Revealing Brønsted Acidic Bridging SiOHAl Groups on Amorphous Silica-Alumina by Ultrahigh Field Solid-State NMR.

Revealing Brønsted Acidic Bridging SiOHAl Groups on Amorphous Silica-Alumina by Ultrahigh Field Solid-State NMR.
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超高场固体核磁共振揭示非晶硅铝上的Brønsted酸桥SiOHAl基团。

DOI:
10.1021/acs.jpclett.1c02975
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发表时间:
2021-12-02
影响因子:
5.7
通讯作者:
Huang, Jun
Huang, Jun
中科院分区:
化学2区
文献类型:
--
作者:
Wang, Zichun;Chen, Kuizhi;Jiang, Yijiao;Trebosc, Julien;Yang, Wenjie;Amoureux, Jean-Paul;Hung, Ivan;Gan, Zhehong;Baiker, Alfons;Lafon, Olivier;Huang, Jun

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无定形硅铝(ASA)是重要的酸性催化剂和许多工业上必不可少的和可持续的过程的载体。确定表面酸位点及其局部结构对调节其催化性能至关重要,但仍然是一个巨大的挑战和争论。在这里,超高磁场(35.2 T)27 Al-{1H} D-HMQC(偶极介导的异核多量子相关)二维NMR实验证明了阿萨催化剂中的两种类型的布朗斯特酸位点。除了已知的假桥连硅醇酸位点之外,超高场NMR的使用为ASA中存在桥连硅醇(BS:SiOHA 1)酸位点提供了第一个直接的实验证据,这在过去几十年中一直受到激烈的争论。这一发现为科学家和工程师在各种反应过程中开发和应用ASA提供了新的机会,因为BS在化学和燃料生产中的重要性基于其强大的布朗斯台德酸性。
Amorphous silica-aluminas (ASAs) are important acidic catalysts and supports for many industrially essential and sustainable processes. The identification of surface acid sites with their local structures on ASAs is of critical importance for tuning their catalytic properties, but still remains a great challenge and under debate. Here, ultra-high magnetic field (35.2 T) 27Al-{1H} D-HMQC (dipolar-mediated hetero-nuclear multiple-quantum correlation) two-dimensional NMR experiments demonstrate two types of Brønsted acid sites in ASA catalysts. In addition to the known pseudo-bridging silanol acid site, the use of ultra-high field NMR provides the first direct experimental evidence for the existence of bridging silanol (BS: SiOHAl) acid sites in ASAs, which has been hotly debated in the past few decades. This discovery provides new opportunities for scientists and engineers to develop and apply ASAs in various reaction processes, due to the significance of BS in chemical and fuel productions based on its strong Brønsted acidity.
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