Zheng Yao, Lv Peiyuan, Yang Jie, Xu Gangchun
Key Laboratory of Integrated Rice-Fish Farming Ecology, Ministry of Agriculture and Rural Affairs, Freshwater Fisheries Research Center (FFRC), Chinese Academy of Fishery Sciences (CAFS), Wuxi, Jiangsu 214081, China.
Wuxi Fishery College, Nanjing Agricultural University, Wuxi, Jiangsu 214081, China.
ACS Omega. 2023 Aug 10;8(33):29966-29978. doi: 10.1021/acsomega.3c01251. eCollection 2023 Aug 22.
In this study, a composite of pond mud and lanthanum- and nano-zero valent iron-modified-biochar was investigated for its ability to adsorb methylene blue (MB) and sulfamethazine (SMZ). La-modified attapulgite and nano-zero valent iron (surface area enhanced by 43.7% via Brunauer-Emmett-Teller analysis) were successfully loaded onto the straw-sediment biochar (BC) surface. With the increase in pyrolysis temperature, the biocompatibility yield, the H, O, and N content, and the ratio of carbon elements decreased, while the pH value, surficial micropores, C element, and ash content increased. The biocarbon small molecules were gradually and tightly ordered, and the organic groups such as hydroxyl, carboxyl groups, and carbon oxygen double bonds were gradually lost or disappeared. The original Fe-BC had more phenolic hydroxyl groups forming an intermolecular hydrogen bond than others with a higher adsorption capacity possibly through the Schiff base reaction. The effect of various pH (2-9), temperature (15-35 °C), and initial concentration (1-25 mg L) on adsorption was investigated. pH and temperature were the main factors governing the adsorption process. The maximum adsorption capacity was observed at pH 4. The adsorption performances for MB followed the order Fe-BC > La-BC > BC, and the maximum removal rate was over 98.45% with pH = 7. The three types of BC dosages between 0.2 (6.67 g L) and 0.4 g showed a removal rate of 99% for MB. The adsorption capacity of Fe-BC, La-BC, and BC for MB was 2.201, 1.905, and 2.401 mg L with pH = 4, while 4.79, 4.58, and 5.55 mg g were observed with BC dosage at 0.025 g. For SMZ, the higher the temperature, the better the adsorption effect, and it reaches saturation at approximately 25 °C. To further evaluate the nature of adsorption, Langmuir/Freundlich/Temkin models were tested and the adsorption capacities were evaluated on the surface of the BC composite. The three modified materials were physisorbed to SMZ, while MB was chemisorbed. For MB, the adsorption performance of BC is the best < 0.2 g (6.67 g L) at pH 7.0 at 35 °C. The Elovich model was more suitable for MB, while the Freundlich and Temkin models could better fit the adsorption process of MB. The preparatory secondary dynamics equation and Langmuir equation were more compliant for SMZ, and the saturated adsorption capacities of straw-modified, La-BC, and Fe-BC reached 5.699, 6.088, and 5.678 mg L, respectively.
在本研究中,对池塘淤泥与镧和纳米零价铁改性生物炭的复合物吸附亚甲基蓝(MB)和磺胺二甲嘧啶(SMZ)的能力进行了研究。镧改性凹凸棒石和纳米零价铁(通过布鲁诺尔-埃米特-泰勒分析,表面积提高了43.7%)成功负载到秸秆-沉积物生物炭(BC)表面。随着热解温度的升高,生物相容性产率、H、O和N含量以及碳元素比例降低,而pH值、表面微孔、C元素和灰分含量增加。生物炭小分子逐渐紧密有序排列,羟基、羧基和碳氧双键等有机基团逐渐减少或消失。原始的Fe-BC比其他材料具有更多形成分子间氢键的酚羟基,其吸附能力可能通过席夫碱反应更高。研究了不同pH值(2-9)、温度(15-35℃)和初始浓度(1-25mg/L)对吸附的影响。pH值和温度是控制吸附过程的主要因素。在pH值为4时观察到最大吸附容量。对MB的吸附性能顺序为Fe-BC>La-BC>BC,在pH=7时最大去除率超过98.45%。三种类型的BC剂量在0.2(6.67g/L)至0.4g之间时,对MB的去除率为99%。在pH=4时,Fe-BC、La-BC和BC对MB的吸附容量分别为2.201、1.905和2.401mg/L,而在BC剂量为0.025g时,观察到的吸附容量分别为4.79、4.58和5.55mg/g。对于SMZ,温度越高,吸附效果越好,在约25℃时达到饱和。为了进一步评估吸附性质,测试了朗缪尔/弗伦德利希/坦金模型,并在BC复合材料表面评估了吸附容量。三种改性材料对SMZ为物理吸附,而对MB为化学吸附。对于MB,在35℃、pH值为7.0时,BC的吸附性能在<0.2g(6.67g/L)时最佳。埃洛维奇模型更适合MB,而弗伦德利希和坦金模型能更好地拟合MB的吸附过程。预备二级动力学方程和朗缪尔方程对SMZ更符合,秸秆改性、La-BC和Fe-BC的饱和吸附容量分别达到5.699、6.088和5.678mg/L。