Geometrical and Chemical-Dependent Hydrolysis Mechanisms of Silicon Nanomembranes for Biodegradable Electronics
Geometrical and Chemical-Dependent Hydrolysis Mechanisms of Silicon Nanomembranes for Biodegradable Electronics
复制标题
用于可生物降解电子产品的硅纳米膜的几何和化学依赖性水解机制
DOI：
10.1021/acsami.9b03546
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发表时间：
2019
影响因子：
9.5
通讯作者：
Yin Lan
中科院分区：
文献类型：
--
作者：
Wang Liu;Gao Yuan;Dai Fanqi;Kong Deying;Wang Huachun;Sun Pengcheng;Shi Zhao;Sheng Xing;Xu Baoxing;Yin Lan
在生理或环境溶液中物理消失的可生物降解电子设备对于医疗保健管理和环境可持续性的广泛应用至关重要。然而，材料和器件的溶解与按需使用寿命的精确调节仍然是一个关键挑战。硅纳米膜(SiNMS)是系统级高性能生物可降解电子器件的重要半导体元件之一。在这项工作中，我们发现了硅纳米管的异常水解行为，这在很大程度上取决于器件的尺寸以及它们的表面化学状态。实验表明，较大尺寸的p型硅纳米管的水解率显著提高，机械搅拌使溶解速率显著降低。溶液中磷酸盐和钾离子的存在，或较低掺杂水平的Si NMS都会促进Si NMS的降解，并会导致更强的尺寸效应。通过分子动力学模拟揭示了不同表面电荷状态下Si NMS的离子吸附机理，验证了我们的实验结果。通过几何设计，形成了溶解寿命可调的纳米硅电极阵列，并对其体外电化学性质进行了分析。这些结果为通过几何设计和表面化学修饰来调节Si NMS的工作时间框架提供了新的控制策略，并为工程高性能生物降解电子学提供了重要的基础性认识。
Biodegradable electronic devices that physically disappear in physiological or environmental solutions are of critical importance for widespread applications in healthcare management and environmental sustainability. The precise modulation of materials and devices dissolution with on-demand operational lifetime, however, remain a key challenge. Silicon nanomembranes (Si NMs) are one of the essential semiconductor components for high-performance biodegradable electronics at the system level. In this work, we discover unusual hydrolysis behaviors of Si NMs that are significantly dependent on the dimensions of devices as well as their surface chemistry statuses. The experiments show a pronounced increase in hydrolysis rates of p-type Si NMs with larger sizes, and mechanical stirring introduces a significant decrease in dissolution rates. The presence of phosphates and potassium ions in solutions, or lower dopant levels of Si NMs will facilitate the degradation of Si NMs and will also lead to a stronger size-dependent effect. Molecular dynamics simulations are performed to reveal ion adsorption mechanisms of Si NMs under different surface charge statuses and confirm our experimental observations. Through geometrical designs, Si NM-based electrode arrays with tunable dissolution lifetime are formed, and their electrochemical properties are analyzed in vitro. These results offer new controlling strategies to modulate the operational time frames of Si NMs through geometrical design and surface chemistry modification and provide crucial fundamental understandings for engineering high-performance biodegradable electronics.