Sun Yingtao, Hu Chun, Lyu Lai
Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China.
JACS Au. 2024 Dec 23;5(1):271-280. doi: 10.1021/jacsau.4c00950. eCollection 2025 Jan 27.
Slow mass transfer processes between inert emerging contaminants (ECs) and dissolved oxygen (DO) limit natural water self-purification; thus, excessive energy consumption is necessary to achieve ECs removal, which has become a longstanding global challenge. Here, we propose an innovative water self-purification expansion strategy by constructing asymmetric surfaces that could modulate trace HO as trigger rather than oxidant to bridge a channel between inert ECs and natural dissolved oxygen, achieved through a dual-reaction-center (DRC) catalyst consisting of Cu/Co lattice-substituted ZnO nanorods (CCZO-NRs). During water purification, the bond lengths of emerging contaminants (ECs) adsorbed on the asymmetric surface were stretched, and this stretching was further enhanced by HO mediation, resulting in a significant reduction of bond-breaking energy barriers. As a result, the consumption rate of HO was reduced by two-thirds in the presence of ECs. In contrast, the removal of ECs was increased approximately 95-fold mediated by trace HO. It exhibits the highest catalytic performance with the lowest dosage of HO among numerous similarly reported systems. This discovery is significant for the development of water self-purification expansion technologies.
惰性新兴污染物（ECs）与溶解氧（DO）之间缓慢的传质过程限制了天然水的自净能力；因此，需要消耗大量能量才能实现对ECs的去除，这已成为一个长期存在的全球性挑战。在此，我们提出了一种创新的水自净扩展策略，即通过构建不对称表面，该表面可以调节痕量羟基自由基（HO）作为引发剂而非氧化剂，以在惰性ECs和天然溶解氧之间架起一座通道，这是通过由铜/钴晶格取代的氧化锌纳米棒（CCZO-NRs）组成的双反应中心（DRC）催化剂实现的。在水净化过程中，吸附在不对称表面上的新兴污染物（ECs）的键长被拉长，并且这种拉长通过HO的介导进一步增强，从而导致键断裂能垒显著降低。结果，在存在ECs的情况下，HO的消耗速率降低了三分之二。相比之下，痕量HO介导的ECs去除率提高了约95倍。在众多类似报道的体系中，它以最低的HO用量展现出最高的催化性能。这一发现对水自净扩展技术的发展具有重要意义。
