Interactions of Catalytic Enzymes with n-Type Polymers for High-Performance Metabolite Sensors.
Interactions of Catalytic Enzymes with n-Type Polymers for High-Performance Metabolite Sensors.
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DOI：
10.1021/acsami.2c20502
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发表时间：
2023-02-07
影响因子：
9.5
通讯作者：
Inal, Sahika
中科院分区：
文献类型：
--
作者：
Ohayon, David;Renn, Dominik;Wustoni, Shofarul;Guo, Keying;Druet, Victor;Hama, Adel;Chen, Xingxing;Maria, Iuliana Petruta;Singh, Saumya;Griggs, Sophie;Schroeder, Bob C.;Rueping, Magnus;McCulloch, Iain;Inal, Sahika
关键词：
对体内葡萄糖浓度的严格调节对平衡生理功能至关重要。我们开发了一种包括n型共轭聚合物薄膜的电化学晶体管，该薄膜与催化酶接触，用于灵敏和选择性地检测体液中的葡萄糖。尽管这些传感器前景看好，但导致如此高性能的聚合物的性质仍然未知，电荷传输是人们关注的唯一特征。在这里，我们结合物理化学表征方法研究了聚合物化学结构对薄膜表面性质和酶吸附行为的影响，并将我们的发现与所产生的传感器性能进行了关联。我们开发了五种具有相同主链的n型聚合物，侧链的极性和电荷不同。我们发现，侧链的性质调节了膜的表面性质，决定了酶和聚合物膜之间相互作用的程度。石英晶体微天平与耗散监测研究表明，疏水表面以密集排列的方式保留了更多的酶，而亲水表面以平坦的构象捕获了较少的酶。表面的X射线光电子能谱分析表明，酶与聚合物的乙醇化侧链有很强的相互作用，与支链相比，线形侧链的相互作用更好。我们用圆二色谱探讨了吸附过程中酶结构的变化，这表明蛋白质在疏水表面发生了变性。我们的研究结论是，带负电荷、光滑和亲水性的薄膜表面为酶的吸附提供了最佳的环境，具有所需的质量和构象，从而最大化了传感器的性能。这些知识将指导旨在建立蛋白质和电子材料之间密切相互作用的合成工作，这对于开发高性能的酶代谢物生物传感器和生物催化电荷转换设备至关重要。
The tight regulation of the glucose concentration in the body is crucial for balanced physiological function. We developed an electrochemical transistor comprising an n-type conjugated polymer film in contact with a catalytic enzyme for sensitive and selective glucose detection in bodily fluids. Despite the promise of these sensors, the property of the polymer that led to such high performance has remained unknown, with charge transport being the only characteristic under focus. Here, we studied the impact of the polymer chemical structure on film surface properties and enzyme adsorption behavior using a combination of physiochemical characterization methods and correlated our findings with the resulting sensor performance. We developed five n-type polymers bearing the same backbone with side chains differing in polarity and charge. We found that the nature of the side chains modulated the film surface properties, dictating the extent of interactions between the enzyme and the polymer film. Quartz crystal microbalance with dissipation monitoring studies showed that hydrophobic surfaces retained more enzymes in a densely packed arrangement, while hydrophilic surfaces captured fewer enzymes in a flattened conformation. X-ray photoelectron spectroscopy analysis of the surfaces revealed strong interactions of the enzyme with the glycolated side chains of the polymers, which improved for linear side chains compared to those for branched ones. We probed the alterations in the enzyme structure upon adsorption using circular dichroism, which suggested protein denaturation on hydrophobic surfaces. Our study concludes that a negatively charged, smooth, and hydrophilic film surface provides the best environment for enzyme adsorption with desired mass and conformation, maximizing the sensor performance. This knowledge will guide synthetic work aiming to establish close interactions between proteins and electronic materials, which is crucial for developing high-performance enzymatic metabolite biosensors and biocatalytic charge-conversion devices.
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影响因子：
5.6
作者：
HECHT, HJ;KALISZ, HM;SCHOMBURG, D
通讯作者：
SCHOMBURG, D
影响因子：
3.3
作者：
Muguruma, Hitoshi;Kase, Yoshihiro;Matsumura, Kazunari
通讯作者：
Matsumura, Kazunari
DOI：
10.1021/la901885d
发表时间：
2009-08-18
期刊：
Langmuir : the ACS journal of surfaces and colloids
影响因子：
--
作者：
Fears KP;Sivaraman B;Powell GL;Wu Y;Latour RA
通讯作者：
Latour RA
影响因子：
6.2
作者：
Bhakta SA;Evans E;Benavidez TE;Garcia CD
通讯作者：
Garcia CD
DOI：
10.1021/acs.chemmater.8b00321
发表时间：
2018-05-08
期刊：
Chemistry of materials : a publication of the American Chemical Society
影响因子：
--
作者：
Giovannitti A;Maria IP;Hanifi D;Donahue MJ;Bryant D;Barth KJ;Makdah BE;Savva A;Moia D;Zetek M;Barnes PRF;Reid OG;Inal S;Rumbles G;Malliaras GG;Nelson J;Rivnay J;McCulloch I
通讯作者：
McCulloch I