Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-08-05 , DOI: 10.1016/j.apcatb.2022.121815 Tao Chen , Tong Liu , Li Zhou , Mingxin Li , Qi Meng , Kaifu Yu , Jie Lian , Wenkun Zhu
Light-driven catalysis-assisted uranium extraction from seawater opens up a promising avenue to enhance the extraction capacity, kinetics, and selectivity for uranium removal. Herein, we report novel ternary boron carbon nitride hollow nanotubes (BCN-HNTs) with tunable p-n homojunction as metal-free photocatalyst for efficient uranium extraction. Relying on the density functional theory calculations, in conjunction with other spectral analyses, we distinguish the six-membered carbon rings introduced in h-BN to form a tunable p-n homojunction. Accordingly, the BCN-HNTs exhibit a remarkable U(VI) removal rate of >95% under a wide range of uranium concentrations. By virtue of the X-ray absorption spectroscopy technique, we identify the conversion of 3Oax-U-4Oeq moieties into the 2Oax-U-3Oeq moieties during the transition from dark to light conditions, further verifying the reduction of high-valent uranium. In addition, we find that the introduction of carbon into h-BN lattice enhances the adsorption energy for uranium species, thereby improving the extraction capacity of uranium.
中文翻译:
具有可调 pn 同质结的三元碳氮化硼中空纳米管用于光辅助铀提取:组合批次、EXAFS 和 DFT 计算
光驱动催化辅助从海水中提取铀开辟了一条有希望的途径,以提高铀去除的提取能力、动力学和选择性。在此,我们报告了具有可调谐 pn 同质结的新型三元碳氮化硼中空纳米管 (BCN-HNT) 作为无金属光催化剂用于高效铀提取。依靠密度泛函理论计算,结合其他光谱分析,我们区分了h -BN 中引入的六元碳环,形成了可调谐的 pn 同质结。因此,在很宽的铀浓度范围内,BCN-HNTs 的 U(VI) 去除率高达 95% 以上。借助 X 射线吸收光谱技术,我们确定了 3O ax -U-4O eq的转换在从黑暗到光照条件的转变过程中,部分进入 2O ax -U-3O eq部分,进一步验证了高价铀的还原。此外,我们发现在h -BN 晶格中引入碳增强了对铀物种的吸附能,从而提高了铀的提取能力。