity of NH3. Overall, through the optimization of catalysts and reaction systems, NH3 can be synthesized with high efficiency. The two-step strategy is the most realistic process for mass NH3 production, but several challenges still need to be addressed, including improving the overall energy efficiency and scaling up the technology for industrial applications.

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构建可持续氨生产的反应系统和调节催化剂活性位点
氨(NH3)被广泛应用于人类生活,并被认为是一种不排放二氧化碳的绿色能源载体,因此,绿色和可持续的 NH3 合成工艺具有重要意义。传统的 Haber-Bosch 工艺需要苛刻的条件,对环境造成严重影响。因此,大量研究集中在利用可再生能源,在环境条件下从丰富的 N2/空气和水中高效合成 NH3。尽管电催化 N2 还原反应(eNRR)是合成 NH3 的理想方法,但由于 N2 的惰性,NH3 产量和法拉第效率(FE)受到严重影响,阻碍了其工业应用。为了提高 NH3 产率和 FE,人们提出了各种策略来合成用于 N2 吸附和解离的高效异相催化剂。此外,得益于非热等离子体 N2 氧化反应(pNOR)和电催化硝酸盐/亚硝酸盐还原反应(eNOxRR),两步法克服了 eNRR 的局限性,引起了人们的极大兴趣。这种策略有利于 N2 分离,而 N2 分离是合成 NH3 的关键步骤。此外,eNOxRR 涉及复杂的中间产物,因此研究具有高 NH3 选择性的催化剂至关重要。总之,通过优化催化剂和反应体系,可以高效合成 NH3。两步法是大规模生产 NH3 的最现实的工艺,但仍有一些挑战需要解决,包括提高整体能效和扩大该技术的工业应用规模。
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