第一作者：殷俞 副教授
通讯作者：殷俞 副教授/崔升 教授
通讯单位：南京理工大学材料科学与工程学院
DOI:10.1016/j.apsusc.2024.161535
氮化碳（C3N4）被制作成内部中空的风琴状管状形态。原子分散的 Co 位点被成功地封闭在手风琴状管状 C3N4（atCN）基体中，并与 N 以 Co-N4 构型配位。得到的 Co-atCN 催化剂被用于过一硫酸盐（PMS）活化，以降解 4-氯苯酚（4-CP）。最佳的 2.9Co-atCN/PMS 系统只需 10 分钟就能完全降解 4-CP（k = 0.426 min-1）。当使用具有半空心内壁的风琴状管状 C3N4（atCN-sh）时，2.9Co-atCN-sh/PMS 系统仅用了 60 分钟就降解了 72.0% 的 4-CP（k = 0.020 min-1）。此外，2.9Co-atCN/PMS 在去除多种污染物（如甲基橙 (MO)、亚甲基蓝 (MB)、2,4,6-三氯苯酚 (TCP) 和对乙酰氨基酚 (ACT)）方面表现出卓越的活性。去除率分别在 5 分钟、45 分钟、45 分钟和 20 分钟内达到 100%。此外，2.9Co-atCN/PMS 系统还具有良好的抗环境干扰能力。电子顺磁共振（EPR）和淬灭试验表明，2.9Co-atCN/PMS 反应体系在降解 4-CP 的过程中会产生 -OH、SO4-、O2- 和 1O2。
Fig. 1. Schematic diagram of fabricating atomically dispersed Co sites within the accordion-like tubular C3N4 with entirely hollow interior (Co-atCN).
Fig. 2. (A-B) XRD patterns of C3N4 and Co modified samples; SEM images of (C) atCN-sh, (D) 2.9Co-atCN-sh, (E) atCN, (F) 2.9Co-atCN; (G-J) SEM images and corresponding EDS elemental mapping of 2.9Co-atCN.
Fig. 3. (A) XPS survey spectra of atCN and 2.9Co-atCN; (B) XPS spectrum of Co 2p region of 2.9Co-atCN; XPS spectra of atCN and 2.9Co-atCN for (C-D) C 1s region, (E-F) N 1s region.
Fig. 4. (A) AC HAADF-STEM image of 2.9Co-atCN; (B) Co K-edge XANES, (C) k3-Weighted χ(k) function, and (D) Fourier-transformed EXAFS spectra of Co foil, CoO, Co2O3, and 2.9Co-atCN; (E) Wavelet transform of EXAFS spectrum of 2.9Co-atCN; (F) the EXAFS fitting of 2.9Co-atCN at R space.
Fig. 5. Catalytic degradation of 4-CP by (A-B) various catalysts under PMS activation; influences of different reaction conditions in the 2.9Co-atCN/PMS system: (C) temperatures, (D) inorganic anions and cations, (E) initial and constant pH, (F) other contaminants, (G) various water matrix. (Experimental parameters if not specified: [Cat]0 = 0.2 g·L−1, [PMS]0 = 2.0 g/L, [Contaminant]0 = 20 mg·L−1, [leaching Co2+]0 = 0.43 mg·L−1, [HCO3–]0 = [Cl–]0 = [SO42–]0 = [NO3–]0 = [K+]0 = [Ca2+]0 = [Na+]0 = [Mg2+]0 = 5.0 mM, T = 25 °C).
Fig. 6. (A-C) EPR tests for the 2.9Co-atCN/PMS system in 4-CP degradation, (D) the changes in k after adding scavengers, and (E) proposed degradation pathways. (Experimental parameters: [Cat]0 = 0.2 g·L−1, [PMS]0 = 2.0 g/L, [4-CP]0 = 20 mg·L−1, T = 25 °C, DMPO-•OH: ♥, DMPO-SO4• −: ♣, DMPO-O2• −: ♦, TEMP-1O2: •, [TBA = p-BQ = EtOH]0 = 200 mM, [L-his]0 = 5.0 mM).
Yu Yin, Rongrong Fang, Bing Hu, Qinxin Wang, Mengxuan Liu, Abdul Hannan Asif, Shaobin Wang, Hongqi Sun, Sheng Cui, Confining cobalt sites within the matrix of accordion-like tubular carbon nitride for peroxymonosulfate activation to produce sulfate radicals and desirable singlet oxygen, Applied Surface Science, 2025, https://doi.org/10.1016/j.apsusc.2024.161535
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