采用同步加速器SVUV-PIMS技术捕获草酸二甲酯加氢过程中的(CHO)Cu1*物质
DOI:
https://doi.org/10.18686/cncest.v2i3.228关键词:
SVUV-PIMS;草酸二甲酯加氢;铜纳米粒子;脱铝β沸石;中间体;催化剂稳定性摘要
采用同步辐射真空紫外光电离质谱(synchrotron vacuum ultraviolet photoionization mass spectrometry,SVUV-PIMS)捕捉中间产物极大地促进了对催化反应的理解。这篇评论介绍了SVUV-PIMS的结构,然后重温了一项出色的科学工作,该工作利用SVUV-PIMS阐明了草酸二甲酯(mechanisms of dimethyl oxalate,DMO)在铜纳米颗粒(copper nanoparticles,Cu NPs)支撑的脱铝β沸石(dealuminated Beta zeolite,Beta-deAl)上加氢转化为乙二醇的机理。采用SVUV-PIMS观察关键中间产物,特别是(CHO)Cu1*物质,可实时、原位地了解Cu NPs在DMO加氢过程中的动态行为。研究结果表明,甲醇处理后形成了硅醇巢,并出现了金属铜和Cu2O相。这种处理有助于保持较小的纳米颗粒尺寸,从而获得较高的乙二醇产率和较长的催化剂稳定性。此外,他们的催化剂还解决了二氧化硅浸出等常见问题,这些问题往往会影响基于CuSiO2基催化剂的耐久性。通过重新审视他们的工作,这篇评论强调了SVUV-PIMS在催化研究中的变革潜力,对反应中间产物的操作适应性对于开发更高效、更耐用的催化剂非常宝贵。
参考
Li Y, Qi F. Recent applications of synchrotron VUV photoionization mass spectrometry: Insight into combustion chemistry. Accounts of Chemical Research. 2009; 43(1): 68-78. doi: 10.1021/ar900130b
Li X, Sun Y, Xu J, et al. Selective visible-light-driven photocatalytic CO2 reduction to CH4 mediated by atomically thin CuIn5S8 layers. Nature Energy. 2019; 4(8): 690-699. doi: 10.1038/s41560-019-0431-1
Musab Ahmed S, Ren J, Ullah I, et al. Ni‐based catalysts for CO2 methanation: Exploring the support role in structure‐activity relationships. ChemSusChem. 2024; 17(9). doi: 10.1002/cssc.202400310
Qi F. Combustion chemistry probed by synchrotron VUV photoionization mass spectrometry. Proceedings of the Combustion Institute. 2013; 34(1): 33-63. doi: 10.1016/j.proci.2012.09.002
Takahashi LK, Zhou J, Wilson KR, et al. Imaging with mass spectrometry: A secondary ion and VUV-photoionization study of ion-sputtered atoms and clusters from GaAs and Au. The Journal of Physical Chemistry A. 2009; 113(16): 4035-4044. doi: 10.1021/jp810408v
Wen W, Yu S, Zhou C, et al. Formation and fate of formaldehyde in methanol-to-hydrocarbon reaction: In situ synchrotron radiation photoionization mass spectrometry study. Angewandte Chemie International Edition. 2020; 59(12): 4873-4878. doi: 10.1002/anie.201914953
Liu L, Lu J, Yang Y, et al. Dealuminated Beta zeolite reverses Ostwald ripening for durable copper nanoparticle catalysts. Science. 2024; 383(6678): 94-101. doi: 10.1126/science.adj1962
van den Berg R, Parmentier TE, Elkjær CF, et al. Support functionalization to retard Ostwald ripening in copper methanol synthesis catalysts. ACS Catalysis. 2015; 5(7): 4439-4448. doi: 10.1021/acscatal.5b00833
##submission.downloads##
已出版
文章引用
期
栏目
执照
版权声明
CC BY-NC 4.0