Probing the role of surface acid sites on the photocatalytic degradation of tetracycline hydrochloride over cerium doped CdS via experiments and theoretical calculations
Probing the role of surface acid sites on the photocatalytic degradation of tetracycline hydrochloride over cerium doped CdS via experiments and theoretical calculations
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DOI：
10.1039/d1dt02852a
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发表时间：
2021-10-26
影响因子：
4
通讯作者：
Wang, Peifang
中科院分区：
文献类型：
--
作者：
Chen, Ran;Chen, Juan;Wang, Peifang
光催化剂的表面酸位调控是提高其性能的一个很有前途的策略。其中，Ce掺杂合理地调节了硫化镉表面的酸性中心，从而显著提高了对四环素盐酸盐(TC-HCl)的光催化降解活性。生成的Bronsted酸中心具有较强的亲和力，有利于有机分子的吸附。同时，通过亲核取代反应，Lewis酸位成为C-C键断裂的活性中心，Fukui函数和静电势证明了这一点。此外，Ce3+的掺杂抑制了电子-空穴对的复合，从而提高了TC-HCl的降解性能。此外，根据理论计算和高效液相色谱-质谱联用结果，推测了TC-HCl的降解途径。并对污染物和中间体的毒性进行了评价。该工作为环境净化用高效光催化剂的合理设计和制备提供了新的思路。
Surface acid site regulation of photocatalysts is a promising strategy to improve their performance. Herein, surface acid sites of cadmium sulfide were rationally regulated by cerium doping, which resulted in significantly increased photocatalytic activity for tetracycline hydrochloride (TC-HCl) degradation. The generated Bronsted acid sites were verified to favor the adsorption of organic molecules because of their strong affinity. Meanwhile, Lewis acid sites acted as the active sites for C-C bond cleavage via a nucleophilic substitution process, which was testified by the Fukui function and electrostatic potential. Besides, Ce3+ doping suppressed the recombination of electron-hole pairs, which also boosted the performance of TC-HCl degradation. Moreover, the degradation pathway of TC-HCl was deduced based on theoretical calculations and HPLC-MS results. The toxicity of pollutants and intermediates was also evaluated. This work provided new insight into the rational design and preparation of highly efficient photocatalysts for environmental purification.