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能带中心上移至费米能级以促进银离子释放、细菌失活和合金纳米银的伤口愈合。

Upshift of the d Band Center toward the Fermi Level for Promoting Silver Ion Release, Bacteria Inactivation, and Wound Healing of Alloy Silver Nanoparticles.

机构信息

University of Chinese Academy of Sciences , Beijing 10049 , China.

University of Science and Technology of China , Hefei , Anhui 230026 , China.

出版信息

ACS Appl Mater Interfaces. 2019 Apr 3;11(13):12224-12231. doi: 10.1021/acsami.8b21768. Epub 2019 Mar 21.

Abstract

Silver (Ag)-based nanoparticles (NPs) with a high potential of Ag release have been known to be capable of promoting bacteria inactivation and the wound healing process; however, keeping a steady flux of high levels of Ag in Ag-based NPs is still challenging. Herein, a novel strategy in terms of altering the intrinsic electronic structure of Ag NPs was attempted to facilitate Ag oxidation and boost the Ag flux, as results of improved antibacterial and wound healing performance of Ag NPs. Gold (Au), platinum (Pt), and palladium (Pd) were doped into Ag NPs to tune their d band centers to upshift toward the Fermi level, and the formed Pd-Ag alloy NPs showed the largest shift, followed by Pt-Ag and Au-Ag NPs, as determined by density function theory calculation and ultraviolet photoemission spectroscopy measurement. Further X-ray photoelectron spectroscopy analysis indicates that a larger upshift could induce less electron filling in the antibonding orbital and a higher Ag oxidation level, leading to the more remarkable Ag release as determined by inductively coupled plasma optical emission spectrometry. All these alloy Ag NPs could more efficiently inhibit bacterial growth and accelerate the wound healing process than pure Ag NPs, and their antibacterial activity and wound healing performance were progressively proportional to the upshift values of the d band center. Taken together, tuning the d band center to upshift toward the Fermi level becomes a feasible strategy for designing therapeutic Ag-based NPs with a promising antibacterial and wound healing performance.

摘要

具有高银释放潜力的银(Ag)基纳米颗粒(NPs)已被证明能够促进细菌失活和伤口愈合过程;然而,保持Ag 基 NPs 中高水平稳定的 Ag 通量仍然具有挑战性。在此,尝试了一种改变 Ag NPs 本征电子结构的新策略,以促进 Ag 氧化并提高 Ag 通量,从而提高 Ag NPs 的抗菌和伤口愈合性能。将金(Au)、铂(Pt)和钯(Pd)掺杂到 Ag NPs 中,以将它们的 d 带中心调谐到费米能级以上,并且形成的 Pd-Ag 合金 NPs 显示出最大的偏移,其次是 Pt-Ag 和 Au-Ag NPs,这是通过密度泛函理论计算和紫外光电子能谱测量确定的。进一步的 X 射线光电子能谱分析表明,更大的上移可以导致反键轨道中电子填充减少和更高的 Ag 氧化水平,从而导致电感耦合等离子体发射光谱更显著的 Ag 释放。所有这些合金 Ag NPs 都比纯 Ag NPs 更有效地抑制细菌生长并加速伤口愈合过程,其抗菌活性和伤口愈合性能与 d 带中心上移值成正比。综上所述,将 d 带中心调谐到费米能级以上是设计具有良好抗菌和伤口愈合性能的治疗性 Ag 基 NPs 的一种可行策略。

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