Ultra-high-efficiency capture of lead ions over acetylenic bond-rich graphdiyne adsorbent in aqueous solution

作者:Xie, Shuanglei*; Pan, Chuanqi; Yao, Yuan; Yu, Xianglin; Xu, Ze; Yuan, Weidong; Zhang, Yi; Guo, Ning; Li, Xue; Mao, Xuefei; Xiao, Shengqiang; Li, Junbo*; Guo, Yanbing*
来源:PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2023, 120(16): e2221002120.
DOI:10.1073/pnas.2221002120

摘要

A satisfactory material with high adsorption capacity is urgently needed to solve the serious problem of environment and human health caused by lead pollution. Herein, hydrogen-substituted graphdiyne (HsGDY) was successfully fabricated and employed to remove lead ions from sewage and lead-containing blood. The as-prepared HsGDY exhibits the highest adsorption capacity of lead among the reported materials with a maximum adsorption capacity of 2,390 mg/g, i.e., similar to five times larger than that of graphdiyne (GDY). The distinguished hexagonal hole and stack mode of HsGDY allows the adsorption of more lead via its inner side adsorption mode in one single unit space. In addition, the Pb 6s and H 1s hybridization promotes the strong bonding of lead atom adsorbed at the acetylenic bond of HsGDY, contributing to the high adsorption capacity. HsGDY can be easily regenerated by acid treatment and showed excellent regeneration ability and reliability after six adsorption-regeneration cycles. Langmuir isotherm model, pseudo second order, and density functional theory (DFT) demonstrated that the lead adsorption process in HsGDY is monolayer chemisorption. Furthermore, the HsGDY-based portable filter can handle 1,000 mu g/L lead-containing aqueous solution up to 1,000 mL, which is nearly 6.67 times that of commercial activated carbon particles. And, the HsGDY shows good biocompatibility and excellent removal efficiency to 100 mu g/L blood lead, which is 1.7 times higher than that of GDY. These findings suggest that HsGDY could be a promising adsorbent for practical lead and other heavy metal removal.

  • 单位
    武汉理工大学; 武汉工程大学