Geng Junjie, Liang Qianwei, Yu Wenyi, Chen Wei, Lu Guining, Luo Hanjin
School of Environment and Energy, South China University of Technology, Guangzhou, Guangdong 510006, China.
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, Guangdong 510641, China.
J Hazard Mater. 2022 Aug 15;436:129184. doi: 10.1016/j.jhazmat.2022.129184. Epub 2022 May 18.
The efficient removal of heavy metal by rationally designed carbon-based adsorbents is a key challenge in the field of water purification. Herein, we report a nitrogen-enriched lignosulfonate exfoliated graphene oxide (N-LEGO) for hexavalent chromium (Cr(VI)) removal from aqueous solution. The nitrogen content of N-LEGO reached 13.28%, and the ratio of N-bonding configurations (pyri-N:amine-N:pyrro-N:grap-N) was 2.3:1.6:1:2.3. For Cr(VI) with initial concentration of 70 mg L under pH= 2, the residuary concentration after treated by N-LEGO was close to 0.004 mg L, which meets the industrial wastewater discharge standard. The Cr(VI) adsorption behavior on N-LEGO can be fitted with the pseudo-second-order kinetics and Freundlich isotherm model well. The adsorption mechanism of Cr(VI) on N-LEGO includes anions electrostatic attraction, reduction and surface chelation. Density functional theory (DFT) simulations showed that N atoms doping was feasible and thermodynamically stable, meanwhile the N-doped system was easier to adsorb CrO than HCrO. The findings of this work can provide a new idea for the development of N-doped carbon-based adsorbents for the removal of highly toxic Cr(VI) from aqueous solutions.
通过合理设计的碳基吸附剂高效去除重金属是水净化领域的一项关键挑战。在此,我们报道了一种用于从水溶液中去除六价铬(Cr(VI))的富氮木质素磺酸盐剥离氧化石墨烯(N-LEGO)。N-LEGO的氮含量达到13.28%,氮键合构型(吡啶-N:胺-N:吡咯-N:石墨-N)的比例为2.3:1.6:1:2.3。对于初始浓度为70 mg/L、pH = 2的Cr(VI),经N-LEGO处理后的残留浓度接近0.004 mg/L,符合工业废水排放标准。Cr(VI)在N-LEGO上的吸附行为可以很好地用伪二级动力学和Freundlich等温线模型拟合。Cr(VI)在N-LEGO上的吸附机制包括阴离子静电吸引、还原和表面螯合。密度泛函理论(DFT)模拟表明,N原子掺杂是可行的且在热力学上是稳定的,同时N掺杂体系比HCrO更容易吸附CrO。这项工作的发现可为开发用于从水溶液中去除剧毒Cr(VI)的N掺杂碳基吸附剂提供新思路。