Aasi Aref, Mehdi Aghaei Sadegh, Panchapakesan Balaji
Small Systems Laboratory, Department of Mechanical Engineering, Worcester Polytechnic Institute, Worcester, Massachusetts 01609, United States.
ACS Omega. 2021 Feb 5;6(7):4696-4707. doi: 10.1021/acsomega.0c05495. eCollection 2021 Feb 23.
In the present work, we report highly sensitive and selective nanosensors constructed with metal-decorated graphene-like BCN employing nonequilibrium Green's function (NEGF) formalism combined by density functional theory (DFT) toward multiple inorganic and sulfur-containing gas molecules (NO, NO, NH, CO, CO, HS, and SO) as disease biomarkers from human breath. Monolayer sheets of pristine BCN and Pd-decorated BCN were evaluated for their gas adsorption properties, electronic property changes, sensitivity, and selectivity toward disease biomarkers. The pristine BCN nanosheets exhibited sharp drops in the bandgap when interacted with gases such as NO while barely affected by other gases. However, the nanosecond recovery time and low adsorption energies limit the gas sensing applications of the pristine BCN sheet. On the other hand, the Pd-decorated BCN-based sensor underwent a semiconductor to metal transition upon the adsorption of NO gas molecules. The conductance change of the sensor's material in terms of - characteristics revealed that the Pd-decorated BCN sensor is highly sensitive (98.6-134%) and selective (12.3-74.4 times) toward NO gas molecules with a recovery time of 270 s under UV radiation at 498 K while weakly interacting with interfering gases in exhaled breath such as CO and HO. The gas adsorption behavior suggests that metal-decorated BCN sensors are excellent candidates for analyzing pulmonary disease and cardiovascular biomarkers, among other ailments of the stomach, kidney, and intestine.
在本工作中，我们报道了采用非平衡格林函数（NEGF）形式结合密度泛函理论（DFT）构建的对多种无机和含硫气体分子（NO、NO、NH、CO、CO、HS和SO）具有高灵敏度和选择性的纳米传感器，这些气体分子作为来自人类呼出气体的疾病生物标志物。评估了原始BCN和钯修饰的BCN单层片材的气体吸附特性、电子性质变化、对疾病生物标志物的灵敏度和选择性。原始BCN纳米片与NO等气体相互作用时带隙急剧下降，而几乎不受其他气体影响。然而，纳秒级的恢复时间和低吸附能限制了原始BCN片材的气体传感应用。另一方面，基于钯修饰的BCN的传感器在吸附NO气体分子时经历了从半导体到金属的转变。传感器材料的电导变化特性表明，钯修饰的BCN传感器对NO气体分子具有高灵敏度（98.6 - 134%）和选择性（12.3 - 74.4倍），在498 K的紫外辐射下恢复时间为270 s，同时与呼出气体中的干扰气体如CO和HO相互作用较弱。气体吸附行为表明，金属修饰的BCN传感器是分析肺部疾病和心血管生物标志物以及胃、肾和肠道等其他疾病的优秀候选者。
