| Tetracyclines(TCs),as one of the widely used antibiotics in medical,husbandry and aquaculture,are frequently detected in the water environment due to their stable structure and difficulty to be biodegraded,resulting in generation of drug-resistant bacteria and spread of resistant genes.This seriously endangers the security of ecological environment.In view of current tetracycline-related environmental pollution,herein,graphene oxide(GO)was prepared from flake graphite and different graphene composites(α-FeOOH/rGO and C-rGO)were subsequently prepared by oxidation-reduction and hydrothermal method.After systematic characterization,α-FeOOH/rGO and C-rGO were applied to TC adsorption removal.Specific research contents and results are as follows:α-FeOOH/rGO was prepared by the reduction of ferrous ion.The characterization results indicated thatα-FeOOH nanoparticle was rod-like and anchored on surface of graphene.α-FeOOH/rGO showed the adsorption capacity of TC with a value of 219mg·g-1 when the preparation condition was adding 5 mmol ferrous sulfate and reacting24 h at 90℃.And the adsorption kinetic and isotherm experiments for TC ontoα-FeOOH/rGO illustrated that pseudo-second-order model and Freundlich model were more suitable for describing this adsorption process,indicating multilayer adsorption nature of this process.In order to enhance the TC adsorption capacity by graphene composites,C-rGO was prepared via in-situ formations of copper nanoparticle on the surface of rGO under hydrothermal method.Characterization results indicated that Cu nanoparticles and a small amount of cuprous oxide nanoparticles were formed on surface of rGO.The effect of preparation conditions on the TC adsorption performance of C-rGO was also investigated,demonstrating that the GO/Cu2+mass ratio of 1:0.5 at 80℃for 24 h exhibited better adsorption performance with a high value of 3070 mg·g-1.Such high TC adsorption capacity of C-rGO was attributed to load Cu particle and abundant oxygen-containing function group on the surface of rGO.Experiment of adsorption kinetics and isotherms for TC onto C-rGO illustrated that pseudo-first order kinetic model and Langmuir model were more suitable for describing the adsorption process.Furthermore,liquid film diffusion was rate-controlling step of TC adsorption on C-rGO.In addition,the removal efficiency of C-rGO still kept relatively high level after being used for 4 cycles.And C-rGO showed excellent adsorption capacities for other antibiotics,such as oxytetracycline,chlortetracycline hydrochloride,ciprofloxacin,sulfamethoxazole and norfloxacin.The ultrahigh TC adsorption ability and excellent reusability highlighted its great application potential in the field of antibiotic-related wastewater treatment. |