具有增强类过氧化物酶活性的硼掺杂石墨氮化碳负载单原子铁催化剂

B-doped graphite carbon nitride loaded Fe single atoms with enhanced peroxidase-like activity

开发具有高活性的生物医药和环保催化剂是目前的研究热点.本文中,我们通过三聚氰胺与氧化硼混合搅拌后热解而获得硼掺杂石墨相氮化碳(B-g-C_(3)N_(4)).通过离子交换后热解的方式制备了硼掺杂石墨氮化碳上负载Fe单原子的纳米酶(SA Fe/B-g-C_(3)N_(4)).同步辐射和扫描透射电子显微镜研究表明单原子Fe催化剂被成功制备.得到的SA Fe/B-gC_(3)N_(4)在H2O_(2)存在下能够表现出良好的类过氧化物酶活性.同时,密度泛函理论计算进一步验证了B掺杂对催化反应的促进作用.基于这些发现,我们利用SA Fe/B-g-C_(3)N_(4)构建了一个比色传感器,用于检测硫化物阴离子的浓度,其检测限为0.57μmol L-1.本方法对自来水和海水中的S2-检测被验证真实可靠.

Development of catalysts with high activities for biomedicine and environmental protection has attracted widespread attention.In this study,B-doped graphite carbon nitride(B-g-C_(3)N_(4))was obtained by polycondensation of melamine with boron oxide as a dopant.The single-atom Fe nanozymes supported on B-g-C_(3)N_(4)(SA Fe/B-g-C_(3)N_(4))were prepared via ion exchange,followed by annealing at elevated temperatures.Synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy investigations demonstrated the successful synthesis of single-atom Fe catalysts.The obtained SA Fe/B-g-C_(3)N_(4) showed good peroxidaselike activity in the presence of H2O_(2).Density functional theory calculations verified the promotion effect of B doping on catalytic reactions.Based on these findings,SA Fe/B-g-C_(3)N_(4) was constructed as a 3-minute colorimetric sensor in response to sulfide anion concentration with a detection limit of 0.57μmol L−1.The feasibility of such protocol in S2−detection was verified in tap water and sea water.