High-yield synthesis of quasi-MOF using synergistic modulated hydrothermal process for NH3-SCR of NOx

IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL Process Safety and Environmental Protection Pub Date : 2024-09-11 DOI:10.1016/j.psep.2024.09.044
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Abstract

Metal-organic frameworks (MOFs) hold immense promise for low-temperature denitrification (de-NOx) owing to their tunable pore size and active sites, nevertheless, their practical application is impeded by low yields. In this investigation, we introduce a synergistic modulated hydrothermal (SMHT) method designed to cooperatively control pre-cluster and solution pH using acetic acid and N, N-dimethylformamide, with the aim of enhancing MOFs yields. The TEOS&Mn-BTC-HY catalyst synthesized by the method of SMHT successfully increased the yield from 21 % of the input to 63 % compared with the TEOS&Mn-BTC catalyst synthesized by the hydrothermal method. Characterization analysis and performance testing reveal that the structure of TEOS&Mn-BTC-HY is minimally affected by the SMHT method, and its performance remains excellent. The de-NOx efficiency remained above 90 % in the temperature range of 90–300 ℃, and even under challenging conditions such as 6 % H2O or 100 ppm SO2 at 150 ℃ for 10 h, the performance still exceeded 90 %. The designed SMHT process offers valuable insights for expanding MOFs production and further advancing the application of MOFs in the realm of de-NOx.

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利用协同调制水热法高产合成准MOF,用于氮氧化物的 NH3-SCR 处理
金属有机框架(MOFs)因其可调的孔径和活性位点而在低温脱硝(脱氮)方面前景广阔,但其实际应用却因产量低而受到阻碍。在这项研究中,我们介绍了一种协同调制水热法(SMHT),旨在利用醋酸和 N,N-二甲基甲酰胺协同控制预簇和溶液的 pH 值,从而提高 MOFs 的产量。与采用水热法合成的 TEOS&Mn-BTC 催化剂相比,采用 SMHT 法合成的 TEOS&Mn-BTC-HY 催化剂成功地将产率从投入量的 21% 提高到了 63%。表征分析和性能测试表明,TEOS&Mn-BTC-HY 的结构受 SMHT 方法的影响很小,其性能依然优异。在 90-300 ℃ 的温度范围内,其脱氮效率始终保持在 90% 以上,即使在极具挑战性的条件下,如 6% H2O 或 100ppm SO2 在 150 ℃ 下持续 10 小时,其性能仍然超过 90%。所设计的 SMHT 工艺为扩大 MOFs 的生产和进一步推动 MOFs 在脱氮领域的应用提供了宝贵的启示。
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来源期刊
Process Safety and Environmental Protection
Process Safety and Environmental Protection 环境科学-工程:化工
CiteScore
11.40
自引率
15.40%
发文量
929
审稿时长
8.0 months
期刊介绍: The Process Safety and Environmental Protection (PSEP) journal is a leading international publication that focuses on the publication of high-quality, original research papers in the field of engineering, specifically those related to the safety of industrial processes and environmental protection. The journal encourages submissions that present new developments in safety and environmental aspects, particularly those that show how research findings can be applied in process engineering design and practice. PSEP is particularly interested in research that brings fresh perspectives to established engineering principles, identifies unsolved problems, or suggests directions for future research. The journal also values contributions that push the boundaries of traditional engineering and welcomes multidisciplinary papers. PSEP's articles are abstracted and indexed by a range of databases and services, which helps to ensure that the journal's research is accessible and recognized in the academic and professional communities. These databases include ANTE, Chemical Abstracts, Chemical Hazards in Industry, Current Contents, Elsevier Engineering Information database, Pascal Francis, Web of Science, Scopus, Engineering Information Database EnCompass LIT (Elsevier), and INSPEC. This wide coverage facilitates the dissemination of the journal's content to a global audience interested in process safety and environmental engineering.
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