Visible-light-driven photocatalytic degradation of a typical UV filter by a novel composite photocatalyst: DFT calculation, degradation pathway, and toxicity evolution
Visible-light-driven photocatalytic degradation of a typical UV filter by a novel composite photocatalyst: DFT calculation, degradation pathway, and toxicity evolution
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DOI：
10.1016/j.cej.2023.146281
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发表时间：
2023-09
影响因子：
15.1
通讯作者：
Daoyue Xie;Huinan Che;Juan Chen;Y. Ao
中科院分区：
文献类型：
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作者：
Daoyue Xie;Huinan Che;Juan Chen;Y. Ao
二苯甲酮-1 （BP1）是一种典型的紫外线过滤器，在水生环境中大量存在，并通过生物积累对人类健康构成威胁。为了有效去除水环境中的BP1，制备了AgI/Bi2Fe4O9（AgI/BFO）异质结，并将AgI颗粒紧密生长在Bi2Fe4O9纳米片上。由此形成的AgI/BFO异质结扩大了AgI的光吸收范围，促进了电荷转移，显著提高了BP1降解的光催化性能。结果表明，得到的AgI/BFO异质结对BP1的降解速率常数为0.159 min−1，是BFO的15.9倍和AgI的4.1倍。捕获实验证明，超氧自由基（·O2 -）和空穴（h+）是主要的活性物质。根据高效液相色谱-质谱分析（HPLC-MS）结果，结合密度泛函理论（DFT）计算C5、C7和C11为活性物质的主要攻击位点，提出了10种可能的降解中间体。与BP1相比，这些降解中间体的毒性越来越低。本研究为光催化技术降解水中bp污染物的研究提供了新的思路。
Benzophenone-1 (BP1), as a typical ultraviolet (UV) filter, has been detected in large quantities in aquatic environments and can pose a threat to human health through bioaccumulation. To efficiently remove BP1 from the water environment, a type-II AgI/Bi2Fe4O9(AgI/BFO) heterojunction with AgI particles tightly grown on Bi2Fe4O9nanosheets was fabricated. The resultant AgI/BFO heterojunction extended the light absorption range of AgI and promoted charge transfer, which significantly enhanced the photocatalytic performance in BP1 degradation. As a result, the obtained AgI/BFO heterojunction has a degradation rate constant of 0.159 min−1for BP1, which was 15.9 times BFO and 4.1 times AgI. Capture experiments proved that superoxide radicals (·O2–) and holes (h+) are the main active species. According to the high-performance liquid chromatography-mass spectrometry (HPLC-MS) results, combined with density functional theory (DFT) calculations C5, C7, and C11 were the main attack sites of active species, proposed ten possible degradation intermediates. These degradation intermediates showed increasingly lower toxicity compared to BP1. This work provides a new idea for the study of photocatalytic technology to degrade BPs pollutants in water.