Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States.
ACS Appl Mater Interfaces. 2022 Aug 31;14(34):39515-39523. doi: 10.1021/acsami.2c09555. Epub 2022 Aug 19.
Self-powered, biocompatible pumps in the nanometer to micron length scale have the potential to enable technology in several fields, including chemical analysis and medical diagnostics. Chemically powered, catalytic micropumps have been developed but are not able to function well in biocompatible environments due to their intolerance of salt solutions and the use of toxic fuels. In contrast, enzymatically powered catalytic pumps offer good biocompatibility, selectivity, and scalability, but their performance at length scales below a few millimeters, which is important to many of their possible applications, has not been well tested. Here, urease-based enzyme pumps of millimeter and micrometer dimensions were fabricated and studied. The scaling of the pumping velocity was measured experimentally and simulated by numerical modeling. Pumping speeds were analyzed accurately by eliminating Brownian noise from the data using enzyme patches between 5 mm and 350 μm in size. Pumping speeds of microns per second could be achieved with urease pumps and were fastest when the channel height exceeded the width of the catalytic pump patch. In all cases, pumping was weak when the dimensions of the patch were 100 μm or less. Experimental and simulation results were consistent with a density-driven pumping mechanism at all sizes studied and served as a framework for the in silico study of more complex two-dimensional (2D) and three-dimensional (3D) geometries. Attempts to create directional flow by juxtaposing inward and outward pumps were unsuccessful because of the symmetry of convection rolls produced by millimeter-size pump patches and the slow speeds of smaller pumps. However, simulations of a corrugated ratchet structure showed that directional pumping could be achieved with pump patches in the millimeter size range.
自供电、生物兼容的纳米到微米级别的泵具有在多个领域实现技术的潜力,包括化学分析和医疗诊断。已经开发出了化学动力、催化微型泵,但由于它们不能耐受盐溶液和使用有毒燃料,因此在生物兼容环境中不能很好地工作。相比之下,酶动力催化泵具有良好的生物兼容性、选择性和可扩展性,但在几毫米以下的长度尺度上的性能尚未得到很好的测试,这对于它们许多可能的应用至关重要。在这里,我们制造并研究了毫米和微米级别的基于脲酶的酶泵。通过数值模拟实验测量和模拟了泵送速度的缩放。通过使用酶片在 5 毫米到 350 微米之间的大小从数据中消除布朗噪声,准确地分析了泵送速度。可以实现每秒微米级的泵送速度,当通道高度超过催化泵片的宽度时,泵送速度最快。在所有情况下,当贴片尺寸为 100 微米或更小尺寸时,泵送都很弱。实验和模拟结果与在所有研究尺寸下的密度驱动泵送机制一致,并为更复杂的二维(2D)和三维(3D)几何形状的计算机模拟研究提供了框架。由于毫米尺寸泵片产生的对流卷的对称性以及较小泵的缓慢速度,通过并列向内和向外的泵来尝试产生定向流的尝试都没有成功。然而,波纹棘轮结构的模拟表明,通过在毫米尺寸范围内的泵片可以实现定向泵送。