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Homogenous graphene oxide-peptide nanofiber hybrid hydrogel as biomimetic polysaccharide hydrolase
Nanoscale ( IF 5.8 ) Pub Date : 2017-10-30 00:00:00 , DOI: 10.1039/c7nr06525f Xingxing He 1, 2, 3, 4, 5 , Fuyuan Zhang 1, 2, 3, 4, 5 , Jifeng Liu 1, 2, 3, 4, 5 , Guozhen Fang 1, 2, 3, 4, 5 , Shuo Wang 1, 2, 3, 4, 5
Nanoscale ( IF 5.8 ) Pub Date : 2017-10-30 00:00:00 , DOI: 10.1039/c7nr06525f Xingxing He 1, 2, 3, 4, 5 , Fuyuan Zhang 1, 2, 3, 4, 5 , Jifeng Liu 1, 2, 3, 4, 5 , Guozhen Fang 1, 2, 3, 4, 5 , Shuo Wang 1, 2, 3, 4, 5
Affiliation
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Cellulose, an impressive potential sustainable fuel, is difficult to hydrolyze because of the protection of β-1,4-glycosidic bonds through the tight hydrogen bonding network. In this study, homogenous graphene oxide (GO)-peptide nanofiber hybrid hydrogels (GO-PNFs) were designed as a β-glycosyl hydrolase mimetic to achieve efficient degradation of cellobiose and cellopentaose. For comparison, free peptides, graphene oxide mixed with free peptides (GO-peptdies) and self-assembled peptide nanofibers (PNFs) were also studied for their activity as a hydrolase mimetics for degradation of cellobiose. Among these materials, GO-PNFs showed the highest hydrolysis activity. Transmission electron microscopy, atomic force microscopy, fluorescence analysis, circular dichroism spectroscopies, X-ray diffraction, Raman spectra and computational modeling were used to interpret the difference in activity mechanism in these artificially designed enzymes. These investigations suggested that high catalytic performance of GO-PNFs toward cellobiose and cellopentaose hydrolysis could be attributed to the formation of nanofiber structures of peptides, optimal molecular conformation and less steric hindrance to access the substrate. More importantly, GO not only served as a platform for attaching PNFs, but also created a hydrophobic microenvironment and facilitated proton transfer, an essential step in catalytic hydrolysis, thus enhancing catalytic activity. All these provided insights into the potential use of peptides and GO hybrid composite nanoenzymes in efficient cellulose hydrolysis.
中文翻译：
均相氧化石墨烯-肽纳米纤维杂化水凝胶作为仿生多糖水解酶
纤维素是一种令人印象深刻的潜在可持续燃料，由于其紧密的氢键网络保护了β-1,4-糖苷键，因此难以水解。在这项研究中，均相氧化石墨烯（GO）-肽纳米纤维杂化水凝胶（GO-PNFs）被设计为β-糖基水解酶模拟物，以实现纤维二糖和纤维戊糖的有效降解。为了进行比较，还研究了游离肽，与游离肽混合的氧化石墨烯（GO肽）和自组装肽纳米纤维（PNF）作为水解酶模拟物降解纤维二糖的活性。在这些材料中，GO-PNFs表现出最高的水解活性。透射电子显微镜，原子力显微镜，荧光分析，圆二色性光谱，X射线衍射，拉曼光谱和计算模型被用来解释这些人工设计的酶在活性机制上的差异。这些研究表明，GO-PNF对纤维二糖和纤维戊糖水解的高催化性能可能归因于肽的纳米纤维结构的形成，最佳的分子构象和较少的进入基质的空间障碍。更重要的是，GO不仅充当附着PNF的平台，而且还创造了疏水性微环境并促进了质子转移，这是催化水解的必要步骤，从而增强了催化活性。所有这些都为深入了解肽和GO杂化复合纳米酶在有效纤维素水解中的潜在用途提供了见识。
更新日期：2017-11-23
中文翻译：
均相氧化石墨烯-肽纳米纤维杂化水凝胶作为仿生多糖水解酶
纤维素是一种令人印象深刻的潜在可持续燃料，由于其紧密的氢键网络保护了β-1,4-糖苷键，因此难以水解。在这项研究中，均相氧化石墨烯（GO）-肽纳米纤维杂化水凝胶（GO-PNFs）被设计为β-糖基水解酶模拟物，以实现纤维二糖和纤维戊糖的有效降解。为了进行比较，还研究了游离肽，与游离肽混合的氧化石墨烯（GO肽）和自组装肽纳米纤维（PNF）作为水解酶模拟物降解纤维二糖的活性。在这些材料中，GO-PNFs表现出最高的水解活性。透射电子显微镜，原子力显微镜，荧光分析，圆二色性光谱，X射线衍射，拉曼光谱和计算模型被用来解释这些人工设计的酶在活性机制上的差异。这些研究表明，GO-PNF对纤维二糖和纤维戊糖水解的高催化性能可能归因于肽的纳米纤维结构的形成，最佳的分子构象和较少的进入基质的空间障碍。更重要的是，GO不仅充当附着PNF的平台，而且还创造了疏水性微环境并促进了质子转移，这是催化水解的必要步骤，从而增强了催化活性。所有这些都为深入了解肽和GO杂化复合纳米酶在有效纤维素水解中的潜在用途提供了见识。
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