Design of core-shelled g-C3N4@ZIF-8 photocatalyst with enhanced tetracycline adsorption for boosting photocatalytic degradation
Design of core-shelled g-C3N4@ZIF-8 photocatalyst with enhanced tetracycline adsorption for boosting photocatalytic degradation
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增强四环素吸附的核壳g-C3N4@ZIF-8光催化剂的设计促进光催化降解
DOI：
10.1016/j.cej.2021.129148
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发表时间：
2021-07
影响因子：
15.1
通讯作者：
Ping Cai
中科院分区：
文献类型：
--
作者：
Xin Yuan;Senlin Qu;Xiaoyan Huang;Xiaogang Xue;Changlai Yuan;Songwei Wang;Lai Wei;Ping Cai
将活性物种和中间体限制在有限的空间内，对于推动污染物转化（包括促进降解的连续反应）至关重要。本文通过ZIF-8原位生长，对g- c3n4进行剥离包覆，制备了核壳g-C3N4@ZIF-8。XRD、SEM、TEM和EDX图谱显示ZIF-8中含有卷曲的g- c3n4薄片。UV-vis、PL、FTIR、XPS证实了TC与ZIF-8中Zn的配合性。稳态瞬态PL、EIS和瞬态光电流响应表明，两种材料的结合有利于载流子的分离和转移。进一步的能带分析表明，g- c3n4的界面带弯曲促进了电子空穴的分离和电子向ZIF-8的扩散。结果表明，优化后的g-C3N4@ZIF-8具有较好的TC降解速率常数（k= 0.068 min−1），是g-C3N4（k= 0.014 min−1）的4.8倍，TC去除率比g-C3N4（58.6%）提高了87.6%。优化后的材料对地表水中RhB（99.3%）和Cr (VI)（96.6%）均有较好的降解率和去除率。对活性物质和降解途径的研究（EPR, LC-MS）表明，ZIF-8约束的g- c3n4的协同作用促进了氧自由基（自由基dotO2−）的形成和向单线态氧（1O2）的转化，促进了TC的降解。
Confining active species and intermediates in a limited spatial is critical to driving pollutant transformation involving successive reactions for boosting degradation. Herein, core–shell g-C3N4@ZIF-8 were prepared by exfoliating-wrapping of g-C3N4via ZIF-8 in-situ growth. XRD, SEM, TEM, and EDX mapping demonstrate the inclusion of curled g-C3N4sheets in ZIF-8. UV–vis, PL, FTIR, and XPS confirm the coordination of TC with Zn of ZIF-8. Steady-transient PL, EIS and transient photocurrent response indicate that the combination of two materials favors the carriers’ separation and transfer. Further band analysis suggests that interfacial band bending of g-C3N4promotes the separation of electron-hole and electron diffusion toward ZIF-8. As result, the optimized g-C3N4@ZIF-8 exhibits a superior TC degradation rate constant (k= 0.068 min−1), 4.8 times higher than that of g-C3N4(k= 0.014 min−1), and enhanced TC removal rate of 87.6% higher than g-C3N4(58.6%). Also, the optimized material shows superior degradation rate and removal efficacy in RhB (99.3%) and Cr (VI) (96.6%) in surface water. The investigations on active species and degradation routes (EPR, LC-MS) reveal that synergetic effects of ZIF-8 confined g-C3N4facilitate the formation of oxygen radicals (radical dotO2−) and their transformation toward singlet oxygen (1O2) for boosting TC degradation.
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