Zhou Hongjie, An Xiaoqiang, Zhang Tianshu, Li Mingran, Kong Lingru, Lan Huachun, Liu Huijuan, Qu Jiuhui
Center for Water and Ecology, State Key Laboratory of Iron and Steel Industry Environmental Protection, School of Environment, Tsinghua University, Beijing, China.
Adv Sci (Weinh). 2025 Sep;12(35):e06580. doi: 10.1002/advs.202506580. Epub 2025 Aug 13.
Sulfur-containing fused heterocyclic polybenzothiazoles are promising materials with advanced functionalities, yet their synthesis has long been constrained by substrate limitations and scalability challenges. Here, a base-mediated multicomponent polymerization strategy using readily available elemental sulfur, aromatic diamines, and aromatic dialdehydes is developed to synthesize unprecedented polybenzothiazoles with scalability. By efficient alkaline activation of substrates through nucleophilic sulfurization-cyclization cascades, this method enables economically viable kilogram-scale production in a one-pot process with high yields (73-98%) and monomer universality, including previously incompatible electron-deficient aromatic amines. The resulting polybenzothiazoles unlock their long-overlooked potential in precious metal recovery, demonstrating selective, rapid, and efficient extraction (>99%) of gold (Au), palladium (Pd), and platinum (Pt) from ultra-trace concentrations (1 ppb) to complex matrices including surface water, e-waste, and spent catalyst leachates. Mechanistic studies reveal that the synergistic nitrogen (N)/sulfur (S) participation and π-conjugation in their fused heterocycles govern metal coordination selectivity and redox stability. This work establishes a practical yet versatile platform to advance polybenzothiazoles from synthesis to resource utilization, highlighting their transformative role in addressing critical challenges through adaptive material design and precious metal recovery.
含硫稠合杂环聚苯并噻唑是具有先进功能的有前途的材料,但其合成长期以来受到底物限制和可扩展性挑战的制约。在此,开发了一种使用易得的元素硫、芳香二胺和芳香二醛的碱介导多组分聚合策略,以可扩展地合成前所未有的聚苯并噻唑。通过亲核硫化-环化级联对底物进行有效的碱活化,该方法能够在一锅法中以高收率(73-98%)和单体通用性实现经济可行的公斤级生产,包括以前不相容的缺电子芳香胺。所得的聚苯并噻唑释放出其在贵金属回收方面长期被忽视的潜力,证明了从超痕量浓度(1 ppb)到包括地表水、电子废物和废催化剂浸出液在内的复杂基质中选择性、快速且高效地提取金(Au)、钯(Pd)和铂(Pt)(>99%)。机理研究表明,其稠合杂环中协同的氮(N)/硫(S)参与和π共轭决定了金属配位选择性和氧化还原稳定性。这项工作建立了一个实用且通用的平台,将聚苯并噻唑从合成推进到资源利用,突出了它们通过适应性材料设计和贵金属回收在应对关键挑战方面的变革性作用。