Activity and Mechanism of Catalytic Degradation of Rhodamine B by Ni(Ⅱ) Complex Derived from Polycarboxylate Ligand
LIU Yang1,*, MA Zhanying1, LI Wuwu1, GUO Naini1, HOU Lei2,*, FAN Xingyu1, WANG Ying’ai1, WANG Yaoyu2
1 School of Chemistry and Chemical Engineering, Xianyang Normal University, Xianyang 712000, Shaanxi, China 2 College of Chemistry & Materials Science, Northwest University, Xi’an 710069, China
Abstract: With the rapid expansion of textile and printing industry scale, the dye wastewater generated in the production process has brought huge pressure to living environment. At present, in the field of remediation and treatment of dye wastewater, advanced oxidation technology based on SO4·- has attracted much attention due to its oxidation advantages. In general, peroxymonosulfate (PMS) can self-decompose to produce SO4·-, but the efficiency is low, so searching for an effective PMS catalyst has become a focus recently. Here a 3D complex Ni4(odip)2-(μ2-OH2)2(H2O)8 was prepared by solvothermal method using 5, 5′-oxydiisophthalic acid (H4odip) and Ni(NO3)2·6H2O, which has good water stability and can exist stably in weak acid and weak alkali environment. To study it’s structure and composition, X-ray single crystal and powder diffraction, infrared spectroscopy, thermogravimetric analysis and elemental analyses are adopted here. The activity and mechanism of catalytic degradation of Rhodamine B were tested by UV-Vis spectrophotometer. At the same time, the effects of the complex and peroxymonosulfate loading, reaction temperature and pH on dye degradation were systematically studied. Compared with no catalyst, the degradation rate of Rhodamine B was increased by two times with the addition of the complex. In the neutral environment, the PMS/complex catalytic system has a stronger degradation ability, and the degradation rate can reach 92.3%. A comprehensive analysis of the active oxygen species (ROS) capture experiment and electron paramagnetic resonance (EPR) test results confirmed that the ROS produced by the PMS/complex system include SO4·-, ·OH, 1O2 and O2·-, and the contribution of the four ROS in the degradation of rhodamine B was similar. Therefore, the complex can be used as an effective and recyclable new heterogeneous catalyst in the field of catalytic PMS for dye wastewater remediation.
刘洋, 马占营, 李午戊, 郭乃妮, 侯磊, 樊星宇, 王樱嫒, 王尧宇. 多羧酸镍配合物催化降解罗丹明B的活性与机理[J]. 材料导报, 2024, 38(16): 24030040-6.
LIU Yang, MA Zhanying, LI Wuwu, GUO Naini, HOU Lei, FAN Xingyu, WANG Ying’ai, WANG Yaoyu. Activity and Mechanism of Catalytic Degradation of Rhodamine B by Ni(Ⅱ) Complex Derived from Polycarboxylate Ligand. Materials Reports, 2024, 38(16): 24030040-6.
1 Sriram G, Bendre A, Mariappan E, et al. Sustainable Materials and Technologies, 2022, 31, e00378. 2 Zhao W W, Wang Y L. Acta Chimica Sinica, 2019, 77(8), 717 (in Chinese). 赵微微, 王毅琳. 化学学报, 2019, 77(8), 717. 3 Liu Y C, Zhu M, Chen M Y, et al. Materials Reports, 2020, 34(7), 7004 (in Chinese). 刘宇程, 祝梦, 陈明燕, 等. 材料导报, 2020, 34(7), 7004. 4 Tambat S N, Sane P K, Suresh S, et al. Advanced Powder Technology, 2018, 29, 2626. 5 Ma Z H, Ren Y X, Wang Z X, et al. Chinese Journal of Inorganic Chemistry, 2023, 39(10), 2009. 6 Wang Y Y, Yan X, Ai T, et al. Materials Reports, 2022, 36(17), 193 (in Chinese). 王渊源, 阎鑫, 艾涛, 等. 材料导报, 2022, 36(17), 193. 7 Yang G, Mo S, Xing B, et al. Environmental Pollution, 2020, 258, 113687. 8 Li X, Jia Y, Zhou M, et al. Journal of Hazardous Materials, 2020, 397, 122764. 9 Sun Y, Xie H, Zhou C, et al. Journal of Hazardous Materials, 2020, 398, 122827. 10 Clothier L N, Gieg L M. Water Research, 2016, 90, 156. 11 Pham T D, Bui V P, Pham T N, et al. Polymers, 2021, 13(10), 1536. 12 Chen Y, Liu H, Hu X, et al. Fibers and Polymers, 2017, 18(7), 1250. 13 You W Q. Degradation of organic dyes by different activation systems of peroxymonosulfate. Master’s Thesis, Southwest University, China, 2022 (in Chinese). 游温侨. 过一硫酸盐的不同活化体系对有机染料污染物的降解研究. 硕士学位论文, 西南大学, 2022. 14 Kohantorabi M, Moussavi G, Giannakis S. Chemical Engineering Journal, 2021, 411, 127957. 15 Qi C, Liu X, Ma J, et al. Chemosphere, 2016, 151, 280. 16 Duan X, Sun H, Wang S. Accounts of Chemical Research, 2018, 51(3), 678. 17 Wacławek S, Lutze H V, Grübel K, et al. Chemical Engineering Journal, 2017, 330, 44. 18 Li X J, Ye Z Y, Xie S H, et al. Acta Chimica Sinica, 2022, 80(9), 1238 (in Chinese). 李小娟, 叶梓瑜, 谢书涵, 等. 化学学报, 2022, 80(9), 1238. 19 Wang J L, Wang S Z. Chemical Engineering Journal, 2018, 334(15), 1502. 20 Ding Y, Pan C, Peng X, et al. Chemical Engineering Journal, 2020, 384, 123378. 21 Guan Y H, Ma J, Ren Y M, et al. Water Research, 2013, 47(14), 5431. 22 Xiao Z Y, Li Y, Fan Lu, et al. Journal of Colloid and Interface Science, 2021, 589, 298. 23 Chi H Y, Wan J Q, Ma Y W, et al. Journal of Hazardous Materials, 2019, 377(5), 163. 24 Zhang W X, Zhang H, Yan X, et al. Journal of Hazardous Materials, 2020, 387(5), 121701. 25 Gua A T, Wang P, Chen K W, et al. Separation and Purification Technology, 2022, 298, 121461. 26 Li J L, Zhu W H, Gao Y, et al. Separation and Purification Technology, 2022, 285, 120362. 27 Rojas S, Horcajada P. Chemical Reviews, 2020, 120(16), 8378. 28 Lv H, Yang Q, Kong Y. Materials Reports, 2023, 37(4), 170 (in Chinese). 鲁浩, 杨强, 孔赟. 材料导报, 2023, 37(4), 170. 29 Yang Y, Fu P, Li X, et al. Inorganic Chemistry Communications, 2020, 122, 108282. 30 Xu L L, Liu W P, Li X F, et al. RSC Advances, 2015, 5, 12248. 31 Wang Y, Li X, Hu X Li, et al. Journal of Solid State Chemistry, 2020, 289, 121443. 32 Xie W, Yuan Y, Wang J J, et al. Dalton Transactions, 2023, 52, 14852. 33 Liu Y, Gao F Q, Ma Z Y, et al. Acta Chimica Sinica, 2024, 82(2), 152 (in Chinese). 刘洋, 高丰琴, 马占营, 等. 化学学报, 2024, 82(2), 152. 34 Luo X S, Bai L M, Xing J J, et al. ACS Applied Materials & Interfaces, 2019, 11(39), 35720.