Rong Zhang, Xintao Ma, Shaoce Zhang, Huilin Cui, Chuan Li, Yanbo Wang, Qing Li, Prof. Chao Peng, Dr. Ying Guo, Prof. Chunyi Zhi
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引用次数: 0
摘要
氨(NH3)是重要的工业原料,是理想的能量载体,也是氢的理想储存介质。近年来,酸性条件下电化学还原NO3−的研究备受关注,但其效率有限,特别是在低NO3−浓度条件下。在这里,我们报道了在酸性条件下原位形成带正电的聚乙烯亚胺修饰Cu作为电化学NO3−还原为NH3的催化剂-电解质界面(CEI)。这种CEI可以通过静态相互作用有效地积累NO3−阴离子,通过削弱*NO中间吸附在Cu位点上,加速*NO加氢到*NOH,从而促进NO3−向nh3的转化。这种CEI在10 mM NO3 -溶液(pH = 1)中提供了83.5%的NH3法拉第效率(FE)和令人印象深刻的37.1%的半电池能量效率(EE)。在0.5 M NO3−条件下,NH3 FE和EE分别提高到90.2%和44.1%。CEI的高EE超过了之前报道的NO3−还原催化剂的性能。最后,我们展示了一种新型NO3−-糠醛电池的可行性,展示了一种能够同时处理NO3−污染物,产生增值NH3和升级生物质的自供电电催化系统。这项工作为构建催化剂-电解质界面以提高NH3合成效率提供了有价值的见解。
Acidic Nitrate Electroreduction with Ultrahigh Energy Efficiency
Ammonia (NH3) is an important feedstock for industry, an ideal energy carrier, and a perspective storage media for hydrogen. Recently, electrochemical nitrate (NO3−) reduction under acidic conditions has received considerable attention but it suffers from limited efficiency especially under low NO3− concentration. Here, we report an in situ formed positively charged polyethyleneimine-modified Cu under acidic conditions as a catalyst-electrolyte interface (CEI) for electrochemical NO3− reduction to NH3. Such CEI can effectively accumulate NO3− anions via static interactions and accelerate *NO hydrogenation to *NOH by weakening *NO intermediate adsorption on Cu site, thereby facilitating NO3−-to-NH3 conversion. Such CEI delivers an increased NH3 Faradaic efficiency (FE) of 83.5% and an impressive half-cell energy efficiency (EE) of 37.1% in 10 mM NO3− solution (pH = 1). The NH3 FE and EE can further increase to 90.2% and 44.1% in 0.5 M NO3−, respectively. The high EE of CEI surpasses previously reported catalyst performances for NO3− reduction. Finally, we demonstrate the feasibility of a novel NO3−-furfural battery, showcasing a self-power electrocatalytic system capable of simultaneously treating NO3− pollutants, generating value-added NH3 and upgrading biomass. This work offers valuable insights into the construction of a CEI to enhance the efficiency of NH3 synthesis.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.