Benchmarking photocatalysts for dinitrogen photoreduction reaction

IF 11.5 Q1 CHEMISTRY, PHYSICAL Chem Catalysis Pub Date : 2024-10-02 DOI:10.1016/j.checat.2024.101128
Po-Wei Huang, Danae A. Chipoco Haro, Hakhyeon Song, Andrew J. Medford, Marta C. Hatzell
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Abstract

The photocatalytic nitrogen reduction reaction (pNRR) for ammonia (NH3) production is often discussed as a sustainable alternative to the thermocatalytic Haber-Bosch process. One of the main challenges in pNRR research is the lack of reliable detection of photochemically produced NH3 since NH3 concentrations are often low and nitrogen-containing impurities may be present. Here, we identify three key sources of contamination (feed gases, catalyst precursors, and hole scavengers) and systematically quantify and reduce the contamination. We developed a custom photoreactor setup to minimize contamination and benchmarked three photocatalysts previously reported to be active toward pNRR. Our results indicate that the pNRR rates of all three catalysts under benchmarking conditions are much lower than previously reported and in some cases have negligible activity. We suggest essential control experiments to contribute to the standardization of NH3 measurements in the pNRR field and to help the field elucidate the photoactivity of catalysts toward pNRR.

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二氮光氧化反应光催化剂的基准测试
用于生产氨气(NH3)的光催化氮还原反应(pNRR)经常作为热催化哈伯-博什工艺的可持续替代工艺而被讨论。pNRR 研究的主要挑战之一是缺乏对光化学产生的 NH3 的可靠检测,因为 NH3 浓度通常很低,而且可能存在含氮杂质。在此,我们确定了三个主要污染源(原料气体、催化剂前体和空穴清除剂),并系统地量化和减少了污染。我们开发了一种定制的光反应器装置,以最大限度地减少污染,并对之前报道的对 pNRR 具有活性的三种光催化剂进行了基准测试。我们的结果表明,在基准条件下,所有三种催化剂的 pNRR 转化率都比之前报道的低得多,在某些情况下,其活性甚至可以忽略不计。我们建议进行必要的对照实验,以促进 pNRR 领域的 NH3 测量标准化,并帮助该领域阐明催化剂对 pNRR 的光活性。
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来源期刊
CiteScore
10.50
自引率
6.40%
发文量
0
期刊介绍: Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.
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