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Operando Monitoring of the Polymerization Process of Lignin Monomer and Oligomer Surrogates with Microstructured Fiber Grating Sensor
Analytical Chemistry ( IF 6.7 ) Pub Date : 2024-09-04 , DOI: 10.1021/acs.analchem.4c02791
Xin Xin 1, 2 , Junjun Wu 1, 2 , Ao Xia 1, 2 , Yun Huang 1, 2 , Xianqing Zhu 1, 2 , Xun Zhu 1, 2 , Qiang Liao 1, 2
Affiliation  

The enzymatic depolymerization is a promising route to valorize the lignin polymers by turning the cross-linked polymers into monomers or oligomers. However, the lignin polymers cannot be effectively converted into small chemicals, as the oligomers are prone to polymerization, which is particularly challenging to monitor and thus regulate. Here, we develop a microstructured fiber Bragg grating (mFBG) sensor to probe the dynamic polymerization process of typical lignin oligomer surrogates─guaiacol (monomer) and guaiacylglycerol-β-guaiacyl ether (GBG, dimer)─catalyzed by laccase in an operando way. The mFBG sensor was developed with its reliability well validated by control experiments at first. Further, operando monitoring of the polymerization reaction process of the typical lignin monomer (i.e., guaiacol) and dimer (guaiacylglycerol-β-guaiacyl ether, GBG) was demonstrated under various conditions with the mFBG sensor. The GC-MS and UV–vis absorption measurements were carried out as a further check. Finally, the specific polymerization characteristics and reaction mechanism were studied. The mFBG sensor enables operando monitoring of the heterogeneous polymerization process of lignin monomers and oligomers and can potentially be tailored to probe more complex lignin depolymerization processes and unveil enzymatic synergistic mechanisms for the biological transition of biomass.

中文翻译:


使用微结构纤维光栅传感器对木质素单体和低聚物替代物的聚合过程进行原位监测



酶解聚是通过将交联聚合物转化为单体或低聚物来使木质素聚合物增值的一种很有前途的途径。然而,木质素聚合物不能有效地转化为小的化学品,因为低聚物容易发生聚合,这尤其难以监测和调节。在这里,我们开发了一种微结构纤维布拉格光栅 (mFBG) 传感器,以探测典型的木质素寡聚物替代物——愈创木酚(单体)和愈创木酚-β-愈创木酚醚(GBG,二聚体)——在漆酶以原位方式催化的动态聚合过程。mFBG 传感器的可靠性最初通过对照实验得到了很好的验证。此外,在各种条件下,mFBG 传感器证明了典型木质素单体(即愈创木酚)和二聚体(愈创木酚-β-愈创木酚醚,GBG)的聚合反应过程的原位监测。进行 GC-MS 和 UV-Vis 吸收测量作为进一步检查。最后,研究了具体的聚合特性和反应机理。mFBG 传感器能够对木质素单体和低聚物的异质聚合过程进行原位监测,并且可以进行定制以探测更复杂的木质素解聚过程,并揭示生物质生物转变的酶协同机制。
更新日期:2024-09-04
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