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.

中文翻译：

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利用协同调制水热法高产率合成 NOx 的 NH3-SCR 准 MOF


金属有机框架 （MOF） 由于其可调的孔径和活性位点，在低温反硝化 （de-NOx） 方面具有巨大的前景，然而，它们的实际应用受到低产率的阻碍。在这项研究中，我们介绍了一种协同调制水热 （SMHT） 方法，旨在使用乙酸和 N，N-二甲基甲酰胺协同控制团簇前和溶液 pH 值，以提高 MOF 产量。与水热法合成的 TEOS&Mn-BTC-BTC 催化剂相比，SMHT 法合成的 TEOS&Mn-BTC-HY 催化剂成功地将产率从输入的 21 % 提高到 63 %。表征分析和性能测试表明，TEOS&Mn-BTC-HY 的结构受 SMHT 方法的影响最小，其性能仍然优异。在 90–300 °C 的温度范围内，脱硝效率保持在 90% 以上，即使在 6% H2O 或 100 ppm SO2 在 150 °C 下持续 10 小时，性能仍然超过 90%。设计的 SMHT 工艺为扩大 MOF 生产和进一步推进 MOF 在脱硝领域的应用提供了有价值的见解。